Journal of the Energy Institute 116 (2024) 101694

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Journal of the Energy Institute

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Industrial solid waste as oxygen carrier in chemical looping gasification

technology: A review
Lizhuo Peng a, 1 , Senlin Dong a, c, 1 , Jie Yang a, * , Junyuan Gou b , Lan Shao a , Liping Ma a ,
Rui Nie a , Junjie Shi a , Yalei Du d , Yongqing Liu a , Changye Han a
a
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, Yunnan, 650093, China
b
College of Resources and Environment, Chengdu University of Information Technology, Chengdu, Sichuan, 610225, China
c
University Strasbourg, Institute of Chemistry and Processes for Energy, Environment and Health (ICPEES) UMR 7515, CNRS, 25 Rue Becquerel, F-67087, Strasbourg,
France
d
Ecological and Environmental Monitoring Station of Kunming Municipal Ecology and Environment Bureau Songming Branch, Kunming, Yunnan, 651700, China

A R T I C L E I N F O A B S T R A C T

Handling Editor: Dr. Paul Williams Chemical looping gasification is an innovative gasification method in which oxygen carrier plays a crucial role. In
line with the principles of the “green circular economy,” researchers have proposed using industrial solid waste
Keywords: as the oxygen carrier in chemical looping technology. To address the gaps in previously published works, this
Industrial solid waste review aims to summarize the current state of research on the use of industrial solid wastes as oxygen carriers,
Oxygen carrier
focusing on the feasibility, process control and reaction mechanism. Based on the current state of research, four
CLG
recommendations are made for further research on industrial solid waste as an oxygen carrier. Firstly, when bulk
Research suggestions
industrial solid waste is used as an oxygen carrier, it can be considered not to regenerate. Next, it is necessary to
consider the subsequent resource utilization methods of the slag from chemical looping gasification to avoid
turning solid waste into “solid waste” again. Then, multiple solid wastes can be used as oxygen carriers to
improve reaction performance and avoid the disadvantages of individual active ingredients. Finally, when solid
waste is used as an oxygen carrier, it is necessary to pay attention to the migration and transformation of sec­
ondary components.

1. Introduction include CO, H2 and CH4 [48–51]. Syngas can be used for a wide range of
applications in the chemical, energy and metallurgical industries
With the development of industry and the proliferation of car [52–54]. In the CLG process, the OC is reduced and subsequently re­
ownership, CO2 emissions are increasing rapidly. Among the many generated by oxidation with air or vapor [55–57]. CLG is a very prom­
technologies available to reduce the amount of CO2, carbon capture and ising and environmentally friendly coal gasification technology with
storage (CCS) is an effective way to achieve a “dual carbon strategy” high energy efficiency. The basic principles of the CLG process are
[1–5]. It includes pre-combustion capture, post-combustion capture, illustrated in Fig. 1 [58–61]. In the CLG process, the mechanism of the
and oxygen-enriched combustion technologies [6–11]. Chemical loop­ solid fuel in the fuel reactor is as follows (using lignite as an example)
ing combustion (CLC) is a pre-combustion capture method [8,12–16]. In from R1.1.1 to R1.1.4 [62].
the last few years, CLC has made significant progress in utilizing solid
lignite → C + CO + H2 + CO2 + CH4 + H2 S + N2 + other substances
fuels [17–20], especially coal [21–25] or biomass [26–32]. On the basis
of CLC, researchers have developed a new gasification technology called (R1.1.1)
chemical looping gasification (CLG) [33–38], which aims to convert
C + H2 O → CO + H2 (R1.2.1)
solid fuels into syngas [39–44]. The technology requires fuel, an oxygen
carrier (OC) and water vapor [45–47]. The fuel is partially oxidized 3H2 + CO → CH4 + H2 O (R1.3.1)
during CLG and syngas can be obtained. Main components of syngas

* Corresponding author.
E-mail address: [email protected] (J. Yang).
1
These authors contribute equally to this work.

https://doi.org/10.1016/j.joei.2024.101694
Received 11 April 2024; Received in revised form 27 May 2024; Accepted 29 May 2024
Available online 31 May 2024
1743-9671/© 2024 Energy Institute. Published by Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

CLG as well as comprehensive analyses of the advantages and disad­

vantages of multiple industrial solid wastes as OCs. Therefore, this paper
summarizes the fuels and industrial solid wastes used as OCs in the CLG
process. Four industrial solids including RM, PG, converter steel slag (LD
slag) and carbide slag are considered for analysis. As these four wastes
have different major constituents, they can provide pointers for other
industrial solids with the same major constituents. This work focuses on
the feasibility, process control and reaction mechanisms of CLG. Based
on the current status of research on industrial solid waste as OCs, rele­
vant recommendations are made. This work can provide a guidance for
the subsequent development of CLG production syngas using industrial
solid waste as OCs.

