Rec ZN 4

Journal of Cleaner Production 149 (2017) 1079e1100
Contents lists available at ScienceDirect
Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro
Review
Pyrometallurgical recycling of electric arc furnace dust

Xiaolong Lin a, Zhiwei Peng a, *, Jiaxing Yan a, Zhizhong Li a, Jiann-Yang Hwang b,
Yuanbo Zhang a, Guanghui Li a, Tao Jiang a
a
School of Minerals Processing and Bioengineering, Central South University, Changsha, Hunan 410083, China
b
Department of Materials Science and Engineering, Michigan Technological University, Houghton, MI 49931, USA
a r t i c l e i n f o a b s t r a c t
Article history: Electric arc furnace (EAF) dust is an important secondary resource which contains multiple metallic
Received 22 July 2016 elements, such as zinc, lead, iron, chromium and cadmium. Recycling of EAF dust is not only favorable to
Received in revised form increasing economic potential of the dust by recovering these valuable metals, but also of benefit to
25 January 2017
solving disposal and environmental problems caused by the heavy metals (e.g., lead, chromium and
Accepted 17 February 2017
cadmium) entrained in the dust. Among the existing processes and those under development, pyro-
Available online 17 February 2017
metallurgical routes are considered the primary choice for processing of EAF dust because of its high
potential metal recovery, easy treatment of residue and relatively short flow sheet. In this paper, the
Keywords:
Electric arc furnace dust
authors reviewed the chemical and physical properties of EAF dust and its thermodynamic character-
Recycling istics in pyrometallurgical processing, followed by an in-depth discussion of a variety of the pyromet-
Pyrometallurgical process allurgical processes for recycling of the dust, including Waelz kiln process, rotary hearth furnace (RHF)
Zinc process, PRIMUS process, OXYCUP process, coke-packed bed process, Ausmelt process, electric smelting
Iron reduction furnace (ESRF) process, Plasamadust process, plasma-arc process, Elkem multi-purpose
Hazardous pollutants furnace (EMPF) process, submerged plasma process, pig iron zinc oxide (PIZO) process, flame reactor
process, thermal plasma reduction process, microwave processing, solar thermal reduction process, iron
bath smelting process, calcification process and halogenation process. Particular attention is devoted to
specific technical challenges emerging in the pyrometallurgical processing of EAF dust and to the cor-
responding potential measures for improving the dust recycling by promoting the processing efficiency
with elimination of secondary hazardous pollutants.
© 2017 Elsevier Ltd. All rights reserved.
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1080
2. Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3. Chemical and physical characteristics of EAF dust . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3.1. Chemical composition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3.2. Phase composition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3.3. Particle size distribution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3.4. Density and moisture content . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1081
3.5. Microstructural morphology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1082
3.6. Thermal property . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1082
4. Thermodynamics concerning pyrometallurgical processing of EAF dust . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1083
5. Pyrometallurgical processes for recycling of EAF dust . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1084
5.1. Waelz kiln process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1085
5.2. Rotary hearth furnace process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1085
5.3. PRIMUS process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1088
5.4. OXYCUP process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1089
* Corresponding author.
E-mail address: [email protected] (Z. Peng).
http://dx.doi.org/10.1016/j.jclepro.2017.02.128
0959-6526/© 2017 Elsevier Ltd. All rights reserved.
1080 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
5.5. Coke-packed bed process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1090

5.6. Ausmelt process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1090
5.7. ESRF process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1091
5.8. Plasamadust process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1091
5.9. Plasma-arc process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1091
5.10. EMPF process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1092
5.11. Submerged plasma process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1092
5.12. PIZO process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1093
5.13. Flame reactor process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1093
5.14. Thermal plasma reduction process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1093
5.15. Microwave processing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1094
5.16. Solar thermal reduction process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1094
5.17. Iron bath smelting process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1094
5.18. Calcification process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1095
5.19. Halogenation process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1095
6. Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1096
7. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1097
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1098
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1098
1. Introduction and dissolution of iron (e.g., up to 45% even when diluted sulfuric
acid (acid normality ¼ 3 N) was used) (Oustadakis et al., 2010)
With the rapid development of steelmaking industry, the global which hinders the subsequent operations such as zinc electro-
crude steel production reached a stage of 1.623 billion tons in 2015 winning (Tsakiridis et al., 2010). Compared with acidic solvents,
(World Steel Association, 2016). The crude steel production is alkaline lixivants (e.g., sodium hydroxide) are more selective with
accompanied by a large amount of dust/sludge, slag, wastewater respect to multiple metals (Bakkar, 2014). The alkaline route may
and exhaust gas which pose a great threat to both environment and achieve better results technically and economically, with less gen-
human health (Mo et al., 2015; Gomes et al., 2016; Pan et al., 2016). eration of residue (Palencia et al., 1999). The shortcoming of alka-
The steel plant dusts are an important by-product of the steel- line leaching is the undesirable leaching of lead (Youcai and
making industry with output accounting for about 10% of the crude Stanforth, 2000). Because of these problems, particularly the
steel production (Dutra et al., 2006). As a representative type of strongly pH dependent leaching of zinc and lead (Kumpiene et al.,
steel plant dust, electric arc furnace (EAF) dust has an output equal 2008), complex operations and multiple steps are often necessary
to approximately 1%e2% of the charge in a typical EAF operation for hydrometallurgical processes to improve recovery of the metals
(Dutra et al., 2006). In 2014, the global EAF dust output soared to (Tang and Steenari, 2016), especially for leaching of the dust with a
8.764 million tons. This dust generally contains up to 40 wt% zinc high content of slightly soluble zinc ferrite (Youcai and Stanforth,
(Nolasc-Sobrinho et al., 2003) and 50 wt% iron (Orhan, 2005; 2000). Furthermore, severe leachate contamination issues may
Salihoglu and Pinarli, 2008). It is also accompanied with a variety occur arising from the halogens (Ruiz et al., 2007) and the other
of harmful heavy metals, e.g., Pb, Cr and Cd (Salihoglu and Pinarli, components in the EAF dust (Oustadakis et al., 2010). The principle
2008), and thereby frequently categorized as one of most trouble- of chemical stabilization/vitrification (e.g., the Oregon process), on
some and hazardous waste being difficult to store and transport (Lis the other hand, is to mold EAF dust into lump by direct sintering or
et al., 2015). For disposal of the dust, landfilling offers a simple by sintering with chemical additives, e.g., CaCO3, Na2CO3 and SiO2
solution (Donald and Pickles, 1996). However, it not only causes (Kavouras et al., 2007), or by stabilization with addition of lime
accumulation of heavy metals in the groundwater and soil under (Pereira et al., 2001), other wastes such as blast furnace slag, coal fly
the impact of rain, posing harm to animals and plants as well as ash or aluminum cement after mixing, molding and compacting
human survival environment, but also results in a waste of re- (Salihoglu and Pinarli, 2008). Because this method is solely used for
sources as valuable elements such as zinc and iron are not generating impermeable substrate which encapsulates dust parti-
recovered. cles for stabilization of hazardous components in dust, it does not
In view of the potential economic and environmental benefits of sufficiently take into account the recovery of metals of economic
EAF dust, it is of importance to develop appropriate approaches for interest, therefore representing a waste of resources (Pickles,
treatment of the dust. The emergent processing methods can be 2008a,b). Unlike hydrometallurgical processes and chemical sta-
classified into three categories, namely pyrometallurgical pro- bilization/vitrification, the principle of pyrometallurgical processes
cesses, hydrometallurgical processes and chemical stabilization/ is to recover the metals, primarily based on carbothermic reduction
vitrification (Donald and Pickles, 1996). The principle of hydro- or other thermal reactions (e.g., calcification and halogenation)
metallurgical approaches, for example, the classical ZINCEX process (Guo et al., 2010). Although hydrometallurgical processes and
(Díaz et al., 2001) and EZINEX process (Castro and Marques, 2001), chemical stabilization/vitrification method have relatively lower
is to leach metal oxides (ZnO, PbO, etc.) from the dust in either an energy consumption (Mauthoor et al., 2014), pyrometallurgical
acidic (Hilber et al., 2003) or an alkaline solvent (Havlík et al., 2005). processes, featured by high potential metal recovery, easy treat-
These processes usually place stringent requirements on the ment of residue and short flow sheet, are deemed the preferential
leaching apparatus due to the lixiviants of relatively high concen- option for recycling of EAF dust and remain the only ones which
tration (Havlík et al., 2006). The acidic lixiviants, such as sulfuric have reached commercialization (Huaiwei and Xin, 2011).
acid (Li et al., 2010), have good recovery of zinc (Leclerc et al., 2002), Currently, recognition in recycling of the dust via pyrometal-
but may simultaneously cause secondary wastes (Pickles, 2009a,b) lurgical processing is still incomplete despite the progress of
X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100 1081
treatment of EAF dust in the past decades. The aim of the present Table 1
study is to present a critical review of pyrometallurgical processes Typical chemical compositions of EAF dust (NR ¼ not reported).
for recycling of EAF dust. The chemical/physical characteristics of Element Low zinc dust (wt.%) Medium zinc dust (wt.%) High zinc dust (wt.%)
the dust and its thermodynamic characteristics in pyrometallurgi- (Sofili
c et al., 2004) (Sofili
c et al., 2004) (Suetens et al., 2015)
cal processing are provided, followed by a detailed review of the Zn 3.75 8.10 27
mainstream and recently developed routes for recovery of metal Fe 48.58 41.08 29
values from the dust. Lastly, the technical challenges to the progress Ca 3.79 4.07 3.1
Na 0.57 0.61 1.5
of the pyrometallurgical processing of EAF dust are summarized
Pb 1.02 2.07 2.5
and corresponding potential/promising measures are expounded Si 1.91 1.91 1.3
with aim to offer a useful guideline for sustainable recycling of the K 0.67 0.78 1.2
dust. Mn 5.76 5.18 2.3
S 0.55 0.66 0.6
C 0.38 0.35 3.0
2. Methods Cl NR NR 3.6
Mg 2.16 2.00 0.4
This review is designed to summarize and evaluate recent ad- Al 0.20 0.26 0.4
vancements in the recycling of EAF dust via various pyrometallur- Ni 0.019 0.023 NR
Cu 0.22 0.27 0.3
gical processes. A number of commercial websites, scientific
Cr 0.22 0.21 0.5
journal articles, proceedings papers and reports were selected and Cd 0.011 0.025 0.1
reviewed. The literature search was carried out using the most As <0.01 <0.01 NR
important and commonly used databases, such as Web of Science, Hg <0.01 <0.01 NR
Scopus, SciFinder and Google Scholar. At first, the following specific
keywords were chosen: electric arc furnace dust, dust recycling,
carbothermic reduction, pyrometallurgical process, zinc, lead, iron because of the high operating temperature of EAF and their rela-
and hazardous pollutant. Subsequently, the abstracts were carefully tively low boiling temperatures. Due to the complicated occurrence
examined before the publications were determined based on the of these elements, prior treatments before pyrometallurgical step,
criteria which correlate to the paper’s objective and fit its scope. such as In-Process Separation (Ma, 2011, 2016), may be imple-
Particularly, the authors appraised studies: 1) characterizing mented to enrich beneficial elements and to reduce concentrations
physiochemical properties of EAF dust; 2) exploring reaction of harmful elements in the dust.
mechanisms during pyrometallurgical processing; 3) providing
sustainable approaches with crucial technologies parameters; and 3.2. Phase composition
4) addressing future prospects of pyrometallurgical processes
without secondary hazardous pollution. The phase composition of EAF dust is summarized in Table 2.
The main phases of EAF dust are zinc oxide (zincite), zinc ferrite
3. Chemical and physical characteristics of EAF dust (franklinite), ferric oxide (hematite), ferrous-ferric oxide (magne-
tite), calcium oxide (lime), calcium carbonate (calcite), calcium-iron
The chemical and physical characteristics of EAF dust are the silicate (hedenbergite), etc. The hazardous metals, such as lead and
starting point in the definition of a suitable recycling process. These chromium, are mainly present in the form of oxides (e.g., cerusite
characteristics mainly include chemical composition, phase and chromite). The occurrences of these elements are consistent
composition, particle size distribution, density and moisture con- with their contents in EAF dust shown in Table 1. The formations of
tent, microstructural morphology and thermal property. the major phases are a result of intensive reactions between zinc,
iron and calcium species which are involved in the EAF smelting.
3.1. Chemical composition The minor phases, such as lead and chromium oxides, are present
due to volatilization and subsequent oxidation or entrainment of
EAF dust is produced when zinc-bearing scrap is remelted in an relevant metals.
electric arc furnace. The type of scrap processed in an EAF has a
substantial effect on the dust composition and properties. The
components of EAF dust originate from vaporized and subsequently 3.3. Particle size distribution
oxidized non-ferrous metals, metal and slag constituents formed
due to the explosion of CO gas bubbles at the slag-gas interface, and The formation process of the EAF dust implies that the dust
from low density furnace additions, such as carbon and lime which would be a complex powdered waste composed of fine-grained
are captured by the off-gas handling system (Pickles, 2009a,b). The particles. The dust particle size usually ranges from 0.1 to 100 mm
prevailing elements in EAF dust are zinc, iron and calcium. Other (Ranitovic et al., 2014). Fig. 1 shows the particle size distribution of
less prevalent elements include sodium, potassium, manganese an EAF dust sample (Oustadakis et al., 2010). It is observed that the
and silicon. The dust also contains hazardous lead, chromium and dust had two main size fractions, namely a very fine-grained
cadmium. According to zinc content, it can be divided into 3 cate- portion (0.1e1 mm) and a coarser portion (1e100 mm). Half of the
gories: low zinc dust (<4 wt%), medium zinc dust (4%-20 wt%) and dust particles were below 19.3 mm, and approximately 90% of the
high zinc dust (>20 wt%) (Lis et al., 2015), as shown in Table 1. The particles were less than 100 mm. It is worth noting that the particle
zinc content in the dust increases with declining iron content. This size distribution of EAF dust is closely associated with its moisture
trend is attributed to the reactions of zinc oxide with iron oxides in content. The large solid agglomerates in EAF dust are often a result
EAF, which elevate the content of iron in the EAF dust by forming of long period storage (Huaiwei and Xin, 2011).
ferrites. For the other major element in the EAF dust, calcium, its
content remains relatively constant because it is primarily intro- 3.4. Density and moisture content
duced to EAF by addition of flux which can be controlled exactly in
practice. The above-mentioned minor elements in the dust are Table 3 lists the density and moisture content of EAF dust
mostly originated from the feed of EAF. Most of them enter the dust collected from two different locations. The apparent density of the
Table 2
Typical crystalline phases present in EAF dust.
Element Phases References
Zn Zinc oxide, zinc ferrite, hydrated zinc chloride da Silva et al., 2008; da Silva Machado et al., 2006
Fe Zinc ferrite, ferric oxide, ferrous-ferric oxide, ferrous oxide, metallic iron, iron de Souza et al., 2010; Ma and Garbers-Craig, 2006
silicates, iron sulfides, iron sulfates
Ca Calcium oxide, calcium carbonate, calcium silicates, calcium aluminosilicates, Mantovani et al., 2004; Martins et al., 2008
calcium fluoride, calcium magnetite
Pb Lead oxide, lead chloride, lead sulfide, lead sulfate, lead hydroxyl chloride, lead Oustadakis et al., 2010; Ranitovi
c et al., 2014
chloride carbonate
Si Iron silicates, calcium silicates, calcium aluminosilicates, silicon dioxide Oustadakis et al., 2010; Ranitovic et al., 2014; Xia and Pickles, 2000
Mg Magnesium oxide, magnesium ferrite da Silva et al., 2008; da Silva Machado et al., 2006
S Iron sulfides, iron sulfates, lead sulfide, lead sulfate, sulfur Mantovani et al., 2004; Ranitovi c et al., 2014
Cl Sodium chloride, potassium chloride, zinc chloride, calcium chloride, lead Ma and Garbers-Craig, 2006; Xia and Pickles, 2000
hydroxyl chloride
F Calcium fluoride, sodium fluoride, potassium fluoride Ma and Garbers-Craig, 2006; Mantovani et al., 2004
K Potassium oxide, potassium chloride da Silva et al., 2008; Mantovani et al., 2004
Na Sodium oxide, sodium chloride Ma and Garbers-Craig, 2006; Mantovani et al., 2004
Mn Manganese oxides, manganese sulfide, manganese sulfate da Silva et al., 2008; da Silva Machado et al., 2006; Ma and Garbers-
Craig, 2006
Al Aluminum oxide, calcium aluminosilicates Martins et al., 2008; Ma and Garbers-Craig, 2006; da Silva et al., 2008
Ni Nickel oxide, nickel sulfides, nickel chromite Ma and Garbers-Craig, 2006; Mantovani et al., 2004
Cu Copper oxide, copper sulfides de Souza et al., 2010; Martins et al., 2008;
Cr Chromium oxides, chromite, nickel chromite da Silva et al., 2008; de Souza et al., 2010; Ma and Garbers-Craig, 2006
Cd Cadmium oxide, cadmium sulfate Xia and Pickles, 2000; Mantovani et al., 2004
dust varies significantly, depending on the source position, while (Nolasc-Sobrinho et al., 2003). Additionally, a number of metal-
the real density remains relatively constant. In general, EAF dust oxygen structural forms may appear, as demonstrated by the
has a very low moisture content (<1 wt%). match of metal and oxygen distribution in accumulations in Fig. 3
(Sofili
c et al., 2004) which shows the elemental distribution im-
ages of oxygen, zinc, magnesium, aluminum, silicon, sulfur, lead,
3.5. Microstructural morphology calcium, manganese, iron and copper.
Fig. 2 shows an electron micrograph of dispersed EAF dust

