Journal of Cleaner Production 149 (2017) 1079e1100

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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: zwpeng@csu.edu.cn (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 (Ranitovi
c 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
1082 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100

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; Ranitovi
c 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
the real density remains relatively constant. In general, EAF dust
has a very low moisture content (<1 wt%).
3.5. Microstructural morphology
(Nolasc-Sobrinho et al., 2003). Additionally, a number of metal-
oxygen structural forms may appear, as demonstrated by the
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,
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
surfaces of the dust particles and some aggregations between the
particles are clearly observed (Badger and Kneller, 1997). The
spherical morphology confirms that the dust formation is a result of
slag (Mantovani et al., 2002) and metal ejection by CO bubble
bursting on the surface of the bath (Gue
zennec et al., 2004). Den-
dritic structures may exist within the spherical particles,
comprising an iron-chromium spinel and a slag matrix composed
of silicon, calcium, iron, aluminum, magnesium and oxygen
3.6. Thermal property
The thermal stability of EAF dust can be revealed by thermog-
ravimetric analysis (TGA). Fig. 4 shows the TGA profile of a EAF dust
sample (26.66 wt% Zn) at a ramp rate of 10  C min1 under N2 at-
mosphere (Al-Harahsheh et al., 2014). According to the diagram,
there existed three steps for the mass loss. The first mass loss event
started at 136  C with the maximum mass loss rate occurring at
175  C, corresponding to evaporation of entrained free water and

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

 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100 1083

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-
rides). The second mass loss had an onset temperature of 380  C
with the maximum mass loss occurring in the range 630e700  C,
essentially attributed to the vaporization of metal chlorides (e.g.,
ZnCl2). The final mass loss event initiated at a temperature of
750  C, and the loss was assigned to the vaporization of zinc metal
generated due to reduction of zinc oxide by free carbon (2.2 wt%)
present in the dust.
4. Thermodynamics concerning pyrometallurgical processing
of EAF dust
The principle of pyrometallurgical processing of EAF dust is to
extract valuable metals such zinc, iron, lead, etc, from the dust,
essentially dependent on carbothermic reduction (e.g., Waelz kiln
process), calcification (e.g., calcification process) or halogenation
(e.g., chlorination process). The Gibbs free energy expressions of
main reactions involved in pyrometallurgical processing of EAF dust
were determined by the FactSage™ software [version 7.0, Thermo-
fact/CRCT (Montreal) and GTT-Technologies (Aachen), Federal Uni-
versity of S~
ao Carlos] and the results are summarized in Table 4.
As shown in Table 4, zinc oxide, ferrous oxide, lead oxide,
chromium trioxide and cadmium oxide can be reduced into
metallic forms at relatively low temperatures (<1000  C, see reac-
tion temperature in Table 4 at which the corresponding reaction
takes place) in spite of their endothermic nature. This fact partially
supports recycling EAF dust via pyrometallurgical processes. After
reduction, zinc, lead and cadmium will evaporate because of their
high vapor pressures at the EAF operating temperature. The metal
vapors can then be condensed, separated and recovered using a
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
reclamation. This residue can be used directly, or after simple
treatment, as a qualified secondary raw material for steel
production.
It should be emphasized that most of the existing pyrometal-
lurgical processes are based on carbothermic reactions. The metal
oxides in EAF dust are reduced by either carbon or carbon mon-
oxide. Compared with solid carbon, carbon monoxide has better
reducing ability, demonstrated by its low reduction temperatures
in Table 4. As a matter of fact, many of the metal extraction pro-
cesses involve use of both reducing agents (Zhang et al., 2000a,b).
This statement is particularly true when the dust has a high carbon
content or carbonaceous materials are added as reducing agent. In
such case, the reduction initially depends on the degree of contact

Fig. 2. Electron micrograph of EAF dust showing fine dust particles (Simonyan et al., 2015).
1084 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
Fig. 3. Scanning electron micrograph and elemental distribution image of EAF dust (Sofili
c et al., 2004).
between carbon and the dust particles where the solid/solid reac-
tion occurs, and there are very low vapor partial pressures of CO
and metals (e.g., zinc, lead and cadmium). With gradual con-
sumption of carbon in reduction of the metal oxides, however, the
contact area between carbon and metal compounds decreases. On
the contrary, the CO partial pressure increases steadily with
involvement of Boudouard reaction. Consequently, the solid/solid
reduction reaction becomes more difficult and the reduction re-
actions between CO and the metal oxides in the dust dominate the
extraction process. Hence, for recycling of EAF dust via carbother-
mic reduction, accelerating gasification of carbon and mass transfer
of CO is crucial and is worthy of extensive exploration.
Fig. 4. TGA profile of EAF dust (Al-Harahsheh et al., 2014).
5. Pyrometallurgical processes for recycling of EAF dust
For treatment of EAF dust, many pyrometallurgical processes
have been developed or are under development. In the present
study, the Waelz kiln process, rotary hearth furnace (RHF) process,
PRIMUS process, OXYCUP process, coke-packed bed process, Aus-
melt process, electric smelting reduction furnace (ESRF) process,
Plasamadust process, plasma-arc process, Elkem multi-purpose
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 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
the gas from 1000  C to about 450  C. Condensed zinc and lead
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100 1085

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,
while iron and slag components are collected in the filter. Ma (2011)
proposed a radical new approach, the In-Process Separation (IPS)
technology, in which zinc is removed from the EAF off-gas before it
reacts with iron-containing particles to form the franklinite phase
in the combustion chamber. The dust collected in the baghouse
filters can be sent directly to the crude zinc oxide treatment plant as
it will no longer contain Fe. However, this technique requires
implementation in each individual EAF plant. It may be impossible
to collect the starting product from a larger area to treat a large
amount of dust simultaneously (Suetens et al., 2014a,b).
5.1. Waelz kiln process
Among all high-temperature metal recovery processes, the dust
processed by the Waelz kiln accounts for about 75% of the total
treated EAF dust globally (Mager et al., 2000). Fig. 5 shows a
simplified flow chart of Waelz kiln process (Mager et al., 2003).
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
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 form of metal vapors. By controlling admission of air at the kiln
outlet end, zinc and lead in the gas phase are oxidized again and
formed as Waelz oxide, while the metallic iron in the charge is re-
oxidized and then constitutes a byproduct called Waelz slag
(Coronado et al., 2016). Meanwhile, the process heat liberated can
be effectively utilized in the charge. In the process, chlorine and
alkalis volatilize together with the heavy metals. The dust-laden
off-gas will be treated in a downstream off-gas unit for
purification. The rotary kiln furnace is used to treat Waelz oxide to
refine zinc with elimination of lead, cadmium and chlorides
(Morcali et al., 2012).
The Waelz kiln process is considered to be a relatively mature
process for recycling of EAF dust in spite of several disadvantages.
The major shortcoming of this process is associated with the
remained zinc and lead in the Waelz slag where iron is not suffi-
ciently enriched after separation of zinc in the form of vapor,
indicating waste of iron units. This problem becomes more serious
when the process produces high amounts of slag (about
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-
nomics of the process (Leclerc et al., 2002). High energy
consumption is another drawback of this process due to its strict
requirements on the operation temperature of units (Mishra et al.,
2002). Moreover, it is an off-site process in which high tipping and
shipping fees ($80-$125 ton1) have to be applied (Sun et al., 2008),
adding cost.