2. Chemical looping gasification of different fuels

The fuels for CLG are mainly coal and biomass. Biomass constitutes
all organic matter from plants [71–74], animals [75,76], and microor­
ganisms [77–79], and also includes by-products and metabolites pro­
duced by such organisms in the biosphere [80,81]. Total global biomass
consists of nearly 550 gigatons of carbon. About 80 % of it is
plant-based, 15 % is bacterial, and the remaining 10 % is animal-based
[82]. This shows that biomass reserves are huge and come from a wide
range of sources. Biomass generates a large number of intermediate
products during CLG process such as tars, nitrogen-based compounds,
sulfur-based compounds and halogen compounds [83]. Researchers
found that at temperatures below 700 ◦ C, it is possible to capture carbon
Fig. 1. Principle of CLG [58–61].
in tars, which is good for the environment. However, this method is also
accompanied by problems such as difficulty in recycling and residual ash
CO2 + H2 O + 2CH4 → 3CO + 5H2 (R1.4.1) that is difficult to separate [84].
China is actively promoting energy supply reform. However, for the
With the development of industry, the production of industrial solid energy structure at this stage, coal will still be dominant for a long time.
waste has gradually increased, but it is not fully utilized. The accumu­ Coal energy is an important material cornerstone for human survival
lation of large quantities of solid waste not only depletes land resources, and development, and it is an indispensable resource. As of 2018, global
but also pollutes the soil, water and atmosphere, and endangers human coal reserves were 1.055 trillion [85]. Currently, the global energy
health. The annual output of industrial solid waste is more than 10 structure is still dominated by fossil fuels and coal still remains the
million tons in China. According to the “14th Five-Year Plan for the world’s main energy source [86]. China’s fossil energy is dominated by
Comprehensive Utilization of Bulk Solid Waste of China”, there is a need coal, and the amount of coal mining has gradually increased in recent
to substantially increase the comprehensive utilization rate of smelting years. However, with rapid industrial development in recent centuries,
slag, industrial by-product gypsum and other bulk solid wastes. The high quality coal has been gradually depleted, leaving behind abundant
comprehensive utilization rate of these bulk solid wastes needs to be reserves of low rank coal, which has since been mined in large quantities
greatly improved [63]. Therefore, it is important to find new ways to [87]. Lignite is a kind of poor-quality coal [88–90]. It is mainly
utilize bulk industrial solid wastes. distributed in the eastern part of Inner Mongolia and the eastern part of
The OC is crucial in CLG as it plays the role of transferring lattice Yunnan Province, with a small amount in north-eastern and southern
oxygen. The performance of the OC greatly affects the gasification China. Lignite accounts for about 13 % of China’s total coal [91], and it
process and efficiency. To realize industrial solid waste resourcing, more can also be used as a fuel for CLG [92–94].
researchers are adopting industrial solid wastes as OCs in chemical
looping technology [64–66], such as red mud (RM) [67,68] and phos­ 3. Progress in industrial solid wastes as oxygen carriers
phogypsum (PG) [69,70]. Mendiara et al. [64] confirmed that aluminum
slag has good oxygen-carrying properties and thermal stability. Liu et al. 3.1. Red mud
[65] investigated the synergistic preparation of compound OCs from
nickel and five industrial solid wastes, including magnesium slag, steel 3.1.1. Physical and chemical characteristics of red mud
slag, blast furnace slag, sulfuric iron ore slag and calcium silicate slag. It RM is also referred to as bauxite residue. It is an industrial solid waste
was found that the compound OC with magnesium slag and Ni had the produced during the extraction of alumina from bauxite ore [95–99].
best reactivity performance, characterized by high reactivity, thermal Typically, it is composed of Fe2O3, SiO2, Al2O3 and other elements
stability and high gas production (1.46 Nm3/kg). Zeng et al. [66] [100–104]. The main components of RM can be found in Table 1 [100,
compared the oxygen-carrying capacity of pure iron oxide, natural he­ 105].
matite and hematite as OCs. After analysis, it was found that RM, an
industrial solid waste, has a higher oxygen-carrying capacity. The above 3.1.2. Red mud applied as an oxygen carrier
results confirm that industrial solid waste has better reaction properties The use of Fe2O3 from RM has been widely studied in CLG process
when used as an OC. with biomass as the reaction fuel [106–110]. For example, Zeng et al.
There exist many reviews of chemical looping technology which
focus on the application of a particular OC in chemical looping tech­
Table 1
nology and trends in chemical looping technology. The use of industrial
Components of RM [100,105].
solid wastes as OCs is a promising pathway for resourcing, which can be
Component Fe2O3 Al2O3 SiO2 Na2O CaO TiO2 Others
“turned into treasure and synergized”. However, there is a lack of re­
views on the application of common industrial solid wastes as OCs in Content (%) 20–40 22–23 17–18 5–8 2–22 5–4 0.5–3