particles (Simonyan et al., 2015). The friability and porosity of the 3.6. Thermal property
surfaces of the dust particles and some aggregations between the
particles are clearly observed (Badger and Kneller, 1997). The The thermal stability of EAF dust can be revealed by thermog-
spherical morphology confirms that the dust formation is a result of ravimetric analysis (TGA). Fig. 4 shows the TGA profile of a EAF dust
slag (Mantovani et al., 2002) and metal ejection by CO bubble sample (26.66 wt% Zn) at a ramp rate of 10 C min1 under N2 at-
bursting on the surface of the bath (Gue zennec et al., 2004). Den- mosphere (Al-Harahsheh et al., 2014). According to the diagram,
dritic structures may exist within the spherical particles, there existed three steps for the mass loss. The first mass loss event
comprising an iron-chromium spinel and a slag matrix composed started at 136 C with the maximum mass loss rate occurring at
of silicon, calcium, iron, aluminum, magnesium and oxygen 175 C, corresponding to evaporation of entrained free water and
Fig. 1. Particle size distribution of EAF dust (Oustadakis et al., 2010).

Table 3
Density and moisture content of EAF dust (NR ¼ not reported).
EAF Dust Apparent density Real density Moisture content Notes References
(g cm3) (g cm3) (wt.%)
#1 2.53 4.90 0.23 Mixing chamber dust Nolasc-Sobrinho et al., 2003