5.2. Rotary hearth furnace process
The rotary hearth furnace (RHF) process is an important coal-
based direct reduction method for dust recycling (Lu and Huang,
2003) and has been practiced in the steel industry (Oda et al.,
2006). Fig. 6 shows the primary flow chart of RHF process for
treatment of EAF dust (Tsutsumi et al., 2010). By this process, the
mixture of the dust, reducing agent and additives is first used for
pelletizing (Wu et al., 2013). The green pellets/briquettes prepared
are sent into the moving RHF and heated to 1000  C in its heating
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
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100 1087

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).
1088 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
high temperature chemical reactions take place and the overall
temperature can reach up to 1300  C. During the process, the metal
oxides are reduced to the corresponding metallic forms. Zinc and
lead are separated from the pellets in the form of vapor and sub-
sequently enter into the exhaust pipe. The metal vapors are
oxidized to zinc oxide and lead oxide, respectively, along with the
movement of waste gas, and collected by the dust collector in the
form of soot. During the process, alkaline metal chlorides are
removed simultaneously. The iron oxides are reduced into direct
reduced iron (DRI) under strong reducing atmosphere and the
percent reduction of DRI reaches up to 90% in 15e20 min
(Kuwauchi and Barati, 2013).
The RHF direct reduction process is deemed effective in pro-
cessing EAF dust containing appreciable amounts of iron, carbon,
zinc, lead and alkalis. With the process, high-grade zinc product
and DRI can be produced instead of slag. It was therefore claimed
that this process may be commercially and environmentally su-
perior to the Waelz kiln technology (Nakayama and Taniishi, 2011).
The iron metallization degree, zinc removal ratio and alkali metals
(K and Na) removal ratios may exceed 75%, 95%, and 80%, respec-
tively, for the reduced pellets/briquettes under the condition of the
molar ratio of carbon to oxygen equals 1.0 at 1230  C for 15 min. The
downside of this process, however, is due to the requirement for
the charge. Until recently, the RHF process was only suited for
recycling EAF dust with low zinc content (<5 wt%) (Suetens et al.,
2014a,b) although this technology has been reengineered to over-
come operational problems such as zinc oxide blockages at higher
zinc content, mainly associated with low compressive strength of
the pellets/briquette which may result in substantial amount of
Fig. 7. Flow chart of PRIMUS process for treatment of EAF dust (Frieden et al., 2001).
broken pellets and fines which must be returned to the pelletizing
step, thereby lowering the process productivity. Moreover, due to
the large initial investment in equipment, the economic benefits of
the process have to be enhanced further, especially at the early
stage of its operation.
5.3. PRIMUS process
The PRIMUS technology involves use of multi-hearth furnace for
metallization of non-agglomerated finely dispersed EAF dust
(Frieden et al., 2001), as shown in Fig. 7. The furnace consists of a
cylindrical chamber on a vertical axis, with multiple superimposed
or stacked annular compartments between which the hearth
floors/roofs are constructed of refractory bricks which form self-
supporting levels with openings. In practice, a mixture of pulver-
ized coal and EAF dust is charged at the uppermost hearth and
transported from one hearth to the next and from the center to the
wall and back with the aid of scrapers. The processing temperature
can be elevated from ambient temperature to 1100  C by the
combustion of coal in burners and by the secondary combustion of
CO formed during reduction. At high temperatures, zinc and lead
compounds are reduced to their metallic forms, evaporated, re-
oxidized by the furnace gas, removed from the furnace through
the exhaust port and collected in the gas-cleaning system (bag
filter) with the recovery degree of 95%. Meanwhile, alkaline com-
pounds are vaporized and captured. At the bottom of the furnace
DRI or iron concentrate with degree of metallization 90e95% is
discharged, cooled and used for BF smelting or EAF steelmaking
(Kurunov, 2012). In this way, separation of iron from zinc and lead
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
and other elements such as sodium and potassium as well as
chlorine is realized.
The PRIMUS process is featured by unprepared and low-cost
feed, rapid reduction of metal oxides due to intensive stirring and
heating, high efficiency with relatively low process temperatures
(1000e1100  C) and excellent quality products, including highly
metallized DRI (>90%) and highly concentrated zinc oxide which
enable selective extraction of the zinc (Roth et al., 2001; Suetens
et al., 2014a,b). The downside of this process is associated with
the corrosion of furnace due to both rapid stirring and evaporation
of alkaline compounds during reduction. Meanwhile, to keep good
kinetic conditions for the charged feed, the furnace has a restricted
size which restrains its productivity, as indicated in Table 5.
5.4. OXYCUP process
The OXYCUP process, developed by Kuttner GmbH& Co., melts
self-reducing briquettes by vibropressing EAF dust, sludge and
scale generated in steelmaking with a cement binder in a cupola
Fig. 8. Section view of OXYCUP furnace (Wang et al., 2015).
1089
operated with an oxygen-enriched blast (5e15% of oxygen enrich-
ment) (Fisch and Kesseler, 2006; Holtzer et al., 2015), as shown in
Fig. 8. The briquettes are charged into the furnace with fluxes and
large pieces of scrap (up to 1 m). Coke and carbon fines are used as
fuels. In particular, coke provides most of the energy source for the
furnace and guarantees the permeability of stock column. At low
temperatures (c.a. 500  C), portions of metallic iron are formed on
the external surface of briquettes. This coating grows and protects
briquette against decomposition beyond 1000  C when the direct
reduction by carbon contained in briquettes initiates. In contrast to
blast-furnace smelting, most iron in the OXYCUP process is reduced
by carbon in the briquettes at 900e1400  C in a short period of time
(20e30 min) (Kurunov, 2012). At temperatures above 1450  C bri-
quettes completely convert into spongy iron, which is melted
together with the metallic charge loaded to the furnace. Molten
metal containing 4 wt% carbon is tapped continuously at 1500  C.
Overall, the process produces “zero waste” (Holtzer et al., 2015).
The resulting pig iron of precisely known quality is delivered to the
steel plant. The slag is granulated and the cleaned top gas rich in CO
1090 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
is used as a fuel. The top dust is recycled into briquettes and sold as
zinc concentrate (crude zinc oxide) with sufficiently high zinc
content (e.g., 30 wt%).
The OXYCUP process shows a good combination of the function
of melting in traditional cupolas and that of reduction in BF, thereby
useful for both high- and low-zinc burdens. It is expected to remedy
some major defects of traditional processes such as Waelz kiln
process (Holtzer et al., 2015). In general, this process produces hot
metal with lower cost than that from BF. It is also an environ-
mentally friendly approach for EAF dust treatment as emissions of
sulfur oxides, nitrogen oxides, dioxins and furans are below the
allowable values. Like those in BF smelting (Hryniewicz and
Janewicz, 2008; Magdziarz et al., 2011, 2015), the prepared charge
should have sufficient strength to sustain the reduction process.
However, information concerning the reduction of the briquettes
composed of EAF dust in the process is insufficient. To improve the
furnace operation, more efforts should be spent on illustrating the
reduction process in the furnace in association with the physico-
chemical properties of the charge.