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L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

[66] investigated the reaction characteristics of trioxo-pure iron oxide, 112]. Wang et al. [105] investigated the effect of RM as an OC on the
natural hematite, and RM as OCs. Pine sawdust was used as fuel in the modulation of tar and gas product formation characteristics during coal
reaction process and the experiment was carried out in a fixed bed pyrolysis. The results showed that Fe2O3 in RM can react with reducing
reactor. The study concluded that the molar amounts of gases produced agents (e.g., solid carbon, H2, and CO) in a coal pyrolysis environment.
were, in descending order, hematite, pure iron (III) oxide, hematite and With the gradual reduction process of Fe2O3, tar and gas products in RM
natural hematite. From maximum to minimum the order of production are formed gradually. Regardless of whether biomass or coal is used as a
was RM, pure iron (III) oxide, and natural hematite. The results fuel, the RM undergoes a crystallization transition. In detail, it goes from
confirmed the suitability of hematite as an OC for pine sawdust. Li et al. R3.1.1 to R.3.1.12 in the reaction process (Fe2 O3 →Fe3 O4 →FeO→Fe)
and Song et al. [111,112] investigated the excellent performance of RM [66,105,113].
as an OC when using distiller grains and sewage sludge as the biomass
3Fe2 O3 + C → 2Fe3 O4 + CO (R3.1.1)
fuel, respectively. Red mud promoted the gasification of fuels containing
Fe, Na and Ca components. In particular, Fe increased the destruction of
Fe3 O4 + C → 3FeO + CO (R3.1.2)
the surface structure of microwave-pretreated biomass (see Fig. 2) [111,

Fig. 2. (A) Performance and mechanisms of sewage sludge CLG with RM; (B) Schematic diagram of action mechanism of microwave pretreatment on surface
structure damage of distillers grains [111,112].

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L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

FeO + C → Fe + CO (R3.1.3) maintained even after 65 redox cycles, suggesting that the introduction
of CuO did not lead to a decrease in surface sintering. This work revealed
Fe2 O3 + 3C → 2Fe + 3CO (R3.1.4) that the introduction of CuO has a great potential to balance the heat in
reactor, while maintaining the reactivity and stability of OC. Thus, it
3Fe2 O3 + H2 → 2Fe3 O4 + H2 O(g) (R3.1.5) provides a guidance for balancing the heat equilibrium in the reaction
process.
Fe3 O4 + H2 → 3FeO + H2 O(g) (R3.1.6)