#2 0.90 4.38 0.62 Baghouse dust Nolasc-Sobrinho et al., 2003
#3 1.01 4.10 NR NR Dai et al., 2004
#4 NR 4.33 0.17 NR Fedorko et al., 2012
chemically adsorbed water (e.g., water bound to the metal chlo- metallic forms at relatively low temperatures (<1000 C, see reac-
rides). The second mass loss had an onset temperature of 380 C tion temperature in Table 4 at which the corresponding reaction
with the maximum mass loss occurring in the range 630e700 C, takes place) in spite of their endothermic nature. This fact partially
essentially attributed to the vaporization of metal chlorides (e.g., supports recycling EAF dust via pyrometallurgical processes. After
ZnCl2). The final mass loss event initiated at a temperature of reduction, zinc, lead and cadmium will evaporate because of their
750 C, and the loss was assigned to the vaporization of zinc metal high vapor pressures at the EAF operating temperature. The metal
generated due to reduction of zinc oxide by free carbon (2.2 wt%) vapors can then be condensed, separated and recovered using a
present in the dust. condenser system. Conversely, iron and chromium will be retained
in the residue after thermal reduction. The iron-rich residue from
reduction of dust, especially from the low-zinc dust, is eligible for
4. Thermodynamics concerning pyrometallurgical processing
reclamation. This residue can be used directly, or after simple
of EAF dust
treatment, as a qualified secondary raw material for steel
production.
The principle of pyrometallurgical processing of EAF dust is to
It should be emphasized that most of the existing pyrometal-
extract valuable metals such zinc, iron, lead, etc, from the dust,
lurgical processes are based on carbothermic reactions. The metal
essentially dependent on carbothermic reduction (e.g., Waelz kiln
oxides in EAF dust are reduced by either carbon or carbon mon-
process), calcification (e.g., calcification process) or halogenation
oxide. Compared with solid carbon, carbon monoxide has better
(e.g., chlorination process). The Gibbs free energy expressions of
reducing ability, demonstrated by its low reduction temperatures
main reactions involved in pyrometallurgical processing of EAF dust
in Table 4. As a matter of fact, many of the metal extraction pro-
were determined by the FactSage™ software [version 7.0, Thermo-
cesses involve use of both reducing agents (Zhang et al., 2000a,b).
fact/CRCT (Montreal) and GTT-Technologies (Aachen), Federal Uni-
This statement is particularly true when the dust has a high carbon
versity of S~
ao Carlos] and the results are summarized in Table 4.
content or carbonaceous materials are added as reducing agent. In
As shown in Table 4, zinc oxide, ferrous oxide, lead oxide,
such case, the reduction initially depends on the degree of contact
chromium trioxide and cadmium oxide can be reduced into
Fig. 2. Electron micrograph of EAF dust showing fine dust particles (Simonyan et al., 2015).
Fig. 3. Scanning electron micrograph and elemental distribution image of EAF dust (Sofilic et al., 2004).
between carbon and the dust particles where the solid/solid reac- 5. Pyrometallurgical processes for recycling of EAF dust
tion occurs, and there are very low vapor partial pressures of CO
and metals (e.g., zinc, lead and cadmium). With gradual con- For treatment of EAF dust, many pyrometallurgical processes
sumption of carbon in reduction of the metal oxides, however, the have been developed or are under development. In the present
contact area between carbon and metal compounds decreases. On study, the Waelz kiln process, rotary hearth furnace (RHF) process,
the contrary, the CO partial pressure increases steadily with PRIMUS process, OXYCUP process, coke-packed bed process, Aus-
involvement of Boudouard reaction. Consequently, the solid/solid melt process, electric smelting reduction furnace (ESRF) process,
reduction reaction becomes more difficult and the reduction re- Plasamadust process, plasma-arc process, Elkem multi-purpose
actions between CO and the metal oxides in the dust dominate the furnace (EMPF) process, submerged plasma process, pig iron zinc
extraction process. Hence, for recycling of EAF dust via carbother- oxide (PIZO) process, flame reactor process, thermal plasma
mic reduction, accelerating gasification of carbon and mass transfer reduction process, microwave processing, solar thermal reduction
of CO is crucial and is worthy of extensive exploration. process, iron bath smelting process, calcification process and
halogenation process are covered and reviewed. A brief comparison
of these pyrometallurgical processes is shown in Table 5. It should
be mentioned that before the pyrometallurgical step, zinc enrich-
ment is also important and sometimes very necessary. In fact, a few
relevant methods have been developed. For example, the EAF dust
injection technology, in which the dust is injected into EAF,
considerably reduces the total amount of dust. Most of the zinc in
the injected dust is returned to the dust fraction in the furnace
atmosphere whereas the rest dissolves in the slag. The zinc accu-
mulates in the EAF filter dust which therefore becomes more
attractive for metal recovery without negative effect on dust
emissions or steel quality (Evans and Hogan, 1987; Jensen and Wolf,
1997; Tsubone et al., 2012). Isozaki et al. (2002) proposed a method
to separate and recover iron and zinc from EAF exhaust gases using
a coke bed filter and a zinc condenser to prevent the formation of
the dust, eliminating the need for its costly recycling processes. The
exhaust gas from EAF passes through the coke bed filter maintained
at 1000 C. The zinc and lead vapors after reduction are collected
and separated in the downstream condenser, which rapidly cools
Fig. 4. TGA profile of EAF dust (Al-Harahsheh et al., 2014). the gas from 1000 C to about 450 C. Condensed zinc and lead
Table 4
Gibbs free energy expressions of main reactions involved in pyrometallurgical processing of EAF dust.
No. Reaction DGQ ¼ A þ BT Reaction Enthalpy Classification

temperature change DHQ
298
A (J mol1) B (J mol1K1) ( C) (kJ mol1)
1 ZnO(s)þC(s) ¼ Zn(g)þCO(g) 362,944.64 295.31 955.88 370.35 Carbothermic reduction (Waelz kiln, RHF,
2 ZnFe2O4(s)þC(s) ¼ Zn(g)þFe(s)þCO(g) 855,953 804.09 791.35 872.19 PRIMUS, OXYCUP, coke-packed bed,
3 PbO(s)þC(s) ¼ Pb(l)þCO(g) 98,050.00 170.28 302.10 113.16 Ausmelt, ESRF, Plasmadust, plasma-arc,
4 CuO(s)þC(s) ¼ Cu(l)þCO(g) 52,337.00 181.52 15.18 57.39 EMPF, submerged plasma, PIZO, flame
5 MnO(s)þC(s) ¼ Mn(s)þCO(g) 272,315.01 160.21 1426.59 274.40 reactor, iron bath smelting, thermal plasma
6 3Fe2O3(s)þC(s) ¼ 2Fe3O4(s)þCO(s) 132,495.49 223.46 319.78 132.03 reduction, microwave processing, and solar
7 Fe3O4(s)þC(s) ¼ 3FeO(s)þCO(g) 197,349.71 203.55 696.39 209.38 thermal reduction)
8 FeO(s)þC(s) ¼ Fe(s)þCO(g) 151,872.55 151.94 726.41 155.31
9 ZnO(s)þFe]Zn(g)þFeO(s) 211,089.01 143.40 1198.88 215.05
10 C þ CO2(g) ¼ 2CO(g) 171,143.98 174.76 706.16 172.47
11 ZnO(s)þCO(g) ¼ Zn(g)þCO2(g) 191,800.66 120.55 1317.90 197.89
12 ZnFe2O4(s) þCO(g) ¼ Zn(g)þFe(s)þCO2(g) 174,271 108.64 1330.96 182.31
11 PbO(s)þCO(g) ¼ Pb(l)þCO2(g) 62076.00 14.54 e 59.31
12 CuO(s)þCO(g) ¼ Cu(l)þCO2(g) 118807.03 6.76 e 115.08
13 MnO2(s)þ2C(s) ¼ Mn(s)þCO(g) 294,473.41 355.52 555.14 299.02
14 3Fe2O3(s)þCO(g) ¼ 2Fe3O4(s)þCO2(s) 38648.00 48.70 e 40.40
15 Fe3O4(s)þCO(g) ¼ 3FeO(s)þCO2(g) 26,206.00 28.79 637.10 36.91
16 FeO(s)þCO(g) ¼ Fe(s)þCO2(g) 19288.00 22.85 570.96 17.16
17 CrO3(s)þ3C(s) ¼ Cr(s)þ3CO(g) 240,039.35 515.58 192.42 246.65
18 CrO3(s)þ3CO(g) ¼ Cr(s)þ3CO2(g) 273392.59 8.70 31,151.28 270.76
19 FeCr2O4(s)þC(s) ¼ Fe þ Cr2O3þCO(g) 222,429.50 167.54 1054.47 220.48
20 CdO(s)þC(s) ¼ Cd(g)þCO(g) 251,964.01 288.92 598.94 260.26
21 CdO(s)þCO(g) ¼ Cd(g)þCO2(g) 80,820.00 114.16 434.80 87.79
22 (ZnO)þ[C] ¼ Zn (g)þ CO(g) 308,552.64 271.12 864.92 315.96 Carbothermic reduction (OXYCUP, coke-
23 (PbO)þ[C] ¼ Pb(g)þ CO (g) 267,096.13 257.22 765.25 277.21 packed bed, Ausmelt, ESRF, Plasmadust,
24 (FeO)þ [C] ¼ [Fe] þCO(g) 138,772.78 143.70 692.56 145.31 Plasma-arc, EMPF, submerged plasma, PIZO,
fame reactor, and iron bath smelting)
25 ZnFe2O4(s)þCaO(s) ¼ Ca2Fe2O5(s)þZnO(s) 23199.00 16.89 e 27.54 Calcification
26 ZnFe2O4(s)þCaCl2(l) ¼ CaFe2O4(s)þZnCl2(g) 201,882.32 125.76 1332.15 214.68 Halogenation
27 Fe2O3þ3CaCl2(l) ¼ 2FeCl3(g)þ3CaO(s) 591,167.98 218.30 2434.90 772.85
28 ZnO(s)þCaCl2(l) ¼ ZnCl2(g)þCaO(s) 209,953.28 120.55 1468.48 223.79
metals are collected in liquid state at the bottom of the condenser, purification. The rotary kiln furnace is used to treat Waelz oxide to
while iron and slag components are collected in the filter. Ma (2011) refine zinc with elimination of lead, cadmium and chlorides
proposed a radical new approach, the In-Process Separation (IPS) (Morcali et al., 2012).
technology, in which zinc is removed from the EAF off-gas before it The Waelz kiln process is considered to be a relatively mature
reacts with iron-containing particles to form the franklinite phase process for recycling of EAF dust in spite of several disadvantages.
in the combustion chamber. The dust collected in the baghouse The major shortcoming of this process is associated with the
filters can be sent directly to the crude zinc oxide treatment plant as remained zinc and lead in the Waelz slag where iron is not suffi-
it will no longer contain Fe. However, this technique requires ciently enriched after separation of zinc in the form of vapor,
implementation in each individual EAF plant. It may be impossible indicating waste of iron units. This problem becomes more serious
to collect the starting product from a larger area to treat a large when the process produces high amounts of slag (about
amount of dust simultaneously (Suetens et al., 2014a,b). 700e800 kg t1 of charged dust) (Antrekowitsch et al., 2015). Also,
as the major aim of this process is to recover zinc, the zinc con-
centration of the dust must be higher than 16 wt% to ensure eco-
5.1. Waelz kiln process nomics of the process (Leclerc et al., 2002). High energy
consumption is another drawback of this process due to its strict
Among all high-temperature metal recovery processes, the dust requirements on the operation temperature of units (Mishra et al.,
processed by the Waelz kiln accounts for about 75% of the total 2002). Moreover, it is an off-site process in which high tipping and
treated EAF dust globally (Mager et al., 2000). Fig. 5 shows a shipping fees ($80-$125 ton1) have to be applied (Sun et al., 2008),
simplified flow chart of Waelz kiln process (Mager et al., 2003). adding cost.
Initially, a homogeneous mixture of EAF dust, reductant and flux is
prepared in the pellet form. The pelletized material is sent into the
Waelz kiln for drying and preheating by the countercurrent-flow 5.2. Rotary hearth furnace process
kiln gas. In the reaction zone, the metal oxides are reduced at
about 1100e1200 C to volatilize zinc and lead from the charge in The rotary hearth furnace (RHF) process is an important coal-
the form of metal vapors. By controlling admission of air at the kiln based direct reduction method for dust recycling (Lu and Huang,
outlet end, zinc and lead in the gas phase are oxidized again and 2003) and has been practiced in the steel industry (Oda et al.,
formed as Waelz oxide, while the metallic iron in the charge is re- 2006). Fig. 6 shows the primary flow chart of RHF process for
oxidized and then constitutes a byproduct called Waelz slag treatment of EAF dust (Tsutsumi et al., 2010). By this process, the
(Coronado et al., 2016). Meanwhile, the process heat liberated can mixture of the dust, reducing agent and additives is first used for
be effectively utilized in the charge. In the process, chlorine and pelletizing (Wu et al., 2013). The green pellets/briquettes prepared
alkalis volatilize together with the heavy metals. The dust-laden are sent into the moving RHF and heated to 1000 C in its heating
off-gas will be treated in a downstream off-gas unit for zone. After they enter into the reaction zone of RHF, a number of
1086
Table 5
Pyrometallurgical processes for treatment of EAF dust.
Process Temperature ( C) Furnace type Inputs Products Scale Capacity References