5.5. Coke-packed bed process
The coke-packed process is a smelting reduction process using a
shaft furnace with a coke packed bed for recycling of steelmaking
dust (e.g., EAF dust) developed by Kawasaki Steel Corp (Itaya et al.,
1990). The furnace is featured by installation of two stage tuyeres,
namely upper and lower tuyeres (Fig. 9). Fine raw materials (EAF
dust, flux and coke) without agglomeration are injected through
the upper tuyeres and then melted instantly in the raceway inside
the shaft furnace. Because of efficient heat exchange between the
ascending gas and the descending coke in the furnace, a high
temperature and intensively reducible region is formed between
the upper and lower tuyeres. The melted oxides in the dust are
easily reduced to metals as they drip through the high-temperature
coke-paced bed. When the molten metals (e.g., iron, chromium and
nickel) and slag drop to the hearth, high-vapor-pressure elements
including zinc and lead are vaporized and extracted through the
furnace top. As shown in Table 5, the process has three products:
Fig. 9. Flow chart of coke-packed bed process for treatment of EAF dust (Hara et al., 2000).
crude zinc oxide, molten metal, and slag. By treating a typical EAF
dust containing 27.7 wt% zinc, 25.0 wt% iron and 3.22 wt% lead, it
was found that zinc and lead were concentrated in the crude zinc
oxide (60 wt% zinc and 6.2 wt% lead) and their contents in the metal
(0.005 wt% zinc and 0.001 wt% lead) and the slag (0.01 wt% zinc and
0.001 wt% lead) were very low (Hara et al., 2000).
The coke-packed process has advantages of efficient separation
of various metals such as zinc, lead and iron. However, the smelting
reduction consumes a huge amount of heat. In practice, it is
necessary to elevate the temperature to over 1550  C at the level of
the lower tuyeres, which supply the majority of heat, to completely
reduce metal oxides. Also, it is crucial to prevent the zinc adhesion
on the wall of the furnace top. Further efforts should be made to
maintain top gas temperature and CO2/CO in the region where zinc
vapor is stable (Hara et al., 2000).
5.6. Ausmelt process
EAF dust can be treated using the Ausmelt technology (Hughes
et al., 2008). In this technology, the granulated mixture consisting
of EAF dust, reducing agent and additives is sent into the Ausmelt
furnace from a lid plug without drying (Hughes et al., 2008). The
powdered coal and fuel gas are injected into welding pool by a
spray gun to maintain the temperature of furnace at about 1300  C.
The melting temperature of EAF dust usually ranges from 1250 to
1400  C. After zinc oxide and lead oxide are reduced to their
metallic forms at about 1100  C, the metals will volatilize and re-
oxidize to their corresponding oxidized forms due to reactions
with the air above the molten pool (Zhou, 2002). These oxides are
collected in a bag filter chamber before further treatment and
recycling (Matusewicz and Mounsey, 1998).
The advantage of the process is ascribed to its good aerodynamic
condition which can promote the reduction of zinc and lead oxides
and volatilization of zinc and lead but hinder the reduction of iron
oxide by controlling the atmosphere and temperature. This feature
allows potential reduction in the energy consumption of the dust
treatment with the removal ratio of zinc amounting to 65%e75%
(Yin, 1998). However, the relatively low purity of zinc soot in the
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
Fig. 10. Flow chart of ESRF process for treatment of EAF dust (Nakayama, 2012).
process and insufficient productivity due to complex bed opera-
tions restrain its development.
5.7. ESRF process
The ESRF process simply uses an electric furnace for material
heating and oxide reduction (Nakayama, 2012). Fig. 10 shows the
primary flow chart of ESRF process for treatment of EAF dust. In this
process, a mixture of agglomerated EAF dust, coke and limestone as
material charge is loaded into the furnace. Carbon monoxide and Zn
vapor in the exhaust gas are oxidized in the combustion chamber (a
simple vertical cylinder) with water-cooled and partially
refractory-lined wall which prohibits the adhesion of softened dust
and facilitates cleaning. Powders of iron oxide and carbon settled at
the bottom of the combustion chamber are recycled to the ESRF.
Hot exhaust gas containing much crude zinc oxide and chlorides is
withdrawn from the combustion chamber and quickly cooled
through the multi-tube gas cooler for recovering the particles in the
bag-house. The temperature of the gas cooler is controlled to so-
lidify the chlorides on the vertical tube surface. By removing the
chlorides a good zinc oxide recovery from crude zinc oxide with
65e82 wt% zinc oxide can be achieved. High-carbon pig iron
(3.44 wt% carbon) is returned to arc furnace steel mills. Slag with
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
heavy metals such as zinc, lead and cadmium, simplifying down-
stream disposals such as landfill or use as aggregate for construc-
tion (Nakayama, 2012).
The ESRF process is characterized by the use of sole electrical
energy for heating, melting and reduction without any fuel and by
the low carry-over of charged dust and high zinc oxide content
(over 70%) in crude zinc oxide. When ESRF is installed in an EAF
plant, energy is saved because molten pig iron can be directly
charged into the EAF, without use of a casting machine to make
ingots. Meanwhile, high gas temperature of over 1250  C
completely decomposes dioxins and other organic substances in
EAF dust. No hazardous materials remain in the slag. The disad-
vantage of this process is the high energy cost. Thermal energy of
the hot exhaust gas is often not actively used, and only a portion of
energy is used for preheating the charged material. It is the main
reason why the process was once abandoned. New ESRF process is
expected to meet the economic requirements when recovered
1091
metal prices increase and environmental regulation becomes more
severe.
5.8. Plasamadust process
The Plasmadust process is carried out in a coke-filled shaft
furnace equipped with D.C. non-transferred plasma devices (e.g.,
three 6 MW plasma generators) (Schoukens et al., 1993). These
devices are mounted on the tuyeres of the shaft through which
EAF dust, pulverized coal, fluxes and superheated plasma gas are
injected. The high temperatures (around 2500  C in the raceway
formed in front of each tuyere) and low oxygen partial pressure in
the furnace enable the reduction of iron and chromium oxides at
1400e1600  C, which is difficult for many traditional fuel-air
based processes, e.g., the Waelz kiln process. Molten iron with
various metallic species and a nonhazardous slag are tapped at the
lower part of the furnace. One of the main shortcomings of this
process is the relatively low zinc content (about 20 wt%) in the
crude zinc oxide produced from the process which needs to be
processed further in a high-temperature furnace, such as Waelz
kiln.
5.9. Plasma-arc process
There are two alternatives of plasma-arc process for treatment
of EAF dust, namely the Tetronics and Enviroplas processes
(Schoukens et al., 1993; Goff and Denton, 2004; Denton et al.,
2005). The former process was developed by Tetronics Research
and Development (TRD) in the UK in the late 1970s (Schoukens
et al., 1993). The feeds, including EAF dust and coke fines, are
charged through ports in the roof of a cylindrical D.C. plasma-arc
furnace. The temperature of the furnace is maintained by supply-
ing electric energy via a graphite electrode in the center. During the
process, the metals produced by reduction of oxides of zinc, lead
and cadmium are vaporized, condensed and captured in a zinc
splash condenser. A non-hazardous slag is formed and tapped
periodically from the furnace while off-gases are withdrawn from
the furnace continuously. The Enviroplas process is another
plasma-arc process developed by Mintek based on the carbother-
mic and metallothermic reduction of metal oxides in the EAF dust
at 1400e1600  C in a DC plasma arc furnace (Assis, 1998). The
Tetronics and Enviroplas processes are differentiated by charging
1092 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
practice. In the Enviroplas process, the feed is transferred to the
furnace via the central hole of the graphite electrode while in the
Tetronics process it is charged through the ports located in the roof
of the furnace. Feeding through the hollow graphite electrode in
the Enviroplas process offers a series of advantages, including direct
delivery of feed into the high temperature reaction zone under the
electrode, rapid absorption of EAF dust into the molten slag, and
reduced contamination and elutriation or carry-over of the feed
due to minimized interaction of the leaving vapor products with
feed materials falling down from feed ports in the roof. The ferro-
alloys produced contain relatively small quantities of sulfur and
phosphorus (about 0.06 wt% and 0.04 wt%, respectively) which
enable further steelmaking. The slag has less than 0.1% of the zinc
input, while the fumes produced contain high grade of zinc oxide
(on average 56.3 wt%). Due to its large energy requirement, this
process has a much smaller capacity, in comparison with the Waelz
kiln process (Table 5).