FeO + H2 → Fe + H2 O(g) (R3.1.7) 3.2. Phosphogypsum

Fe2 O3 + 3H2 → 2Fe + 3H2 O(g) (R3.1.8) 3.2.1. Physical and chemical characteristics of phosphogypsum
PG is a solid waste produced in the wet phosphoric acid process
3Fe2 O3 + CO → 2Fe3 O4 + CO2 (R3.1.9) [116–118]. Its physical and chemical characteristics can be found in
Fig. 5. PG has four crystalline forms [119]: acicular, monodisperse plate,
Fe3 O4 + CO → 3FeO + CO2 (R3.1.9) polycrystalline nuclei and dense, of which plate crystals are dominant
[70,120] (Fig. 4). XRD detection showed that the main component of PG
FeO + CO → Fe + CO2 (R3.1.10)
is calcium sulfate [70]. The particle diameter of PG is generally
100–300 μm [121,122].
Fe2 O3 + 3CO → 2Fe + CO2 (R3.1.10)
RM contains not only Fe2O3 but also CaO and Na2O, which are good 3.2.2. Phosphogypsum applied as an oxygen carrier
sulfur trapping components. Jiang et al. [114] studied the reaction CaSO4 has emerged as a promising OC in the CLG process [123,124],
mechanism of desulfurization using RM as an OC. They concluded that due to its high oxygen capacity. Moreover, the main reduction product
the material form of Fe2O3 does not change after the redox cycle in the (CaS) has a high reaction enthalpy with molecular oxygen in the aera­
oxidation furnace. In this process, H2S is oxidized to SO2, while CaO and tion atmosphere, which is favorable for the regeneration of CaSO4 [125].
Na2O eventually produce sulfates to fix S and reduce or prevent sulfur According to the compositional properties of PG, it is a suitable OC in
release (Fig. 3). CLG process, providing a new way for PG utilization.
Yang et al. experimentally investigated the process of lignite CLG
3.1.3. Red mud-based compound oxygen carrier with PG. The results are shown in Fig. 6 [126]. It was concluded that the
In order to improve the sintering resistance of RM as an OC, the gasification rate of lignite can be increased by keeping the molar ratio of
incorporation of inert and alkali metal components was investigated PG/lignite at around 0.2 and the reaction temperature higher than 1123
[115]. Yang et al. [115] found that biomass ash contains inert and alkali K [126].
metal components, which can improve the reactivity and consolidation For the CLG process with lignite and PG, the study of the reaction
of RM as an OC. Therefore, the effects of rapeseed straw ash, corn stover mechanism helps in the regulation of achievable products. It was found
ash and bagasse ash and sugar cane bagasse ash on the OC reactivity and that the reaction pathway included R3.2.0 - R3.2.7 [126]. Syngas pro­
cumulative loss rate of RM were investigated and the skeletal structure duction was mainly achieved through (C + H2 O(g)→CO + H2 ) and
of OC was analyzed. The results are shown in Fig. 4. It was found that (CaSO4 + 4CH4 →CaS + 4CO + 8H2 ) (gas-solid reaction) and (CaSO4 +
rapeseed straw ash enriched with K and Ca components increased the 4C→CaS + 4CO) (solid-solid reaction). However, the consumption of H2
reactivity of OCs [115]. Although bagasse ash enriched with Si and CO mainly occurred through (CaSO4 + 4C→CaS + 4CO) and
decreased the reactivity of OCs, it improved their wear resistance [115]. (CaSO4 + 4CO→CaS + 4CO2 ), respectively. In addition, the production
Corn stover ash enriched with K and Si components was an effective of syngas (CO, H2) at high temperatures was favored when using PG as
skeletal reinforcement that improved both reactivity and wear resis­ an OC.
tance [115]. It was also found that the fiber structure strengthened the
lignite → C + H2 + CO + CH4 + H2 S + N2 + H2 O(g) + other substances
skeleton of the OC by forming a bridge structure at the defects of the OC
fiber structure [115]. This improved the attrition resistance of the OC. (R3.2.0)
The gasification process in a fuel reactor is an absorptive process, while
C + H2 O(g) → CO + H2 (R3.2.1)
the decomposition of CuO is exothermic. In order to reduce the thermal
imbalance, CuO was introduced in the OC. The results of thermogravi­ CO + H2 O(g) → CO2 + H2 (R3.2.2)
metric analyses showed that the CuO-loaded RM released more oxygen.
In addition, the reactivity and oxygen transport capacity of OC was CO2 + H2 O(g) + 2CH4 → 3CO + 5H2 (R3.2.3)
improved [115]. The overall reactivity and stability were well
CaSO4 + 4C → CaS + 4CO (R3.2.4)

CaSO4 + 4CO → CaS + 4CO2 (R3.2.5)

CaSO4 + 4H2 → 4H2 O(g) + CaS (R3.2.6)

CaSO4 + 4CH4 → CaS + 4CO + 8H2 (R3.2.7)

To determine the interfacial reactions of PG in the lignite CLG pro­
cess, Yang et al. studied a research on the atomic-scale reactions of PG as
an OC in conjunction with lignite CLG for syngas production, employing
density functional theory [127]. Previous research has revealed that in
this process, lignite gasified into C, CO, H2, etc., at low temperatures.
Then, reaction products of lignite gasification reacted with the effective
component CaSO4 in PG and water vapor. Using C, CO, and H2 mole­
Fig. 3. Conversion path diagram for the reaction of sulfur and Fe/Ca/Na ox­ cules as probes, the adsorption energy, transition state barrier, and re­
ides [114]. action pathways on CaSO4 surface were calculated. The results are

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Fig. 4. Performance and mechanisms of biomass and RM-based compound OC in CLG [115].