(kt y1)
Waelz kiln 1150e1200 Rotary kiln Coal, lime/sand, natural gas, air Crude zinc oxide and Fe-slag Commercial 40e250 Piret, 2012
(waste)
RHF 1250e1300 Rotary hearth furnace Coke, binder, and natural gas Crude zinc oxide and DRI/hot Commercial 100e300 Nakayama and Taniishi, 2011
briquetted iron (HBI)
PRIMUS 1000e1100 Multiple hearth furnace Coal and air Crude zinc oxide and DRI/iron Commercial 100 Roth et al., 2001; Suetens et al.,
concentrate 2014a,b
OXYCUP 1500e1600 Cupola Coke, scrap, and bricks Crude zinc oxide, pig iron, and slag Commercial 200 Holtzer et al., 2015
(waste þ cement þ C)
Coke-packed bed 1500e1600 Shaft furnace Coke, fluxes, and O2-enriched Crude zinc oxide, molten metal, and Commercial 10 Hara et al., 2000; Suetens et al.,
air slag 2014a,b
X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100

Ausmelt 1250e1300 Top submerged lance furnace Coal and O2-enriched air Crude zinc oxide, and Fe-slag Commercial 100 Hoang et al., 2009
(waste)
ESRF 1300e1500 EAF Binder, air, and electricity Crude zinc oxide, pig iron, and slag Commercial 36 Nakayama, 2012
Plasamadust 1400e1600 Shaft furnace equipped with Coke, coal, fluxes and Crude zinc oxide, molten iron, and Commercial 10e20 Schoukens et al., 1993; Suetens
plasma devices superheated plasma gas slag et al., 2014a,b
Plasma-arc 1400e1600 Plasma arc furnace Coal, air, and electricity Crude zinc oxide, molten iron, and Commercial 5e40 Schoukens et al., 1993; Denton
slag et al., 2005; Suetens et al.,
2014a,b
EMPF 1400e1600 Slag-resistance furnace Coal and air Crude zinc oxide, molten iron, and Commercial 40 Schoukens et al., 1993;
slag Kennedy et al., 2009; Suetens
et al., 2014a,b
Submerged plasma 1300e1400 Submerged plasma reactor Coke, natural/petroleum gas, Crude zinc oxide and Fe-slag Commercial 40e60 Verscheure et al., 2007a,b
flux, air, and electricity (waste)
PIZO 1300e1500 Induction furnace Coal, air, electricity Crude zinc oxide, pig iron and slag Commercial 50 Bratina and Lenti, 2008
Flame reactor 1600 Flame Reactor Natural gas, O2-enriched air Crude zinc oxide, molten metal, and Commercial 30 Orhan, 2005
slag
Thermal plasma 1000e1400 Plasma arc furnace Natural gas/CO, electricity Crude zinc oxide and Fe-rich slag Lab e Best and Pickles, 2001;
reduction for steelmaking Magdziarz et al., 2015
Microwave processing 1000e1200 Microwave furnace Coke/coal, air, electricity Crude zinc oxide and DRI Lab e Sun et al., 2008; Zhou et al.,
2015
Solar thermal reduction 800e1350 Solar furnace Graphite, silica, and sunlight Zinc, crude zinc oxide, and slag Lab e Schaffner et al., 2003;
Tzouganatos et al., 2013
Iron bath smelting 1400e1500 e Coal/silicon, fluxes, and heat Crude zinc oxide, molten metal, and Lab e Chen and Gammal, 2000; Grillo
slag et al., 2014
Calcification 900e1100 e CaCO3/lime, O2-enriched air, Crude zinc oxide and Ca2Fe2O5 for Lab e Itoh et al., 2008; Chairaksa-
and heat use in blast furnace Fujimoto et al., 2015
Halogenation 875e1050 e PVC and heat ZnCl2 and Fe þ C pellets Lab e Guo et al., 2010
Fig. 5. Flow chart of Waelz kiln process (Mager et al., 2003).
Fig. 6. Flow chart of RHF process for treatment of EAF dust (Tsutsumi et al., 2010).
high temperature chemical reactions take place and the overall broken pellets and fines which must be returned to the pelletizing
temperature can reach up to 1300 C. During the process, the metal step, thereby lowering the process productivity. Moreover, due to
oxides are reduced to the corresponding metallic forms. Zinc and the large initial investment in equipment, the economic benefits of
lead are separated from the pellets in the form of vapor and sub- the process have to be enhanced further, especially at the early
sequently enter into the exhaust pipe. The metal vapors are stage of its operation.
oxidized to zinc oxide and lead oxide, respectively, along with the
movement of waste gas, and collected by the dust collector in the 5.3. PRIMUS process
form of soot. During the process, alkaline metal chlorides are
removed simultaneously. The iron oxides are reduced into direct The PRIMUS technology involves use of multi-hearth furnace for
reduced iron (DRI) under strong reducing atmosphere and the metallization of non-agglomerated finely dispersed EAF dust
percent reduction of DRI reaches up to 90% in 15e20 min (Frieden et al., 2001), as shown in Fig. 7. The furnace consists of a
(Kuwauchi and Barati, 2013). cylindrical chamber on a vertical axis, with multiple superimposed
The RHF direct reduction process is deemed effective in pro- or stacked annular compartments between which the hearth
cessing EAF dust containing appreciable amounts of iron, carbon, floors/roofs are constructed of refractory bricks which form self-
zinc, lead and alkalis. With the process, high-grade zinc product supporting levels with openings. In practice, a mixture of pulver-
and DRI can be produced instead of slag. It was therefore claimed ized coal and EAF dust is charged at the uppermost hearth and
that this process may be commercially and environmentally su- transported from one hearth to the next and from the center to the
perior to the Waelz kiln technology (Nakayama and Taniishi, 2011). wall and back with the aid of scrapers. The processing temperature
The iron metallization degree, zinc removal ratio and alkali metals can be elevated from ambient temperature to 1100 C by the
(K and Na) removal ratios may exceed 75%, 95%, and 80%, respec- combustion of coal in burners and by the secondary combustion of
tively, for the reduced pellets/briquettes under the condition of the CO formed during reduction. At high temperatures, zinc and lead
molar ratio of carbon to oxygen equals 1.0 at 1230 C for 15 min. The compounds are reduced to their metallic forms, evaporated, re-
downside of this process, however, is due to the requirement for oxidized by the furnace gas, removed from the furnace through
the charge. Until recently, the RHF process was only suited for the exhaust port and collected in the gas-cleaning system (bag
recycling EAF dust with low zinc content (<5 wt%) (Suetens et al., filter) with the recovery degree of 95%. Meanwhile, alkaline com-
2014a,b) although this technology has been reengineered to over- pounds are vaporized and captured. At the bottom of the furnace
come operational problems such as zinc oxide blockages at higher DRI or iron concentrate with degree of metallization 90e95% is
zinc content, mainly associated with low compressive strength of discharged, cooled and used for BF smelting or EAF steelmaking
the pellets/briquette which may result in substantial amount of (Kurunov, 2012). In this way, separation of iron from zinc and lead
Fig. 7. Flow chart of PRIMUS process for treatment of EAF dust (Frieden et al., 2001).
and other elements such as sodium and potassium as well as operated with an oxygen-enriched blast (5e15% of oxygen enrich-
chlorine is realized. ment) (Fisch and Kesseler, 2006; Holtzer et al., 2015), as shown in
The PRIMUS process is featured by unprepared and low-cost Fig. 8. The briquettes are charged into the furnace with fluxes and
feed, rapid reduction of metal oxides due to intensive stirring and large pieces of scrap (up to 1 m). Coke and carbon fines are used as
heating, high efficiency with relatively low process temperatures fuels. In particular, coke provides most of the energy source for the
(1000e1100 C) and excellent quality products, including highly furnace and guarantees the permeability of stock column. At low
metallized DRI (>90%) and highly concentrated zinc oxide which temperatures (c.a. 500 C), portions of metallic iron are formed on
enable selective extraction of the zinc (Roth et al., 2001; Suetens the external surface of briquettes. This coating grows and protects
et al., 2014a,b). The downside of this process is associated with briquette against decomposition beyond 1000 C when the direct
the corrosion of furnace due to both rapid stirring and evaporation reduction by carbon contained in briquettes initiates. In contrast to
of alkaline compounds during reduction. Meanwhile, to keep good blast-furnace smelting, most iron in the OXYCUP process is reduced
kinetic conditions for the charged feed, the furnace has a restricted by carbon in the briquettes at 900e1400 C in a short period of time
size which restrains its productivity, as indicated in Table 5. (20e30 min) (Kurunov, 2012). At temperatures above 1450 C bri-
quettes completely convert into spongy iron, which is melted
5.4. OXYCUP process together with the metallic charge loaded to the furnace. Molten
metal containing 4 wt% carbon is tapped continuously at 1500 C.
The OXYCUP process, developed by Kuttner GmbH& Co., melts Overall, the process produces “zero waste” (Holtzer et al., 2015).
self-reducing briquettes by vibropressing EAF dust, sludge and The resulting pig iron of precisely known quality is delivered to the
scale generated in steelmaking with a cement binder in a cupola steel plant. The slag is granulated and the cleaned top gas rich in CO
Fig. 8. Section view of OXYCUP furnace (Wang et al., 2015).