5.10. EMPF process
The EMPF process for treatment of EAF dust is based on a three-
phase slag-resistance furnace characterized by advanced electrode
seal designs, gas tight bodies and roofs, and fully cooled slag zones
using plate coolers which generate a frozen-slag (freeze) lining
(Kennedy et al., 2009). The furnace has high intensity ranging from
300 to 400 kW m2 of hearth area or approximately
300e1000 kW m3 of slag volume. The 10 MW EMPF built at
Laclede Steel, Alton (IL) has an annual designed capacity of 40 kt of
EAF dust (Schoukens et al., 1993; Kennedy et al., 2009). This process
shares several similarities with the plasma-arc process. For
example, like the Tetronics process, vaporized products withdrawn
from the furnace are captured in a zinc splash condenser. The main
Fig. 11. Flow chart of submerged plasma process for treatment of EAF dust (Popovici, 2009).
differences are the use of a three-phase slag-resistance furnace
instead of a D.C. open-arc furnace and the application of briquettes
instead of un-agglomerated feeds. Compared with the Enviroplas
process which has the inherent advantages of a D.C. plasma-arc
furnace over an A.C. slag-resistance furnace, the EMPF process
has relatively higher electrode consumption, lower-symmetry heat
distribution and more complex operation control.
5.11. Submerged plasma process
The submerged plasma zinc-fuming process uses electric
plasma torches (plasma generators) to supply process heat and
good mixing conditions to the slag bath into which a mixture of
pelletized EAF dust, petroleum coke and flux is fed continuously
(Verscheure et al., 2005; Verscheure et al., 2007a,b), as shown in
Fig. 11. Inside the plasma torches, the cold blast air is transformed
into a high enthalpy plasma gas which is mixed with natural/pe-
troleum gas and injected into the slag bath. The solid feed dissolves
into the molten bath and blast gases react with the slag and
reductant. Zinc and other volatile metals fume off. Above the bath,
the fume is post-combusted with secondary air, and the resulting
off-gases and solid zinc oxide particles are removed from the
smelting vessel. After the post-combustion the off-gas is further
oxidized with air in a radiation chamber and treated in an elec-
trostatic precipitator to recover zinc oxide. Part of the heat gener-
ated in the post-combustion is transferred back to the slag bath to
increase energy efficiency of the process. The outputs of the process
are an iron, calcium and silica-rich slag phase, a matte phase, crude
zinc oxide powder (55e65 wt% zinc) and off-gas (Verscheure et al.,
2007a,b).
In the submerged plasma process, the carbon and heat re-
quirements of the process are separated. The molar ratio of carbon
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
to oxygen (C/O) and electrical power can be independently
adjusted to optimize the performance of the furnace. The use of
submerged plasmas also enables high slag bath temperatures
(around 1300e1400  C) which promote high zinc-fuming rates. A
key feature of the process is the use of high temperature freeze
linings (a layer of bath material that protects the furnace wall,
formed on the reactor wall backed by the water-cooled steel
furnace shell) to contain this slag bath, designed through the
control of bath chemistry with use of dolomite flux. Using such
freeze linings promotes maximum operation temperatures of
conventional slag fumers which are restrained by highly super-
heated aggressive fayalite slags, in spite of increased enthalpy
losses to the water cooling system due to the high superheat of the
slags. The design of these freeze linings is crucial for the technical
and economic feasibility of the process. The use of supplementary
heat supplied by the plasma torches helps to maintain high bath
temperatures and the application of high liquidus temperature
slags provides stable freeze linings to keep integrity of the bath
wall. These features and the reactor design lead to higher zinc-
fuming rates than those achievable using conventional zinc-
fuming processes. The use of hydroelectric power in the plasma
offers the opportunity of lowering the environmental impact of
the process through reduced greenhouse gas emissions. Addi-
tional work is required to simultaneously optimize slag compo-
sition and process performance while ensuring vessel integrity via
model development (Verscheure et al., 2007a,b). The challenge is
to engineer or select a slag chemistry which will provide a stable
protective furnace lining and also minimize heat losses through
the furnace shell.
5.12. PIZO process
The PIZO process uses a continuous channel induction furnace
as the primary unit for processing of EAF dust (Bratina and Lenti,
2008). The furnace contains a molten iron bath which serves as a
heat sink to rapidly heat the charged material, a briquetted mix of
EAF dust and reductants. Under high temperature conditions
(1300e1500  C), reduction of oxides of zinc, lead and cadmium
proceeds quickly, followed by that of iron and other metals. Zinc,
lead and cadmium are vaporized and re-oxidized. The metal oxide
dust is collected as crude zinc oxide in a baghouse system. Iron and
some other metals which enter into the molten bath are removed
by rotating the furnace forward and pouring the bath through a
teapot spout into a receiving ladle. The iron product may be sale-
able after pouring into a pig machine or used directly as hot metal.
Remaining materials, including silica, calcium, magnesium and
aluminum, produce a molten slag which can be removed from the
furnace by rotating the furnace backward and used as a slag
modifier or road aggregate.
The channel induction furnace fits in with the needs of contin-
uous feed of raw materials to produce zinc, iron and slag products
which are removed continuously or semi-continuously. The in-
ductors on the furnace serve as an efficient device for providing
energy for the process. All three distinct products of the process, pig
iron, crude zinc oxide and slag, are saleable. Approximately 95% of
the input iron is recovered as pig iron with a much higher market
value than the typical iron/slag mix generated from a Waelz kiln
(The PIZO® Advantage, 2016). Meanwhile, there is very low loss of
iron product to the crude zinc oxide (<1.5 wt% iron in the oxide) and
to the slag (Bratina and Lenti, 2008). Hence, the process reduces the
loss of iron and provides a better feed material for downstream zinc
processing operations. For further improvement of the PIZO pro-
cess, up-scaling its capacity with minimized energy consumption
and environmental impact is ongoing.
1093
5.13. Flame reactor process
The flame reactor process involves use of a flame reactor (a
water-cooled vertical cylinder, diameter 0.6 m  height 3 m) having
an upper combustion zone and a lower smelting zone for EAF dust
treatment (Orhan, 2005). In the combustion zone, CO is produced
by the partial combustion of natural gas with oxygen-enriched air
in a cyclone burner at the top of the reactor. The hot reducing flame
(>2000  C) travels down to the smelting zone, where the dust is
injected pneumatically with feed rates of 1e2 t h1 of EAF dust. Due
to the rapid reactions at high temperatures (about 1600  C), the
average retention time of the dust in the flame reactor is only half a
second. Like many of the approaches for management of EAF dust,
the oxides of zinc, lead and cadmium in the flame reactor process
are reduced to their metallic forms. The metals undergo vapor-
ization and re-oxidization. Lastly, a crude zinc oxide is collected in a
bag filter for subsequent metal extraction in electrothermic zinc
plants. The molten slag generated is tapped continuously from the
reactor for sale or disposal (Assis, 1998). Overall, this process has a
simple operation, despite a relatively low efficiency which is mainly
restricted by the combustion of fuel in the flame reactor.