Fig. 5. Physical and chemical characteristics of PG: (A) SEM image; (B) XRD pattern; (C) PG gradation; (D) particle size distribution of PG [70,120,122].

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Fig. 6. Evolution rates of (a) CO; (b) H2; (c) CH4; (d) CO2 for different X values (molar ratio of lignite and PG) at 1173 K in N2 atmosphere [126].

illustrated in Fig. 7 [127]. The (010) plane of CaSO4 was chosen for the shown in Fig. 9 [130]. The process was divided into two main steps. The
calculations because this plane is stable, has low energy and has a dense first step was the conversion of CaS to CaSO4, Cu2S to CuO/CuSO4 and
oxygen layer build-up. The results revealed that at a reaction tempera­ Cu to Cu2O. The second step was the further oxidation of Cu2O to CuO.
ture of 1173 K, CO and H2 were more prone to oxidation than C. The
CuO + C → Cu + CO (R3.2.8)
presence of S− 6 atoms in the SO2− 4 atop the CaSO4 surface was more
favorable for the oxidation of C, CO, and H2 compared to Ca2+. The
Cu2 O + C → 2Cu + CO (R3.2.9)
oxidation process primarily occurred around the S− 6 atoms, leading to a
transformation from S− 6 to S− 2. Cu2 O + CO → 2Cu + CO2 (R3.2.10)

3.2.3. Phosphogypsum-based compound oxygen carrier 2Cu2 O + C → 4Cu + CO2 (R3.2.11)

In order to further improve the reaction efficiency, Cu/PG compound
OC was prepared by loading Cu onto PG [128]. The reduction charac­ CaS + O2 →CaSO4 (R3.2.12)
teristics and surface acidity of the composite OC were studied. As seen
from Fig. 8 (A), the first three peaks (noted as a, b, γ) matched the 4Cu + 2O2 →2Cu2 O (R3.2.13)
reductive processes of various oxidation states of copper species, with
the reduction steps of Cu2+→Cu+ and Cu+→Cu0. The peaks at 926 K and 2Cu2 O + O2 →4CuO (R3.2.14)
1075 K in Fig. 8 (A) can be assigned to the reduction of CaSO4 [128]. In
Fig. 8 (B), two desorption peaks at 404 K and 518 K were attributed to 2Cu + O2 →2CuO (R3.2.15)
NH3 desorbed from the acid sites. An obvious peak at 404 K can be
2Cu2 S + 5O2 → 2CuSO4 + 2CuO (R3.2.16)
found, which was associated with CuO desorption peak. Thermody­
namic analysis showed that the PG to Cu molar ratio of about 2 was more
conducive to the production of syngas. 3.3. Steel converter slag
The CLG process of Cu/PG based OC with lignite was further studied
by fluidized bed [129]. It was found that the first 5 min of reaction CO 3.3.1. Physical and chemical characteristics of steel converter slag
production occurs mainly through the reactions of (C + H2 O(g)→ CO + Steel slag (SS) is the main by-product of steelmaking industry
H2 ) and (4CuO→2Cu2 O + O2 ). After 5 min, CO was mostly converted to [131–134] and its production is equivalent to 10%–15 % of crude steel
carbon dioxide via (CaSO4 + 4CO→CaS + 4CO2 ) and (Cu2 O + CO→ [135]. The properties of SS are related to the steelmaking process. In
Cu + CO2 ) reactions, respectively. The regeneration process of Cu/PG general, most SS can be roughly divided into three groups: LD slag or
OC from R3.2.12 to R3.2.16 was investigated and the result are been basic oxygen furnace (BOF) slag, blast furnace (BF) slag and electric arc

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Fig. 7. Reaction paths of C, CO and H2 on the interface of CaSO4(010): (A) Energy profile of C on CaSO4 surface; (B) Energy profile of CO on CaSO4 surface; (C)
Energy profile of H2 on CaSO4 surface [127].