is used as a fuel. The top dust is recycled into briquettes and sold as crude zinc oxide, molten metal, and slag. By treating a typical EAF
zinc concentrate (crude zinc oxide) with sufficiently high zinc dust containing 27.7 wt% zinc, 25.0 wt% iron and 3.22 wt% lead, it
content (e.g., 30 wt%). was found that zinc and lead were concentrated in the crude zinc
The OXYCUP process shows a good combination of the function oxide (60 wt% zinc and 6.2 wt% lead) and their contents in the metal
of melting in traditional cupolas and that of reduction in BF, thereby (0.005 wt% zinc and 0.001 wt% lead) and the slag (0.01 wt% zinc and
useful for both high- and low-zinc burdens. It is expected to remedy 0.001 wt% lead) were very low (Hara et al., 2000).
some major defects of traditional processes such as Waelz kiln The coke-packed process has advantages of efficient separation
process (Holtzer et al., 2015). In general, this process produces hot of various metals such as zinc, lead and iron. However, the smelting
metal with lower cost than that from BF. It is also an environ- reduction consumes a huge amount of heat. In practice, it is
mentally friendly approach for EAF dust treatment as emissions of necessary to elevate the temperature to over 1550 C at the level of
sulfur oxides, nitrogen oxides, dioxins and furans are below the the lower tuyeres, which supply the majority of heat, to completely
allowable values. Like those in BF smelting (Hryniewicz and reduce metal oxides. Also, it is crucial to prevent the zinc adhesion
Janewicz, 2008; Magdziarz et al., 2011, 2015), the prepared charge on the wall of the furnace top. Further efforts should be made to
should have sufficient strength to sustain the reduction process. maintain top gas temperature and CO2/CO in the region where zinc
However, information concerning the reduction of the briquettes vapor is stable (Hara et al., 2000).
composed of EAF dust in the process is insufficient. To improve the
furnace operation, more efforts should be spent on illustrating the 5.6. Ausmelt process
reduction process in the furnace in association with the physico-
chemical properties of the charge. EAF dust can be treated using the Ausmelt technology (Hughes
et al., 2008). In this technology, the granulated mixture consisting
5.5. Coke-packed bed process of EAF dust, reducing agent and additives is sent into the Ausmelt
furnace from a lid plug without drying (Hughes et al., 2008). The
The coke-packed process is a smelting reduction process using a powdered coal and fuel gas are injected into welding pool by a
shaft furnace with a coke packed bed for recycling of steelmaking spray gun to maintain the temperature of furnace at about 1300 C.
dust (e.g., EAF dust) developed by Kawasaki Steel Corp (Itaya et al., The melting temperature of EAF dust usually ranges from 1250 to
1990). The furnace is featured by installation of two stage tuyeres, 1400 C. After zinc oxide and lead oxide are reduced to their
namely upper and lower tuyeres (Fig. 9). Fine raw materials (EAF metallic forms at about 1100 C, the metals will volatilize and re-
dust, flux and coke) without agglomeration are injected through oxidize to their corresponding oxidized forms due to reactions
the upper tuyeres and then melted instantly in the raceway inside with the air above the molten pool (Zhou, 2002). These oxides are
the shaft furnace. Because of efficient heat exchange between the collected in a bag filter chamber before further treatment and
ascending gas and the descending coke in the furnace, a high recycling (Matusewicz and Mounsey, 1998).
temperature and intensively reducible region is formed between The advantage of the process is ascribed to its good aerodynamic
the upper and lower tuyeres. The melted oxides in the dust are condition which can promote the reduction of zinc and lead oxides
easily reduced to metals as they drip through the high-temperature and volatilization of zinc and lead but hinder the reduction of iron
coke-paced bed. When the molten metals (e.g., iron, chromium and oxide by controlling the atmosphere and temperature. This feature
nickel) and slag drop to the hearth, high-vapor-pressure elements allows potential reduction in the energy consumption of the dust
including zinc and lead are vaporized and extracted through the treatment with the removal ratio of zinc amounting to 65%e75%
furnace top. As shown in Table 5, the process has three products: (Yin, 1998). However, the relatively low purity of zinc soot in the
Fig. 9. Flow chart of coke-packed bed process for treatment of EAF dust (Hara et al., 2000).
Fig. 10. Flow chart of ESRF process for treatment of EAF dust (Nakayama, 2012).
process and insufficient productivity due to complex bed opera- metal prices increase and environmental regulation becomes more
tions restrain its development. severe.
5.7. ESRF process 5.8. Plasamadust process
The ESRF process simply uses an electric furnace for material The Plasmadust process is carried out in a coke-filled shaft
heating and oxide reduction (Nakayama, 2012). Fig. 10 shows the furnace equipped with D.C. non-transferred plasma devices (e.g.,
primary flow chart of ESRF process for treatment of EAF dust. In this three 6 MW plasma generators) (Schoukens et al., 1993). These
process, a mixture of agglomerated EAF dust, coke and limestone as devices are mounted on the tuyeres of the shaft through which
material charge is loaded into the furnace. Carbon monoxide and Zn EAF dust, pulverized coal, fluxes and superheated plasma gas are
vapor in the exhaust gas are oxidized in the combustion chamber (a injected. The high temperatures (around 2500 C in the raceway
simple vertical cylinder) with water-cooled and partially formed in front of each tuyere) and low oxygen partial pressure in
refractory-lined wall which prohibits the adhesion of softened dust the furnace enable the reduction of iron and chromium oxides at
and facilitates cleaning. Powders of iron oxide and carbon settled at 1400e1600 C, which is difficult for many traditional fuel-air
the bottom of the combustion chamber are recycled to the ESRF. based processes, e.g., the Waelz kiln process. Molten iron with
Hot exhaust gas containing much crude zinc oxide and chlorides is various metallic species and a nonhazardous slag are tapped at the
withdrawn from the combustion chamber and quickly cooled lower part of the furnace. One of the main shortcomings of this
through the multi-tube gas cooler for recovering the particles in the process is the relatively low zinc content (about 20 wt%) in the
bag-house. The temperature of the gas cooler is controlled to so- crude zinc oxide produced from the process which needs to be
lidify the chlorides on the vertical tube surface. By removing the processed further in a high-temperature furnace, such as Waelz
chlorides a good zinc oxide recovery from crude zinc oxide with kiln.
65e82 wt% zinc oxide can be achieved. High-carbon pig iron
(3.44 wt% carbon) is returned to arc furnace steel mills. Slag with 5.9. Plasma-arc process
0.44 wt% zinc and 0.03 wt% lead is cooled down slowly in a slag pot
to generate a crystallized structure with very low leaching values of There are two alternatives of plasma-arc process for treatment
heavy metals such as zinc, lead and cadmium, simplifying down- of EAF dust, namely the Tetronics and Enviroplas processes
stream disposals such as landfill or use as aggregate for construc- (Schoukens et al., 1993; Goff and Denton, 2004; Denton et al.,
tion (Nakayama, 2012). 2005). The former process was developed by Tetronics Research
The ESRF process is characterized by the use of sole electrical and Development (TRD) in the UK in the late 1970s (Schoukens
energy for heating, melting and reduction without any fuel and by et al., 1993). The feeds, including EAF dust and coke fines, are
the low carry-over of charged dust and high zinc oxide content charged through ports in the roof of a cylindrical D.C. plasma-arc
(over 70%) in crude zinc oxide. When ESRF is installed in an EAF furnace. The temperature of the furnace is maintained by supply-
plant, energy is saved because molten pig iron can be directly ing electric energy via a graphite electrode in the center. During the
charged into the EAF, without use of a casting machine to make process, the metals produced by reduction of oxides of zinc, lead
ingots. Meanwhile, high gas temperature of over 1250 C and cadmium are vaporized, condensed and captured in a zinc
completely decomposes dioxins and other organic substances in splash condenser. A non-hazardous slag is formed and tapped
EAF dust. No hazardous materials remain in the slag. The disad- periodically from the furnace while off-gases are withdrawn from
vantage of this process is the high energy cost. Thermal energy of the furnace continuously. The Enviroplas process is another
the hot exhaust gas is often not actively used, and only a portion of plasma-arc process developed by Mintek based on the carbother-
energy is used for preheating the charged material. It is the main mic and metallothermic reduction of metal oxides in the EAF dust
reason why the process was once abandoned. New ESRF process is at 1400e1600 C in a DC plasma arc furnace (Assis, 1998). The
expected to meet the economic requirements when recovered Tetronics and Enviroplas processes are differentiated by charging
practice. In the Enviroplas process, the feed is transferred to the differences are the use of a three-phase slag-resistance furnace
furnace via the central hole of the graphite electrode while in the instead of a D.C. open-arc furnace and the application of briquettes
Tetronics process it is charged through the ports located in the roof instead of un-agglomerated feeds. Compared with the Enviroplas
of the furnace. Feeding through the hollow graphite electrode in process which has the inherent advantages of a D.C. plasma-arc
the Enviroplas process offers a series of advantages, including direct furnace over an A.C. slag-resistance furnace, the EMPF process
delivery of feed into the high temperature reaction zone under the has relatively higher electrode consumption, lower-symmetry heat
electrode, rapid absorption of EAF dust into the molten slag, and distribution and more complex operation control.
reduced contamination and elutriation or carry-over of the feed
due to minimized interaction of the leaving vapor products with 5.11. Submerged plasma process
feed materials falling down from feed ports in the roof. The ferro-
alloys produced contain relatively small quantities of sulfur and The submerged plasma zinc-fuming process uses electric
phosphorus (about 0.06 wt% and 0.04 wt%, respectively) which plasma torches (plasma generators) to supply process heat and
enable further steelmaking. The slag has less than 0.1% of the zinc good mixing conditions to the slag bath into which a mixture of
input, while the fumes produced contain high grade of zinc oxide pelletized EAF dust, petroleum coke and flux is fed continuously
(on average 56.3 wt%). Due to its large energy requirement, this (Verscheure et al., 2005; Verscheure et al., 2007a,b), as shown in
process has a much smaller capacity, in comparison with the Waelz Fig. 11. Inside the plasma torches, the cold blast air is transformed
kiln process (Table 5). into a high enthalpy plasma gas which is mixed with natural/pe-
troleum gas and injected into the slag bath. The solid feed dissolves
5.10. EMPF process into the molten bath and blast gases react with the slag and
reductant. Zinc and other volatile metals fume off. Above the bath,
The EMPF process for treatment of EAF dust is based on a three- the fume is post-combusted with secondary air, and the resulting
phase slag-resistance furnace characterized by advanced electrode off-gases and solid zinc oxide particles are removed from the
seal designs, gas tight bodies and roofs, and fully cooled slag zones smelting vessel. After the post-combustion the off-gas is further
using plate coolers which generate a frozen-slag (freeze) lining oxidized with air in a radiation chamber and treated in an elec-
(Kennedy et al., 2009). The furnace has high intensity ranging from trostatic precipitator to recover zinc oxide. Part of the heat gener-
300 to 400 kW m2 of hearth area or approximately ated in the post-combustion is transferred back to the slag bath to
300e1000 kW m3 of slag volume. The 10 MW EMPF built at increase energy efficiency of the process. The outputs of the process
Laclede Steel, Alton (IL) has an annual designed capacity of 40 kt of are an iron, calcium and silica-rich slag phase, a matte phase, crude
EAF dust (Schoukens et al., 1993; Kennedy et al., 2009). This process zinc oxide powder (55e65 wt% zinc) and off-gas (Verscheure et al.,
shares several similarities with the plasma-arc process. For 2007a,b).
example, like the Tetronics process, vaporized products withdrawn In the submerged plasma process, the carbon and heat re-
from the furnace are captured in a zinc splash condenser. The main quirements of the process are separated. The molar ratio of carbon