5.14. Thermal plasma reduction process
A representative plasma technology is the Scan Dust AB (Li,
2012). In this technology, flue gas is decomposed into the gas
atoms or particles by the electric current on the electrode (copper)
produced by the high temperature (approximately 3000  C)
(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
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 high temperature in the reaction zone. In this process, zinc oxide
and lead oxide are reduced to the vapors of zinc and lead which are
condensed as liquid metals outside the furnace condenser. The
mixture of metal vapors is gradually separated in the condenser
because of the different boiling points of the metals. Meanwhile, iron
is enriched in slag and discharged from the bottom of furnace.
A study by Best and Pickles examined the feasibility of recov-
ering metals of values from EAF dust containing 24.8 wt% zinc using
a 24 kVA AC plasma arc furnace under CO atmosphere between
1000 and 1400  C with reaction ratio of 1e8 g L1 (dust feeding rate
to CO flow rate) and dust feeding rate of 50e150 g min1 (Best and
Pickles, 2001). The volatile elements (zinc, lead, cadmium, potas-
sium and sodium) were collected in a condenser, whereas the
remaining elements (iron and chromium) constituted a slag phase.
The zinc recoveries reached up to 97%, and the removal of lead
closely approximated that of zinc, accomplished by either reduction
of lead oxide which leads to evaporation of lead or volatilization of
lead-bearing species, namely lead sulfide, lead chloride and lead
oxide. The cadmium in the dust was found to be almost totally
recovered in the condensate during cooling of the off-gas phase.
Simultaneously, exceeding 90% of the alkalis (potassium and so-
dium) were removed primarily due to the volatilization of the salts.
In addition, a greater potassium removal was achieved associated
with the higher vapor pressure of potassium chloride compared to
sodium chloride (Magdziarz et al., 2015). Most of chromium (>93%),
on the other hand, was remained in the iron-rich phase because of
high stability of chromium oxides and low equilibrium partial
pressure of chromium-bearing compounds. In principle, the iron-
rich slag could be reclaimed to the steelmaking circuit.
The plasma technology provides more effective recovery of zinc
and iron, in comparison with other approaches such as the Waelz
kiln process. It can be used in large or small operations because of
1094 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
its compact equipment, short payback period of investment, high
efficiency, environmental friendliness, operation flexibility and
special advantage of recovering the valuable metals such as chro-
mium (Huaiwei and Xin, 2011). Currently, the main problem of this
technique is ascribed to the determination of the optimum pa-
rameters of the reactionary zone and velocity of process for
maximum extraction of zinc and lead. This issue is particularly
important for scaling up the plasma process because it is operated
at high temperatures, implying great energy consumption. Further,
there exists a relatively strict requirement for the property of feed.
In general, highly-dispersed powdered EAF dust is preferred
because it fits the needs of the technology.
5.15. Microwave processing
Microwave processing of materials, featured by volumetric
heating, selective heating and non-thermal effects (Peng, 2012), is
an advanced alternative to conventional methods because micro-
wave energy is absorbed at the molecular level and heat can be
generated inside materials (Peng and Hwang, 2015). Processing EAF
dust under microwave irradiation has fast reaction rate, large zinc
removal ratio and high iron metallization degree, thereby receiving
increasing attention. Sun et al. investigated the zinc removal and
metallization of iron as a function of microwave time and carbon
addition at microwave power of 1100 W (Sun et al., 2008). Because
the mixture of EAF dust and carbon powders (20 wt%) was heated
well in the microwave field, the removal of zinc was near
completion in only 12 min, with the highest zinc removal ratio and
iron metallization degree approaching 99.2% and 100%, respec-
tively. Zhou et al. (2015) also assessed the performance of using
microwave energy for recycling of EAF dust. It was found that for
the sample with 16 wt% graphite irradiated by 10 kW microwaves
for 10 min, the removal ratio of zinc varied between 80% and 90%
and the metallization ratio of iron ranged from 40% to 60%. This
result was partially attributed to microwave heating which over-
came the barrier of traditional heating model characterized by in-
ward heat transfer. It was also closely correlated to the magnetic
ferrites contained in the dust which served as strong microwave
absorbers and to the lower processing temperatures associated
with smaller reaction activation energy (Zhou et al., 2015).
Obviously, microwave processing offers an efficient choice for
treatment of EAF dust. It is actually a result of the good microwave
absorbance of the materials used in processing (carbonaceous
materials) and of the components in the dust (e.g., ferrites) (Peng,
2012). Hence, an in-depth exploration of microwave absorbing
properties of iron-bearing and zinc-bearing phases (magnetite,
franklinite, etc.) as well as reducing agents like coal/coke (Peng
et al., 2016, 2017), which depend on their compositions and
structures (Sebastian et al., 2015), will allow further enhancement
of metal recovery and treatment efficiency with great environ-
mental friendliness via microwave processing.
5.16. Solar thermal reduction process
Solar thermal reduction is a clean technology which can be used
to recycle EAF dust and other waste materials in a sustainable
manner. According to Schaffner et al. (2003), it employed a high-
flux solar furnace equipped with a solar chemical receiver-reactor
in which the carbothermic reduction of EAF dust was performed
using concentrated solar energy. For solar thermal reduction, a
solar concentrating facility was an essential prerequisite. Such fa-
cility could offer up to 50 kWth of thermal radiative power at peak
radiative flux of 11 000 kW m2 by incorporating an array of 10
high-pressure Xe arcs coupled with ellipsoidal specular reflectors
(Tzouganatos et al., 2013). The reduction relied on the solar reactor
consisting of an upper cavity and a lower cavity, separated by a
170 mm-diameter 5 mm-thick SiC-coated graphite plate
(Tzouganatos et al., 2013). The upper cavity received concentrated
solar irradiation which passed through a 65 mm-diameter circular
aperture with a 2 mm-thick quartz window. The lower cavity was
an octagonal enclosure (diameter 135 mm  height 170 mm) which
served as the reaction chamber containing a packed bed of solid
reactants. With this arrangement, the concentrated solar radiation
was efficiently adsorbed by the top of the packed bed.
The technical feasibility of solar thermal reduction has been
demonstrated in the temperature range 847e1127  C with both
batch and continuous modes of operation (Schaffner et al., 2003),
which extracted up to 99% and 90% of the zinc in the EAF dust,
respectively. The condensed off-gas products were found to be
mainly constituted by zinc, lead and chlorine. By maintaining the
O2 concentration in the furnace below 2 vol%, the zinc oxide
presence could be minimized.
The solar thermal energy was also used for purification of Waelz
oxide containing 55e65 wt% zinc in oxidic form from the EAF dust
processed in the Waelz kiln process and for extraction of zinc by
carbothermic reduction (Tzouganatos et al., 2013). It was shown that
by clinkering the oxide at above 1265  C using a 10 kWth packed-bed
solar reactor, the content of impurities (e.g., chlorides and fluorides)
in the oxide could be reduced below 0.1 wt%. The clinkered oxide was
reduced under solar irradiation using biochar as CO2-neutral
reducing agent between 1170  C and 1320  C, which yielded 90 wt%
zinc in the condensed product. Incorporation of continuous or semi-
continuous feeding of reactants and removal of products could
further improve product yield and thermal efficiency.
The most prominent advantage of solar thermal reduction
process is the minimization of emissions of greenhouse gases and
other pollutants. For further development of the process, particular
attention should be paid to optimizing solar reactor with maximum
thermal efficiency and chemical reaction. In fact, the thermal effi-
ciency of solar system is relatively low (usually <10%) although it
increases with reactor temperatures and feeding rates (Schaffner
et al., 2003). To obtain high thermal efficiency and chemical con-
version, it is of importance to match the energy absorption rate
with the feeding rate of reactants and the kinetics of the reaction.