furnace (EAF) slag [131]. The particles of LD slag are fine and often gray 3.3.2. Steel converter slag applied as an oxygen carrier
or light red in color. The main components of LD slag are CaO, SiO2, As LD slag contains Ca, Fe, Al and Mn components, it was used as an
Fe2O3 and Al2O3, and it also contains MgO, MnO, P2O5, TiO2 and other OC in the CLG. Hildor et al. [137] studied the wood pellet CLG process
trace components. The fresh LD slag sample (Fig. 10) possessed a porous using LD slag as an OC. It was found that the wood pellet CLG with LD
surface [136]. slag has the following characteristics: 1) LD slag delivers oxygen to the
fuel; 2) LD slag catalyzes the water-gas shift reaction; 3) LD slag reacts

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Fig. 8. (A) H2-TPR analysis of Cu/PG and (B) NH3-TPD analysis of Cu/PG [128].

Fig. 9. Regeneration mechanism of CuO–CaSO4 compound oxygen carrier [130].

Fig. 10. Microstructure of LD slag [136].

with carbon dioxide to form carbonates; and 4) LD slag can decompose as an OC. Three main material fuels were selected for the reaction
water into hydrogen. The overall results show that the higher H2/CO in process, including steam exploded pellets, pine forest residue and straw.
the syngas of LD slag was mainly due to the in-situ trapping of CO2 from It was found that the phases in the LD slag had catalytic properties and
R3.3.1 by CaO in LD slag, which caused the positive shift of the water gas the temperature reduced the tar yield and the proportion of heavy tar
conversion to promote H2 production (Fig. 11) [137]. fraction in the LD slag. Condori et al. [140] studied the reaction process
1
of biomass CLG to syngas using LD slag as an OC in a 1.5 kWth unit. The
CO + H2 O ↔ CO2 + H2 ΔН0298 = − 41 kJ⋅mol− (R3.3.1) research results revealed that LD slag has high biomass conversion,
Hildor et al. [139] further investigated the characteristics of tar efficient carbon conversion, high syngas yield, and a long lifetime.
produced by a 10 kWth chemical-looping biomass gasifier using LD slag Therefore, it verified that LD slag can be considered as a suitable ma­
terial for biomass CLG, because high quality syngas can be obtained

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Fig. 11. Schematic representation of the equilibrium shift of in situ carbon capture component [138].

from different types of biomass with less emissions of tar and CO2. 3.4. Carbide slag
As the CaO in LD slag can solidify the sulfur component of fuels
during CLG process. Hildor et al. [141] further investigated the reaction 3.4.1. Physical and chemical characteristics of carbide slag
mechanism with SO2 during the CLG reaction process. The specific Carbide slag is the waste residue after hydrolysis of calcium carbide
findings are shown in Fig. 12 [141]. There were three important reaction to obtain acetylene gas [143,144]. The main component of carbide slag
pathways for LD slag to react with SO2 during the CLG process. The first is calcium hydroxide [145,146]. In the acetylene production process, 1t
was formation of CaSO4/CaS. The second was formation of of calcium carbide and water can generate more than 300 kg of acety­
surface-active sulfur, which increased the reaction rate toward. Next, lene gas. During this process, 10 t of industrial waste liquid with a solid
the gas rate of carbon SO2 was increased from OC to char due to oxygen content of about 12 % is generated, which is often referred to as calcium
transfer. carbide slurry. The composition of the carbide slag was determined
using X-ray fluorescence spectroscopy (XRF), and presented in Table 2
3.3.3. Steel converter slag-based compound oxygen carrier [147,148].
LD slag, like other iron-based OCs, has relatively low reactivity to
fuel. In order to improve its reactivity, other active components are 3.4.2. Carbide slag as an oxygen carrier
usually loaded on LD slag. For example, Hildor et al. [142] impregnated In the lignite CLG process, carbide slag can be used simultaneously as
LD slag particles with 2 or 5 wt% of Ni, Cu, Mn, or Ce. The model tar an OC, a hydrogen carrier and an in-situ carbon capture material to
molecule benzene, CO and CH4 were evaluated using a laboratory flu­ produce hydrogen [149,150]. Oxygen (OH− ) in the OC may promote the
idized bed reactor. The results can be found in Fig. 13. Even small gasification of lignite. Moreover, the hydrogen (OH− ) in the hydrogen
amounts of Ni, Cu or Mn could promote the reactivity of CO. The release carrier provides a source of hydrogen for the preparation of hydrogen
of oxygen from Mn and Cu during the reaction promoted the conversion [149,150]. Next, the calcium component of Ca(OH)2 in the carbide slag
of CH4 and benzene. Doping with Ni and Ce also increased the methane can in-situ capture CO2 during the CLG [149,150]. Ca(OH)2 of carbide
content, but it had little effect on the benzene conversion. slag first decomposes into H2O and CaO at high temperature. The pro­
duced water vapor provides both oxygen and hydrogen. At the same