Fig. 11. Flow chart of submerged plasma process for treatment of EAF dust (Popovici, 2009).
to oxygen (C/O) and electrical power can be independently 5.13. Flame reactor process
adjusted to optimize the performance of the furnace. The use of
submerged plasmas also enables high slag bath temperatures The flame reactor process involves use of a flame reactor (a
(around 1300e1400 C) which promote high zinc-fuming rates. A water-cooled vertical cylinder, diameter 0.6 m height 3 m) having
key feature of the process is the use of high temperature freeze an upper combustion zone and a lower smelting zone for EAF dust
linings (a layer of bath material that protects the furnace wall, treatment (Orhan, 2005). In the combustion zone, CO is produced
formed on the reactor wall backed by the water-cooled steel by the partial combustion of natural gas with oxygen-enriched air
furnace shell) to contain this slag bath, designed through the in a cyclone burner at the top of the reactor. The hot reducing flame
control of bath chemistry with use of dolomite flux. Using such (>2000 C) travels down to the smelting zone, where the dust is
freeze linings promotes maximum operation temperatures of injected pneumatically with feed rates of 1e2 t h1 of EAF dust. Due
conventional slag fumers which are restrained by highly super- to the rapid reactions at high temperatures (about 1600 C), the
heated aggressive fayalite slags, in spite of increased enthalpy average retention time of the dust in the flame reactor is only half a
losses to the water cooling system due to the high superheat of the second. Like many of the approaches for management of EAF dust,
slags. The design of these freeze linings is crucial for the technical the oxides of zinc, lead and cadmium in the flame reactor process
and economic feasibility of the process. The use of supplementary are reduced to their metallic forms. The metals undergo vapor-
heat supplied by the plasma torches helps to maintain high bath ization and re-oxidization. Lastly, a crude zinc oxide is collected in a
temperatures and the application of high liquidus temperature bag filter for subsequent metal extraction in electrothermic zinc
slags provides stable freeze linings to keep integrity of the bath plants. The molten slag generated is tapped continuously from the
wall. These features and the reactor design lead to higher zinc- reactor for sale or disposal (Assis, 1998). Overall, this process has a
fuming rates than those achievable using conventional zinc- simple operation, despite a relatively low efficiency which is mainly
fuming processes. The use of hydroelectric power in the plasma restricted by the combustion of fuel in the flame reactor.
offers the opportunity of lowering the environmental impact of
the process through reduced greenhouse gas emissions. Addi- 5.14. Thermal plasma reduction process
tional work is required to simultaneously optimize slag compo-
sition and process performance while ensuring vessel integrity via A representative plasma technology is the Scan Dust AB (Li,
model development (Verscheure et al., 2007a,b). The challenge is 2012). In this technology, flue gas is decomposed into the gas
to engineer or select a slag chemistry which will provide a stable atoms or particles by the electric current on the electrode (copper)
protective furnace lining and also minimize heat losses through produced by the high temperature (approximately 3000 C)
the furnace shell. (Simonyan et al., 2015). The gas atoms or particles generated are
burning in the combustion chamber, making the flame center
temperature reach as high as 20 000 C. When the granulated
5.12. PIZO process mixture consisting of EAF dust and reducing agent is sent into the
plasma furnace, a series of reduction reactions occur at once due to
The PIZO process uses a continuous channel induction furnace the high temperature in the reaction zone. In this process, zinc oxide
as the primary unit for processing of EAF dust (Bratina and Lenti, and lead oxide are reduced to the vapors of zinc and lead which are
2008). The furnace contains a molten iron bath which serves as a condensed as liquid metals outside the furnace condenser. The
heat sink to rapidly heat the charged material, a briquetted mix of mixture of metal vapors is gradually separated in the condenser
EAF dust and reductants. Under high temperature conditions because of the different boiling points of the metals. Meanwhile, iron
(1300e1500 C), reduction of oxides of zinc, lead and cadmium is enriched in slag and discharged from the bottom of furnace.
proceeds quickly, followed by that of iron and other metals. Zinc, A study by Best and Pickles examined the feasibility of recov-
lead and cadmium are vaporized and re-oxidized. The metal oxide ering metals of values from EAF dust containing 24.8 wt% zinc using
dust is collected as crude zinc oxide in a baghouse system. Iron and a 24 kVA AC plasma arc furnace under CO atmosphere between
some other metals which enter into the molten bath are removed 1000 and 1400 C with reaction ratio of 1e8 g L1 (dust feeding rate
by rotating the furnace forward and pouring the bath through a to CO flow rate) and dust feeding rate of 50e150 g min1 (Best and
teapot spout into a receiving ladle. The iron product may be sale- Pickles, 2001). The volatile elements (zinc, lead, cadmium, potas-
able after pouring into a pig machine or used directly as hot metal. sium and sodium) were collected in a condenser, whereas the
Remaining materials, including silica, calcium, magnesium and remaining elements (iron and chromium) constituted a slag phase.
aluminum, produce a molten slag which can be removed from the The zinc recoveries reached up to 97%, and the removal of lead
furnace by rotating the furnace backward and used as a slag closely approximated that of zinc, accomplished by either reduction
modifier or road aggregate. of lead oxide which leads to evaporation of lead or volatilization of
The channel induction furnace fits in with the needs of contin- lead-bearing species, namely lead sulfide, lead chloride and lead
uous feed of raw materials to produce zinc, iron and slag products oxide. The cadmium in the dust was found to be almost totally
which are removed continuously or semi-continuously. The in- recovered in the condensate during cooling of the off-gas phase.
ductors on the furnace serve as an efficient device for providing Simultaneously, exceeding 90% of the alkalis (potassium and so-
energy for the process. All three distinct products of the process, pig dium) were removed primarily due to the volatilization of the salts.
iron, crude zinc oxide and slag, are saleable. Approximately 95% of In addition, a greater potassium removal was achieved associated
the input iron is recovered as pig iron with a much higher market with the higher vapor pressure of potassium chloride compared to
value than the typical iron/slag mix generated from a Waelz kiln sodium chloride (Magdziarz et al., 2015). Most of chromium (>93%),
(The PIZO® Advantage, 2016). Meanwhile, there is very low loss of on the other hand, was remained in the iron-rich phase because of
iron product to the crude zinc oxide (<1.5 wt% iron in the oxide) and high stability of chromium oxides and low equilibrium partial
to the slag (Bratina and Lenti, 2008). Hence, the process reduces the pressure of chromium-bearing compounds. In principle, the iron-
loss of iron and provides a better feed material for downstream zinc rich slag could be reclaimed to the steelmaking circuit.
processing operations. For further improvement of the PIZO pro- The plasma technology provides more effective recovery of zinc
cess, up-scaling its capacity with minimized energy consumption and iron, in comparison with other approaches such as the Waelz
and environmental impact is ongoing. kiln process. It can be used in large or small operations because of
its compact equipment, short payback period of investment, high consisting of an upper cavity and a lower cavity, separated by a
efficiency, environmental friendliness, operation flexibility and 170 mm-diameter 5 mm-thick SiC-coated graphite plate
special advantage of recovering the valuable metals such as chro- (Tzouganatos et al., 2013). The upper cavity received concentrated
mium (Huaiwei and Xin, 2011). Currently, the main problem of this solar irradiation which passed through a 65 mm-diameter circular
technique is ascribed to the determination of the optimum pa- aperture with a 2 mm-thick quartz window. The lower cavity was
rameters of the reactionary zone and velocity of process for an octagonal enclosure (diameter 135 mm height 170 mm) which
maximum extraction of zinc and lead. This issue is particularly served as the reaction chamber containing a packed bed of solid
important for scaling up the plasma process because it is operated reactants. With this arrangement, the concentrated solar radiation
at high temperatures, implying great energy consumption. Further, was efficiently adsorbed by the top of the packed bed.
there exists a relatively strict requirement for the property of feed. The technical feasibility of solar thermal reduction has been
In general, highly-dispersed powdered EAF dust is preferred demonstrated in the temperature range 847e1127 C with both
because it fits the needs of the technology. batch and continuous modes of operation (Schaffner et al., 2003),
which extracted up to 99% and 90% of the zinc in the EAF dust,
5.15. Microwave processing respectively. The condensed off-gas products were found to be
mainly constituted by zinc, lead and chlorine. By maintaining the
Microwave processing of materials, featured by volumetric O2 concentration in the furnace below 2 vol%, the zinc oxide
heating, selective heating and non-thermal effects (Peng, 2012), is presence could be minimized.
an advanced alternative to conventional methods because micro- The solar thermal energy was also used for purification of Waelz
wave energy is absorbed at the molecular level and heat can be oxide containing 55e65 wt% zinc in oxidic form from the EAF dust
generated inside materials (Peng and Hwang, 2015). Processing EAF processed in the Waelz kiln process and for extraction of zinc by
dust under microwave irradiation has fast reaction rate, large zinc carbothermic reduction (Tzouganatos et al., 2013). It was shown that
removal ratio and high iron metallization degree, thereby receiving by clinkering the oxide at above 1265 C using a 10 kWth packed-bed
increasing attention. Sun et al. investigated the zinc removal and solar reactor, the content of impurities (e.g., chlorides and fluorides)
metallization of iron as a function of microwave time and carbon in the oxide could be reduced below 0.1 wt%. The clinkered oxide was
addition at microwave power of 1100 W (Sun et al., 2008). Because reduced under solar irradiation using biochar as CO2-neutral
the mixture of EAF dust and carbon powders (20 wt%) was heated reducing agent between 1170 C and 1320 C, which yielded 90 wt%
well in the microwave field, the removal of zinc was near zinc in the condensed product. Incorporation of continuous or semi-
completion in only 12 min, with the highest zinc removal ratio and continuous feeding of reactants and removal of products could
iron metallization degree approaching 99.2% and 100%, respec- further improve product yield and thermal efficiency.
tively. Zhou et al. (2015) also assessed the performance of using The most prominent advantage of solar thermal reduction
microwave energy for recycling of EAF dust. It was found that for process is the minimization of emissions of greenhouse gases and
the sample with 16 wt% graphite irradiated by 10 kW microwaves other pollutants. For further development of the process, particular
for 10 min, the removal ratio of zinc varied between 80% and 90% attention should be paid to optimizing solar reactor with maximum
and the metallization ratio of iron ranged from 40% to 60%. This thermal efficiency and chemical reaction. In fact, the thermal effi-
result was partially attributed to microwave heating which over- ciency of solar system is relatively low (usually <10%) although it
came the barrier of traditional heating model characterized by in- increases with reactor temperatures and feeding rates (Schaffner
ward heat transfer. It was also closely correlated to the magnetic et al., 2003). To obtain high thermal efficiency and chemical con-
ferrites contained in the dust which served as strong microwave version, it is of importance to match the energy absorption rate
absorbers and to the lower processing temperatures associated with the feeding rate of reactants and the kinetics of the reaction.
with smaller reaction activation energy (Zhou et al., 2015).
Obviously, microwave processing offers an efficient choice for 5.17. Iron bath smelting process
treatment of EAF dust. It is actually a result of the good microwave
absorbance of the materials used in processing (carbonaceous The iron bath smelting process was designed to produce hot