5.17. Iron bath smelting process
The iron bath smelting process was designed to produce hot
zinc, lead and iron economically from EAF dust at low capacity with
direct use of coal (particularly non-coking coal). By this process, the
valuable metals can be recovered through forming the alloy with
the melting iron which can be easily separated from the innocuous
slag. Chen and Gammal (2000) investigated zinc recovery from EAF
dust by bath smelting reduction in a furnace using inert gas as
protective gas. For zinc and lead volatilization, a certain amount of
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
ratios was charged. After the desired time the slag and metal
generated were removed, while secondary dust was collected at the
roof of furnace. The main reactions between metal oxide in slag and
carbon in melt are shown in Table 4. It was found that the smelting
reduction of (FeO) with carbon in the melt was 10e100 times faster
than that with solid carbon or CO gas, revealing precisely the
advantage of the process. Both the volatilization degrees of (Zn) and
(Pb) exceeded 99% at 1400  C. After metal-slag separation, iron was
enriched in the metallic part in which the zinc and lead contents
decreased from 22 wt% and 1.12 wt%, respectively, to both less than
0.005 wt%.
Apart from carbon, silicon can also be used for ferrous oxide
reduction and zinc recovery. Grillo et al. (2014) reported that it was
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
possible to recover 98% of the Fe in EAF dust and the secondary dust
collected after the test had a high level of zinc (68 wt%) at 1500  C.
Of interest is the ferrous oxide was reduced by carbon in a lesser
and slower extent than it was reduced in the presence of silicon.
The slag was featured by low ferrous oxide and zinc oxide contents,
implying great potential for complete recovery of these oxides.
It is evident that the bath smelting reduction process has a good
separation of the main metals in the EAF dust treatment. However,
due to the strict requirement for the reduction temperature
(1400e1500  C) which must be maintained to enable melting of the
reaction system (Pickles, 2010) the high energy cost of the process
constitutes a major obstacle to its further development.
5.18. Calcification process
The calcification process aims at recovering zinc oxide from EAF
dust by addition of calcium carbonate (Itoh et al., 2008) or lime
(Chairaksa-Fujimoto et al., 2015). According to Itoh et al. (2008), the
dust and calcium carbonate were initially mixed at an appropriate
ratio and then pressed into the 10 mm diameter 1.5 g tablet under
the pressure of about 400 MPa before heating in air for a desired
holding time at temperature of 900  C or 1100  C. In the reaction
zone, the franklinite, the main zinc-bearing component in EAF dust
reacted with the calcium oxide, producing zinc oxide and calcium
ferrite (Ca2Fe2O5). Because of the remarkable difference between
the magnetic susceptibility of zinc oxide and that of calcium ferrite,
they could be separated under a high gradient magnetic field. It was
reported that 95% of the zinc oxide in the dust was recovered in
spite of approximately 6 wt% calcium ferrite contamination.
Another benefit of this process is the preferential volatilization of
lead, chloride and fluorine in the EAF dust (Chairaksa-Fujimoto
et al., 2015). Most of lead and chloride were removed preferen-
tially at temperatures below 900  C, whereas complete removal of
fluorine occurred above 1000  C in the presence of calcium oxide. In
the process without addition of calcium oxide, on the other hand,
the evaporation of halogens and lead in the dust began at tem-
peratures higher than 560  C and drastically increased at about
900  C (Chairaksa-Fujimoto et al., 2016). Most of the chloride,
fluorine and lead were removed from the remaining dust at 1100  C
(Chairaksa-Fujimoto et al., 2015).
Fig. 12. Schematic of reaction between ZnFe2O4 and CaCl2 (Guo et al., 2010).
1095
The calcification process shows a high recovery ratio of zinc
because the majority of zinc oxide and calcium ferrite in the dust
can be efficiently separated. The by-product of the process, calcium
ferrite, may be used in dephosphorization during the process of
steel making. However, in this process, the large addition of calcium
carbonate or calcium oxide, e.g., Ca/Fe > 1.0 (Chairaksa-Fujimoto
et al., 2015), often leads to low zinc oxide yield in magnetic sepa-
ration and increased contaminants in the Zn-bearing fraction.
5.19. Halogenation process
The halogenation process is based on the reaction between
highly reactive halides (or their derivatives) and non-ferrous metals
in the EAF dust, followed by evaporation of the formed metallic
halides from the solid residue. It can be divided into two main
groups: the chlorination process and the bromination process.
Recently, the chlorination process has attracted increasing atten-
tion. According to Guo et al. (2010), EAF dust was first mixed with
calcium chloride (CaCl2) powders as chlorinating agent to prepare a
charge with Zn/Ca molar ratio of unity before it was transferred into
the hot zone of an electric furnace within flowing purified N2 gas
between 875 and 1050  C. Under this circumstance, zinc, iron and
lead were respectively chlorinated to ferrous chloride, lead chloride
and zinc chloride by calcium chloride. Due to the high vapor
pressures of zinc chloride and lead chloride, they were easy to
volatile and remove at low temperatures. Iron, on the other hand,
remained in the dust residual phase in the form of oxide. The re-
covery ratio of zinc could reach 80% in the temperature range from
875  C to 1050  C. Fig. 12 shows a schematic of the reaction be-
tween zinc ferrite powders and calcium chloride (Guo et al., 2010).
It is observed that the zinc ferrite particles are wrapped by the
molten calcium ferrite and the chlorination reaction occurs at the
solid-liquid interface. The zinc chloride dissolves in the liquid
membrane of calcium chloride and volatilizes at the interface
before the product layer of calcium ferrite is continuously
increasing and enriched in the residue for further removal.
Apart from calcium chloride, hydrogen chloride (HCl) gas
evolved from organic waste (Lee and Song, 2007), such as polyvinyl
chloride (PVC), is used as a chlorinating additive to assess the
feasibility of recycling EAF dust for metal extraction (Zhang et al.,
1096 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
2000a). During the processing of the mixture of EAF dust and PVC,
the metal oxides in the dust are converted to metal chlorides and
recovered in the gaseous form (Zhang et al., 1999). The dust serves
as a viable treating agent for harmless incineration of PVC which, on
the other hand, produces hydrogen chloride through thermal
decomposition in recovering metals from waste stream. After water
leaching, the metals are separated (Sofili
c et al., 2004).
Based on a similar mechanism, the bromination process makes
use of the reaction between reactive bromide with zinc- and lead-
bearing phases in the EAF dust. By this route, Grabda et al. inves-
tigated recycling of EAF dust in the presence of bromine-containing
plastic waste, namely tetrabromobisphenol A (TBBBPA) and tetra-
bromobisphenol A diglycidyl ether (TBBPADGE), which released
reactive HBr gas during thermal decomposition (Grabda et al.,
2014). When the mixture of the dust and TBBBPA/TBBPADGE was
compressed into pellets and heated at 550  C for 80 min under
oxidizing or inert conditions, high separation of zinc and lead from
the dust was achieved. Particularly, in the case of TBBPADGE, a
maximum of 85% of zinc and 81% of lead could be recovered.
The halogenation process is highly selective in separating metal
elements, mainly Zn and Pb, in the dust and meanwhile enriches Fe
in the residual phase. With this process, the reaction temperature
may be reduced considerably regarding the low boiling points of
the metal chlorides or bromides. In addition, the reduction furnace
is unnecessary in the process. The biggest concern about this
technology, however, is the addition of halides which, as expected,
often causes corrosion of apparatus and poses a potential envi-
ronmental threat in the subsequent operations.
6. Discussion
As a typical by-product of electric arc furnace steelmaking, EAF
dust contains a variety of valuable elements (iron, zinc, lead, etc.).
Its chemical/phase composition and fine granularity are compatible
with pyrometallurgical recycling. As aforementioned, most of py-
rometallurgical processes are based on the carbothermic reduction
of metal oxides in the dust, primarily aiming at recovering zinc, lead
and iron. Zinc oxide as a main zinc-bearing phase is easy to reduce,
while the other major phase, zinc ferrite, must decompose to zinc
oxide first under reducing atmosphere before reduction thereafter.
Because a significant amount of gaseous zinc can be formed at
temperatures above 1000  C, the effective removal of zinc from EAF
dust is feasible at a temperature of 1000e1100  C. Unlike zinc oxide,
the lead oxide starts to reduce to its metallic state at 650  C and
begins to evaporate and convert into a gas phase at 900  C. As
expected, these reduction reactions can be accelerated with
increasing temperature. After separation of zinc and lead, iron in
the dust is enriched in the residue for further treatment.
Based on the above principles, the Waelz kiln process, RHF
process, PRIMUS process, OXYCUP process, coke-packed bed pro-
cess, Ausmelt process, ESRF process, Plasamadust process, plasma-
arc process, EMPF process, submerged plasma process, PIZO pro-
cess and flame reactor process (Table 5) have been successfully
used in industry. Meanwhile, some unconventional methods with
higher processing efficiency and metal recovery, such as microwave
processing and solar thermal reduction process, are being devel-
oped for further optimization of treatment of EAF dust in a more
sustainable way, representing future directions of technological
innovation and development in pyrometallurgical recycling of the
waste.
Despite apparent progress in this field, there still exist several
technical challenges/problems. One of the most important de-
ficiencies of the current research which, to some extent, restricts
the development of technologies for EAF dust treatment is the
insufficient exploration of the properties and complex association
of occurrence of iron-, zinc-bearing and other minor phases in the
dust. For instance, it was shown that zinc oxide can restrain the
reduction of iron oxide, but the competing effect of reduction of
zinc oxide and iron oxides are not well illustrated based on the both
thermodynamic and kinetics analyses (Machado et al., 2006). The
activities of these oxides (e.g., zinc oxide and ferrous oxide) may
also be decreased apparently due to the existence of spinel phases
Fe3-xCrxO4 and ZnFe2O4, which shows the close association of these
metals. Secondly, non-ferrous metals, such as Zn, are easy to
vaporize and separate from a Fe-rich phase, but they are usually re-
oxidized in many processes and, therefore, the gaseous product of
the dust processing is often a crude oxide which requires further
treatment and thus additional input of energy. Thirdly, because
certain non-ferrous metals and hazardous elements remain in the
process fume/residue, their disposal may constitute a big puzzle
and sometimes pose harsh requirements on operation apparatus.
As mentioned above, the majority of the pyrometallurgical pro-
cesses focus only on recovery of zinc, lead and iron from EAF dust in
which other hazardous elements such as chlorine and chromium
were not explored adequately (Bruckard et al., 2005).
To tackle the first problem for desirable extraction of these
metals, more efforts should be directed to the formation and
decomposition of the spinel phases and separation of the metals
based on the exploration of properties of the ferrites (Zhang et al.,
2000a,b). It was reported that inside the off-gas ducts of EAF the
spinel phases such as franklinite forms through a gas-solid reaction
starting from pure Fe droplets and Zn vapor (Nedar, 1996). The
amount of the spinel phases at room temperature generally de-
creases with increasing zinc and manganese contents in the dust.
Conversely, it increases with increasing iron content. Hence, from
the point of view of efficient metal extraction, the first choice for
pyrometallurgical processing is to eliminate the formation of spinel
phases, which can be achieved by reducing the oxygen potentials,
operating EAF under airtight conditions (Nedar, 1996), increasing
dust loading, or using additives such as calcium oxide and its de-
rivatives (e.g., CaF2) (de Araújo and Schalch, 2014). It should be
pointed out that although the presence of CaO (in the form of lime
or calcium carbonate) can thermodynamically reduce the amount
of spinel at 1100  C through the formation of various calcium fer-
rites (e.g., CaO.Fe2O3 and 2CaO.Fe2O3) which results in the libera-
tion of zinc oxide and iron oxide, thereby increasing the non-
ferrous metal recoveries (Pickles, 2008a,b), the appropriate use of
the additive deserves special attention in view of its sensitive dose
dependence of relevant phase transformations. Currently, such
dependence can be partially revealed by several advanced micro-
scopy technique (Denning et al., 2016; Payton et al., 2016). In fact,
after all of the ferrite spinel disappears, the amount of zinc oxide
remains relatively constant but that of iron oxide decreases as the
amount of calcium ferrite continues to increase. In EAF dust,
however, the amount of calcium ferrite is relatively low despite a
relative large amount of calcium oxide. This is a result of the slow
kinetics of reactions involving solid calcium oxide (Zhang et al.,
1999), which warrants extra consideration. From the perspective
of decomposition of the spinel phases and separation of the metals,
the preliminary thermodynamic analysis of carbothermic reduction
of spinel phase implied that relatively high temperatures and low
(oxygen) pressure favor high zinc and lead recoveries, while low
temperature and relatively high total pressure/high reactant ratio
are of benefit to high metallic iron recovery (Wu et al., 2014).
Therefore, reducing the total pressure and introducing non-reactive
gas may contribute to increased non-ferrous metal recoveries and
decreased metallic iron recovery. Further separation of zinc, lead
and other non-ferrous metals can be realized by controlling pro-
cessing temperature and reactant ratios considering the difference
in their thermodynamic stability (Pickles, 2007).
 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
To prevent metal re-oxidation during cooling, it is important to
ensure the reducing atmosphere in the whole process using a
suitable reducing agent which simultaneously reduces its CO2
footprint. One option is substituting fossil raw materials (e.g., coal
and coke) with carbon-neutral ones based on biomass, such as
biochar (Griessacher and Antrekowitsch, 2012). This reductant has
a high gasification efficiency and faster reduction speed which help
to maintain the atmosphere in the reduction process. It is also
characterized by very low impurity (e.g., sulfur and phosphorus)
contents and carbon neutrality, producing much less pollution to
the environment. Obviously, the economics of the new processes
involving biomass-based materials depend on many factors, such
as biomass availability and price, costs for biomass conversion,
effectiveness of the carbon-neutral reducing agent, development of
carbon taxes and additional costs arising from environmental
legislation in future. Other than solid reducing agents, gaseous re-
ductants including CO and H2 may be employed to prevent the re-
oxidation of the metals. It was proposed that by using CO gas as a
reducing agent for recycling of EAF dust, an iron-rich residue with
an iron grade of 89.9 wt% and metallization degree over 95% could
be obtained, in spite of 0.26% lead and minor amounts of potassium
(0.19%) and sodium (0.18%) (Wu et al., 2014). Meanwhile, the zinc
dust had over 90% metallization degree of zinc and can be used as
raw material in the zinc refinery dust after removal of chlorides
(Pickles, 2007). In comparison to CO, the use of H2 gas has addi-
tional advantages. For instance, it functions in the minimization of
halogens (chlorine and fluorine) in the separated gaseous product
after reduction, which simultaneously improves the entire process
(Antrekowitsch and Antrekowitsch, 2003). Its use and the com-
bined use of both carbon (Pickles, 2007) and H2 are considered to
be promising in the thermal reduction of EAF dust (Antrekowitsch
and Antrekowitsch, 2003).