materials) and of the components in the dust (e.g., ferrites) (Peng, zinc, lead and iron economically from EAF dust at low capacity with
2012). Hence, an in-depth exploration of microwave absorbing direct use of coal (particularly non-coking coal). By this process, the
properties of iron-bearing and zinc-bearing phases (magnetite, valuable metals can be recovered through forming the alloy with
franklinite, etc.) as well as reducing agents like coal/coke (Peng the melting iron which can be easily separated from the innocuous
et al., 2016, 2017), which depend on their compositions and slag. Chen and Gammal (2000) investigated zinc recovery from EAF
structures (Sebastian et al., 2015), will allow further enhancement dust by bath smelting reduction in a furnace using inert gas as
of metal recovery and treatment efficiency with great environ- protective gas. For zinc and lead volatilization, a certain amount of
mental friendliness via microwave processing. pure iron was first melted at 1400 C in a graphite crucible into
which a mixture of EAF dust and flux with various CaO/SiO2 mass
5.16. Solar thermal reduction process ratios was charged. After the desired time the slag and metal
generated were removed, while secondary dust was collected at the
Solar thermal reduction is a clean technology which can be used roof of furnace. The main reactions between metal oxide in slag and
to recycle EAF dust and other waste materials in a sustainable carbon in melt are shown in Table 4. It was found that the smelting
manner. According to Schaffner et al. (2003), it employed a high- reduction of (FeO) with carbon in the melt was 10e100 times faster
flux solar furnace equipped with a solar chemical receiver-reactor than that with solid carbon or CO gas, revealing precisely the
in which the carbothermic reduction of EAF dust was performed advantage of the process. Both the volatilization degrees of (Zn) and
using concentrated solar energy. For solar thermal reduction, a (Pb) exceeded 99% at 1400 C. After metal-slag separation, iron was
solar concentrating facility was an essential prerequisite. Such fa- enriched in the metallic part in which the zinc and lead contents
cility could offer up to 50 kWth of thermal radiative power at peak decreased from 22 wt% and 1.12 wt%, respectively, to both less than
radiative flux of 11 000 kW m2 by incorporating an array of 10 0.005 wt%.
high-pressure Xe arcs coupled with ellipsoidal specular reflectors Apart from carbon, silicon can also be used for ferrous oxide
(Tzouganatos et al., 2013). The reduction relied on the solar reactor reduction and zinc recovery. Grillo et al. (2014) reported that it was
possible to recover 98% of the Fe in EAF dust and the secondary dust The calcification process shows a high recovery ratio of zinc
collected after the test had a high level of zinc (68 wt%) at 1500 C. because the majority of zinc oxide and calcium ferrite in the dust
Of interest is the ferrous oxide was reduced by carbon in a lesser can be efficiently separated. The by-product of the process, calcium
and slower extent than it was reduced in the presence of silicon. ferrite, may be used in dephosphorization during the process of
The slag was featured by low ferrous oxide and zinc oxide contents, steel making. However, in this process, the large addition of calcium
implying great potential for complete recovery of these oxides. carbonate or calcium oxide, e.g., Ca/Fe > 1.0 (Chairaksa-Fujimoto
It is evident that the bath smelting reduction process has a good et al., 2015), often leads to low zinc oxide yield in magnetic sepa-
separation of the main metals in the EAF dust treatment. However, ration and increased contaminants in the Zn-bearing fraction.
due to the strict requirement for the reduction temperature
(1400e1500 C) which must be maintained to enable melting of the
5.19. Halogenation process
reaction system (Pickles, 2010) the high energy cost of the process
constitutes a major obstacle to its further development.
The halogenation process is based on the reaction between
highly reactive halides (or their derivatives) and non-ferrous metals
5.18. Calcification process in the EAF dust, followed by evaporation of the formed metallic
halides from the solid residue. It can be divided into two main
The calcification process aims at recovering zinc oxide from EAF groups: the chlorination process and the bromination process.
dust by addition of calcium carbonate (Itoh et al., 2008) or lime Recently, the chlorination process has attracted increasing atten-
(Chairaksa-Fujimoto et al., 2015). According to Itoh et al. (2008), the tion. According to Guo et al. (2010), EAF dust was first mixed with
dust and calcium carbonate were initially mixed at an appropriate calcium chloride (CaCl2) powders as chlorinating agent to prepare a
ratio and then pressed into the 10 mm diameter 1.5 g tablet under charge with Zn/Ca molar ratio of unity before it was transferred into
the pressure of about 400 MPa before heating in air for a desired the hot zone of an electric furnace within flowing purified N2 gas
holding time at temperature of 900 C or 1100 C. In the reaction between 875 and 1050 C. Under this circumstance, zinc, iron and
zone, the franklinite, the main zinc-bearing component in EAF dust lead were respectively chlorinated to ferrous chloride, lead chloride
reacted with the calcium oxide, producing zinc oxide and calcium and zinc chloride by calcium chloride. Due to the high vapor
ferrite (Ca2Fe2O5). Because of the remarkable difference between pressures of zinc chloride and lead chloride, they were easy to
the magnetic susceptibility of zinc oxide and that of calcium ferrite, volatile and remove at low temperatures. Iron, on the other hand,
they could be separated under a high gradient magnetic field. It was remained in the dust residual phase in the form of oxide. The re-
reported that 95% of the zinc oxide in the dust was recovered in covery ratio of zinc could reach 80% in the temperature range from
spite of approximately 6 wt% calcium ferrite contamination. 875 C to 1050 C. Fig. 12 shows a schematic of the reaction be-
Another benefit of this process is the preferential volatilization of tween zinc ferrite powders and calcium chloride (Guo et al., 2010).
lead, chloride and fluorine in the EAF dust (Chairaksa-Fujimoto It is observed that the zinc ferrite particles are wrapped by the
et al., 2015). Most of lead and chloride were removed preferen- molten calcium ferrite and the chlorination reaction occurs at the
tially at temperatures below 900 C, whereas complete removal of solid-liquid interface. The zinc chloride dissolves in the liquid
fluorine occurred above 1000 C in the presence of calcium oxide. In membrane of calcium chloride and volatilizes at the interface
the process without addition of calcium oxide, on the other hand, before the product layer of calcium ferrite is continuously
the evaporation of halogens and lead in the dust began at tem- increasing and enriched in the residue for further removal.
peratures higher than 560 C and drastically increased at about Apart from calcium chloride, hydrogen chloride (HCl) gas
900 C (Chairaksa-Fujimoto et al., 2016). Most of the chloride, evolved from organic waste (Lee and Song, 2007), such as polyvinyl
fluorine and lead were removed from the remaining dust at 1100 C chloride (PVC), is used as a chlorinating additive to assess the
(Chairaksa-Fujimoto et al., 2015). feasibility of recycling EAF dust for metal extraction (Zhang et al.,
Fig. 12. Schematic of reaction between ZnFe2O4 and CaCl2 (Guo et al., 2010).
2000a). During the processing of the mixture of EAF dust and PVC, of occurrence of iron-, zinc-bearing and other minor phases in the
the metal oxides in the dust are converted to metal chlorides and dust. For instance, it was shown that zinc oxide can restrain the
recovered in the gaseous form (Zhang et al., 1999). The dust serves reduction of iron oxide, but the competing effect of reduction of
as a viable treating agent for harmless incineration of PVC which, on zinc oxide and iron oxides are not well illustrated based on the both
the other hand, produces hydrogen chloride through thermal thermodynamic and kinetics analyses (Machado et al., 2006). The
decomposition in recovering metals from waste stream. After water activities of these oxides (e.g., zinc oxide and ferrous oxide) may
leaching, the metals are separated (Sofili c et al., 2004). also be decreased apparently due to the existence of spinel phases
Based on a similar mechanism, the bromination process makes Fe3-xCrxO4 and ZnFe2O4, which shows the close association of these
use of the reaction between reactive bromide with zinc- and lead- metals. Secondly, non-ferrous metals, such as Zn, are easy to
bearing phases in the EAF dust. By this route, Grabda et al. inves- vaporize and separate from a Fe-rich phase, but they are usually re-
tigated recycling of EAF dust in the presence of bromine-containing oxidized in many processes and, therefore, the gaseous product of
plastic waste, namely tetrabromobisphenol A (TBBBPA) and tetra- the dust processing is often a crude oxide which requires further
bromobisphenol A diglycidyl ether (TBBPADGE), which released treatment and thus additional input of energy. Thirdly, because
reactive HBr gas during thermal decomposition (Grabda et al., certain non-ferrous metals and hazardous elements remain in the
2014). When the mixture of the dust and TBBBPA/TBBPADGE was process fume/residue, their disposal may constitute a big puzzle
compressed into pellets and heated at 550 C for 80 min under and sometimes pose harsh requirements on operation apparatus.
oxidizing or inert conditions, high separation of zinc and lead from As mentioned above, the majority of the pyrometallurgical pro-
the dust was achieved. Particularly, in the case of TBBPADGE, a cesses focus only on recovery of zinc, lead and iron from EAF dust in
maximum of 85% of zinc and 81% of lead could be recovered. which other hazardous elements such as chlorine and chromium
The halogenation process is highly selective in separating metal were not explored adequately (Bruckard et al., 2005).
elements, mainly Zn and Pb, in the dust and meanwhile enriches Fe To tackle the first problem for desirable extraction of these
in the residual phase. With this process, the reaction temperature metals, more efforts should be directed to the formation and
may be reduced considerably regarding the low boiling points of decomposition of the spinel phases and separation of the metals
the metal chlorides or bromides. In addition, the reduction furnace based on the exploration of properties of the ferrites (Zhang et al.,
is unnecessary in the process. The biggest concern about this 2000a,b). It was reported that inside the off-gas ducts of EAF the
technology, however, is the addition of halides which, as expected, spinel phases such as franklinite forms through a gas-solid reaction
often causes corrosion of apparatus and poses a potential envi- starting from pure Fe droplets and Zn vapor (Nedar, 1996). The
ronmental threat in the subsequent operations. amount of the spinel phases at room temperature generally de-
creases with increasing zinc and manganese contents in the dust.
6. Discussion Conversely, it increases with increasing iron content. Hence, from
the point of view of efficient metal extraction, the first choice for
As a typical by-product of electric arc furnace steelmaking, EAF pyrometallurgical processing is to eliminate the formation of spinel
dust contains a variety of valuable elements (iron, zinc, lead, etc.). phases, which can be achieved by reducing the oxygen potentials,
Its chemical/phase composition and fine granularity are compatible operating EAF under airtight conditions (Nedar, 1996), increasing
with pyrometallurgical recycling. As aforementioned, most of py- dust loading, or using additives such as calcium oxide and its de-
rometallurgical processes are based on the carbothermic reduction rivatives (e.g., CaF2) (de Araújo and Schalch, 2014). It should be
of metal oxides in the dust, primarily aiming at recovering zinc, lead pointed out that although the presence of CaO (in the form of lime
and iron. Zinc oxide as a main zinc-bearing phase is easy to reduce, or calcium carbonate) can thermodynamically reduce the amount
while the other major phase, zinc ferrite, must decompose to zinc of spinel at 1100 C through the formation of various calcium fer-
oxide first under reducing atmosphere before reduction thereafter. rites (e.g., CaO.Fe2O3 and 2CaO.Fe2O3) which results in the libera-
Because a significant amount of gaseous zinc can be formed at tion of zinc oxide and iron oxide, thereby increasing the non-
temperatures above 1000 C, the effective removal of zinc from EAF ferrous metal recoveries (Pickles, 2008a,b), the appropriate use of
dust is feasible at a temperature of 1000e1100 C. Unlike zinc oxide, the additive deserves special attention in view of its sensitive dose