In pyrometallurgical recycling of EAF dust, the fume (e.g., zinc
oxide fume) generated is usually polluted by chlorine and fluorine
(Tsugita, 2003), while the residue/slag produced often has a high
iron content (Barna et al., 2000) and a small amount of non-ferrous
metals such as zinc and lead which can be recycled either in an
electric arc furnace or blast furnace (Peng et al., 2001). For
improved disposal of the fume and residue, removal of chlorine
from raw dust is essential (Tsubouchi et al., 2010). In fact, the ex-
istence of chlorine can cause free dioxins and furans, such as pol-
ychloridedibenzodioxines and dibenzofurans (PCDD/F), during the
thermal treatment of the dust (Ro € sler et al., 2014). It was shown
that by curbing the chlorine load alone a significant PCDD/F mini-
mization formation can be achieved (Mager et al., 2000). The
chlorine content also influences the vaporization behaviors of Zn
and Pb. Lead chloride forms a hydroxyl-halide (PbOHCl) and lead
chloride carbonate (Pb2CO3Cl2) agglutinative matrix which is hard
to remove. In this regard, introducing fresh EAF dust directly to
washing process before fuming or processing the dust in H2 at-
mosphere was recommended for chlorine removal (Abdel-latif,
2002). Another option is roasting the dust with CO2 at 600  C,
followed by water washing, to avoid formation of adhesive lead and
zinc hydroxide chloride to improve the removal of chloride (Chen
et al., 2011). Further dechlorination can be realized by microwave
roasting because of strong microwave absorbance of chlorides in
the dust compared to zinc oxide. A recent study revealed that when
the dust from zinc leaching residue by Waelz kiln volatilizing was
roasted under microwave irradiation at 626  C for 25 min and
stirring at 54 rpm, the dechlorination ratio could reach 90.13%
(Wang et al., 2014). For removal of fluorine, two approaches were
developed, namely fixing fluorine in the by-products as MnF2 or as
FeF2 and eliminating fluorine by alkaline washing prior to the
treatment of the gases with SO2. Both methods are technically
possible and perhaps complementary (Menad et al., 2003). To
1097
remove chlorine and fluorine compounds simultaneously, sepa-
rating these halides in an oxidizing step at about 1150  C for
150 min (also known as clinkering) prior to reduction of remaining
residue seems reasonable in spite of loss of a small amount of
valuable metals (Hung et al., 2012). It was reported that a very high
amount of chlorine (>90%) was removed and similar results were
obtained for fluorine. Further optimization of halides removal relies
on an in-depth exploration of the basic knowledge on the behaviors
of relevant elements. In particular, it is necessary to establish a
competent thermodynamic database from which the behaviors of
halogens and heavy metals (e.g., saturated vapor pressures of heavy
metals and their partition in the fume/residue system) as well as
their interactions in a specific process can be inferred and
identified.
From the above discussion, chromium usually retains in the
residue due to high stability of the chromium oxides and low
equilibrium partial pressure of the chromium-containing com-
pounds over the temperature range from 1000 to 1400  C. Hex-
avalent chromium in the EAF dust has 100-fold more toxicity than
trivalent chromium because of its high water solubility and
mobility (Hara et al., 2000; Kim et al., 2016; Saha et al., 2011). For
safe stabilization and reuse of the chromium-containing residue,
hexavalent chromium inside should undergo a pre-reduction stage
to its trivalent form with appropriate reducing agents (Ferna
ndez
Pereira et al., 2007). The reduced residue with low-valence or
metallic chromium as alloying value after high temperature
reduction (>c.a. 1170  C (Zhang et al., 2000a,b)) can be reclaimed to
the steelmaking circuit if the material is returned to EAF. In this
regard, more attentions should be paid to the conversation of
chromium-bearing phases in the residue for better economic
values.
Inspection of the current pyrometallurgical processes also
shows insufficient recoveries of nickel and copper in the dust.
These two metals have boiling points higher than the operating
temperatures of most metal recovery processes. As a result, they are
concentrated in either the oxide residue or the metallic iron-rich
phase. Similar to chromium, nickel is an alloying element and can
be used in steelmaking. However, copper is generally considered to
be a detrimental impurity element in steel. Thus, it is necessary to
recover copper or remove it from the dust. By now, no viable
method has been reported to recover this metal from EAF dust, the
oxide residue or any metallic iron product using these materials as a
part of the feed. This problem can only be resolved by diluting the
copper-containing iron with another source of iron units with a
much lower copper content. The separation of copper from iron
product appears to be feasible by cementation combined with
suitable treatments (Lindblom et al., 2002).
7. Conclusions
EAF dust is an important secondary resource that contains a
number of metallic elements. Recycling this dust via appropriate
routes such as pyrometallurgical processes has both remarkable
economic and environmental benefits. The authors reviewed the
chemical, physical and thermodynamic characteristics of EAF dust
and the main pyrometallurgical processes for recycling of the dust,
from traditional Waelz kiln process to unconventional processes
such as microwave processing. It is revealed that the physico-
chemical features of EAF dust, including relatively high contents of
valued metals (e.g., zinc and iron) and hazardous elements, com-
plex mineralogical composition, small particle size, low apparent
density and moisture content, spherical morphology, close associ-
ation of metal-bearing phases and relatively low thermal stability,
favor the use of pyrometallurgical routes for recycling of EAF dust.
Most of the reviewed pyrometallurgical processes are based on
1098 X. Lin et al. / Journal of Cleaner Production 149 (2017) 1079e1100
carbothermic reduction and their technical advantages are also
supported by low reduction temperatures of oxides of the valued
metals and efficient separation of the metals because of the dif-
ferences in their vaporization behaviors. Among the commercial
pyrometallurgical processes, the Waelz kiln process is the main
process for recycling of EAF dust but it suffers from several draw-
backs, including waste of iron units, great energy consumption and
high tipping/shipping costs. The RHF direct reduction process is
another relatively mature approach for processing EAF dust with
production of high-grade zinc oxide and DRI. However, it currently
only fits the needs of recycling of low-zinc dust. Several uncon-
ventional methods featured by higher processing efficiency and
metal recovery, e.g., microwave processing and solar thermal
reduction process, are being developed for treatment of EAF dust in
a more sustainable way. Although many of them have not
commercialized yet mainly due to relatively large initial capital
investment in equipment, they represent future directions of
technological innovation and development in pyrometallurgical
recycling of EAF dust. Technically, for further optimization of
treatment of EAF dust, pyrometallurgical recycling of EAF dust has
to confront the challenges due to complex occurrence and associ-
ation of various metal-bearing phases in the dust, re-oxidation of
the non-ferrous metals after reduction, and enrichment of haz-
ardous impurities in the generated fume and residue. To resolve
these issues, the detailed exploration of the metal-bearing phases
in the dust based on thermodynamic and kinetics analysis, use of
highly-reactive non-polluting reducing agent like biochar, and
treatment of the fume and residue via additional handling such as
pre-reduction or clicking, etc., are necessary. The review is expected
to serve as a useful guide for promoting treatment of EAF dust by
pyrometallurgical processing.
Acknowledgements
This work was partially supported by the National Natural Sci-
ence Foundation of China under Grant 51504297, the Innovation-
Driven Program of Central South University under Grant
2016CXS021, the Fundamental Research Funds for the Central
Universities of Central South University under Grant 2016zzts464,
the Shenghua Lieying Program of Central South University under
Grant 502035001, the Natural Science Foundation of Hunan Prov-
ince, China, and the Open-End Fund for the Valuable and Precision
Instruments of Central South University.
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