the lead oxide starts to reduce to its metallic state at 650 C and dependence of relevant phase transformations. Currently, such
begins to evaporate and convert into a gas phase at 900 C. As dependence can be partially revealed by several advanced micro-
expected, these reduction reactions can be accelerated with scopy technique (Denning et al., 2016; Payton et al., 2016). In fact,
increasing temperature. After separation of zinc and lead, iron in after all of the ferrite spinel disappears, the amount of zinc oxide
the dust is enriched in the residue for further treatment. remains relatively constant but that of iron oxide decreases as the
Based on the above principles, the Waelz kiln process, RHF amount of calcium ferrite continues to increase. In EAF dust,
process, PRIMUS process, OXYCUP process, coke-packed bed pro- however, the amount of calcium ferrite is relatively low despite a
cess, Ausmelt process, ESRF process, Plasamadust process, plasma- relative large amount of calcium oxide. This is a result of the slow
arc process, EMPF process, submerged plasma process, PIZO pro- kinetics of reactions involving solid calcium oxide (Zhang et al.,
cess and flame reactor process (Table 5) have been successfully 1999), which warrants extra consideration. From the perspective
used in industry. Meanwhile, some unconventional methods with of decomposition of the spinel phases and separation of the metals,
higher processing efficiency and metal recovery, such as microwave the preliminary thermodynamic analysis of carbothermic reduction
processing and solar thermal reduction process, are being devel- of spinel phase implied that relatively high temperatures and low
oped for further optimization of treatment of EAF dust in a more (oxygen) pressure favor high zinc and lead recoveries, while low
sustainable way, representing future directions of technological temperature and relatively high total pressure/high reactant ratio
innovation and development in pyrometallurgical recycling of the are of benefit to high metallic iron recovery (Wu et al., 2014).
waste. Therefore, reducing the total pressure and introducing non-reactive
Despite apparent progress in this field, there still exist several gas may contribute to increased non-ferrous metal recoveries and
technical challenges/problems. One of the most important de- decreased metallic iron recovery. Further separation of zinc, lead
ficiencies of the current research which, to some extent, restricts and other non-ferrous metals can be realized by controlling pro-
the development of technologies for EAF dust treatment is the cessing temperature and reactant ratios considering the difference
insufficient exploration of the properties and complex association in their thermodynamic stability (Pickles, 2007).
To prevent metal re-oxidation during cooling, it is important to remove chlorine and fluorine compounds simultaneously, sepa-
ensure the reducing atmosphere in the whole process using a rating these halides in an oxidizing step at about 1150 C for
suitable reducing agent which simultaneously reduces its CO2 150 min (also known as clinkering) prior to reduction of remaining
footprint. One option is substituting fossil raw materials (e.g., coal residue seems reasonable in spite of loss of a small amount of
and coke) with carbon-neutral ones based on biomass, such as valuable metals (Hung et al., 2012). It was reported that a very high
biochar (Griessacher and Antrekowitsch, 2012). This reductant has amount of chlorine (>90%) was removed and similar results were
a high gasification efficiency and faster reduction speed which help obtained for fluorine. Further optimization of halides removal relies
to maintain the atmosphere in the reduction process. It is also on an in-depth exploration of the basic knowledge on the behaviors
characterized by very low impurity (e.g., sulfur and phosphorus) of relevant elements. In particular, it is necessary to establish a
contents and carbon neutrality, producing much less pollution to competent thermodynamic database from which the behaviors of
the environment. Obviously, the economics of the new processes halogens and heavy metals (e.g., saturated vapor pressures of heavy
involving biomass-based materials depend on many factors, such metals and their partition in the fume/residue system) as well as
as biomass availability and price, costs for biomass conversion, their interactions in a specific process can be inferred and
effectiveness of the carbon-neutral reducing agent, development of identified.
carbon taxes and additional costs arising from environmental From the above discussion, chromium usually retains in the
legislation in future. Other than solid reducing agents, gaseous re- residue due to high stability of the chromium oxides and low
ductants including CO and H2 may be employed to prevent the re- equilibrium partial pressure of the chromium-containing com-
oxidation of the metals. It was proposed that by using CO gas as a pounds over the temperature range from 1000 to 1400 C. Hex-
reducing agent for recycling of EAF dust, an iron-rich residue with avalent chromium in the EAF dust has 100-fold more toxicity than
an iron grade of 89.9 wt% and metallization degree over 95% could trivalent chromium because of its high water solubility and
be obtained, in spite of 0.26% lead and minor amounts of potassium mobility (Hara et al., 2000; Kim et al., 2016; Saha et al., 2011). For
(0.19%) and sodium (0.18%) (Wu et al., 2014). Meanwhile, the zinc safe stabilization and reuse of the chromium-containing residue,
dust had over 90% metallization degree of zinc and can be used as hexavalent chromium inside should undergo a pre-reduction stage
raw material in the zinc refinery dust after removal of chlorides to its trivalent form with appropriate reducing agents (Ferna ndez
(Pickles, 2007). In comparison to CO, the use of H2 gas has addi- Pereira et al., 2007). The reduced residue with low-valence or
tional advantages. For instance, it functions in the minimization of metallic chromium as alloying value after high temperature
halogens (chlorine and fluorine) in the separated gaseous product reduction (>c.a. 1170 C (Zhang et al., 2000a,b)) can be reclaimed to
after reduction, which simultaneously improves the entire process the steelmaking circuit if the material is returned to EAF. In this
(Antrekowitsch and Antrekowitsch, 2003). Its use and the com- regard, more attentions should be paid to the conversation of
bined use of both carbon (Pickles, 2007) and H2 are considered to chromium-bearing phases in the residue for better economic
be promising in the thermal reduction of EAF dust (Antrekowitsch values.
and Antrekowitsch, 2003). Inspection of the current pyrometallurgical processes also
In pyrometallurgical recycling of EAF dust, the fume (e.g., zinc shows insufficient recoveries of nickel and copper in the dust.
oxide fume) generated is usually polluted by chlorine and fluorine These two metals have boiling points higher than the operating
(Tsugita, 2003), while the residue/slag produced often has a high temperatures of most metal recovery processes. As a result, they are
iron content (Barna et al., 2000) and a small amount of non-ferrous concentrated in either the oxide residue or the metallic iron-rich
metals such as zinc and lead which can be recycled either in an phase. Similar to chromium, nickel is an alloying element and can
electric arc furnace or blast furnace (Peng et al., 2001). For be used in steelmaking. However, copper is generally considered to
improved disposal of the fume and residue, removal of chlorine be a detrimental impurity element in steel. Thus, it is necessary to
from raw dust is essential (Tsubouchi et al., 2010). In fact, the ex- recover copper or remove it from the dust. By now, no viable
istence of chlorine can cause free dioxins and furans, such as pol- method has been reported to recover this metal from EAF dust, the
ychloridedibenzodioxines and dibenzofurans (PCDD/F), during the oxide residue or any metallic iron product using these materials as a
thermal treatment of the dust (Ro € sler et al., 2014). It was shown part of the feed. This problem can only be resolved by diluting the
that by curbing the chlorine load alone a significant PCDD/F mini- copper-containing iron with another source of iron units with a
mization formation can be achieved (Mager et al., 2000). The much lower copper content. The separation of copper from iron
chlorine content also influences the vaporization behaviors of Zn product appears to be feasible by cementation combined with
and Pb. Lead chloride forms a hydroxyl-halide (PbOHCl) and lead suitable treatments (Lindblom et al., 2002).
chloride carbonate (Pb2CO3Cl2) agglutinative matrix which is hard
to remove. In this regard, introducing fresh EAF dust directly to 7. Conclusions
washing process before fuming or processing the dust in H2 at-
mosphere was recommended for chlorine removal (Abdel-latif, EAF dust is an important secondary resource that contains a
2002). Another option is roasting the dust with CO2 at 600 C, number of metallic elements. Recycling this dust via appropriate
followed by water washing, to avoid formation of adhesive lead and routes such as pyrometallurgical processes has both remarkable
zinc hydroxide chloride to improve the removal of chloride (Chen economic and environmental benefits. The authors reviewed the
et al., 2011). Further dechlorination can be realized by microwave chemical, physical and thermodynamic characteristics of EAF dust
roasting because of strong microwave absorbance of chlorides in and the main pyrometallurgical processes for recycling of the dust,
the dust compared to zinc oxide. A recent study revealed that when from traditional Waelz kiln process to unconventional processes
the dust from zinc leaching residue by Waelz kiln volatilizing was such as microwave processing. It is revealed that the physico-
roasted under microwave irradiation at 626 C for 25 min and chemical features of EAF dust, including relatively high contents of
stirring at 54 rpm, the dechlorination ratio could reach 90.13% valued metals (e.g., zinc and iron) and hazardous elements, com-
(Wang et al., 2014). For removal of fluorine, two approaches were plex mineralogical composition, small particle size, low apparent
developed, namely fixing fluorine in the by-products as MnF2 or as density and moisture content, spherical morphology, close associ-
FeF2 and eliminating fluorine by alkaline washing prior to the ation of metal-bearing phases and relatively low thermal stability,
treatment of the gases with SO2. Both methods are technically favor the use of pyrometallurgical routes for recycling of EAF dust.
possible and perhaps complementary (Menad et al., 2003). To Most of the reviewed pyrometallurgical processes are based on
carbothermic reduction and their technical advantages are also leaching and magnetic separation for decreasing the chloride level and
upgrading the zinc content of EAF steelmaking baghouse dusts. Int. J. Min.
supported by low reduction temperatures of oxides of the valued
Process 75, 1e20.
metals and efficient separation of the metals because of the dif- Castro, F., Marques, E., 2001. Some studies on the leaching behaviour of electric arc
ferences in their vaporization behaviors. Among the commercial furnace steelmaking dusts with water and with acetic acid. Acta Metall. Slovaca
pyrometallurgical processes, the Waelz kiln process is the main 4, 36e38.
Chairaksa-Fujimoto, R., Inoue, T., Umeda, N., Itoh, S., Nagasaka, T., 2015. New py-
process for recycling of EAF dust but it suffers from several draw- rometallurgical process of EAF dust treatment with CaO addition. Int. J. Min.
backs, including waste of iron units, great energy consumption and Metall. Mater. 22, 788e796.
high tipping/shipping costs. The RHF direct reduction process is Chairaksa-Fujimoto, R., Maruyama, K., Miki, T., Nagasaka, T., 2016. The selective
alkaline leaching of zinc oxide from Electric Arc Furnace dust pre-treated with
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Journal of Cleaner Production 149 (2017) 1079e1100

Contents lists available at ScienceDirect

Journal of Cleaner Production

Pyrometallurgical recycling of electric arc furnace dust

5.5. Coke-packed bed process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1090

Element Phases References

Fig. 2 shows an electron micrograph of dispersed EAF dust

Fig. 1. Particle size distribution of EAF dust (Oustadakis et al., 2010).

#1 2.53 4.90 0.23 Mixing chamber dust Nolasc-Sobrinho et al., 2003

No. Reaction DGQ ¼ A þ BT Reaction Enthalpy Classiﬁcation

A (J mol1) B (J mol1K1) ( C) (kJ mol1)

Process Temperature ( C) Furnace type Inputs Products Scale Capacity References

X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100

Fig. 5. Flow chart of Waelz kiln process (Mager et al., 2003).

Fig. 8. Section view of OXYCUP furnace (Wang et al., 2015).

5.7. ESRF process 5.8. Plasamadust process

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