Fig. 12. (A) Ca–S–O–H diagram of stable solid phases at different H2 and SO2 partial pressures at different temperatures with a constant partial pressure of steam of
50 %; (B) Ca–S–O–H diagram of stable solid phases at different H2 and SO2 partial pressure at 850 ◦ C with three different partial pressures of steam; (C) A graphical
summary of reaction paths involving sulfur suggested in the discussion section [141].

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Fig. 13. Performance of LD slag impregnated with Ni, Cu, Mn, or Ce element [142].

appeared in the range of 758 K–918 K, which indicated that carbide slag
Table 2
in-situ captured gases generated by lignite gasification. XRD character­
XRF results of carbide slag (wt.%) [147,148].
ization of the solid products after weight gain revealed that they were
Component CaO Al2O3 MgO Fe2O3 SiO2 mainly CaO and CaCO3.
Values (%) 60–80 0.8–4 0.2–3 0.1–0.7 2–3 The reaction mechanism of hydrogen production from lignite CLG
and carbide slag was elucidated by theoretical analysis, experimental
analysis and comprehensive characterization [150]. The results can be
time, the carbon in lignite can be captured in-situ by CaO. This method found in Fig. 15, which revealed the primary component of carbide slag,
not only saves equipment and operating costs for additional water Ca(OH)2, directly participates in the reaction at temperatures below
vapor, but also reduces the cost of hydrogen production from coal. 773 K. However, at temperatures exceeding 773 K, Ca(OH)2 indirectly
Yang et al. [149] investigated lignite CLG into hydrogen-rich syngas engages in the reaction. Calcium hydroxide in carbide slag decomposes
by carbide slag with C replacing lignite and Ca(OH)2 replacing carbide into CaO and water vapor. Furthermore, CaO can solidify CO2 produced
slag by FactSage thermodynamic software. The results can be found in in the reaction process to achieve indirect carbon fixation using carbide
Fig. 14. Reaction temperature was in the range of 623 K–900 K, and the slag. Water vapor provides hydrogen and oxygen, thus promoting the
molar ratio of C: Ca(OH)2 was higher than 1:4, the highest H2 in the gas generation of hydrogen in the reaction process. Additionally, CaCO3
phase product was about 2 mol. It accounted for 100 vol% excepts generated from carbon capture begins to decompose at reaction tem­
vapor. At the same time, C was entirely captured in-situ to form CaCO3. peratures surpassing 1023 K. In summary, this approach a new
The thermal properties of carbide slag, lignite, and mixtures of carbide perspective for preparing hydrogen-rich syngas in the CLG process.
slag and lignite were investigated under nitrogen gas by a simultaneous The main component of lignite is carbon. Analyzing the distribution
thermal analyzer. Compared with the thermal decomposition of lignite of carbon in the gas-solid phase can provide a theoretical foundation for
alone, the reaction rate of lignite in the mixture of lignite and carbide controlling in-situ carbon capture. Sulfur in lignite is considered an
slag was faster. Moreover, there was a loss of weight in the mixture at the impurity, and its presence may have adverse effects on the hydrogen
reaction temperatures from 705 K to 755 K. Then, a weight gain stage production reaction of lignite CLG with carbide slag. Investigation of the

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L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

Fig. 14. Characterizations of the synergistic OC, hydrogen carrier and in-situ carbon capture effect of carbide slag in CLG of lignite to hydrogen-rich syngas: (A) Gas-
phase product distribution by FactSage calculation; (B) Solid-phase product distribution by FactSage calculation; (C) XRD characterization of carbide slag before and
after CLG; (D) Thermal decomposition analyses of carbide slag, lignite, and mixtures of carbide slag and lignite [149].

migration and transformation of carbon and sulfur can help enhance the 3.4.2.1. Lignite gasification
yield and quality of hydrogen and also contribute to reducing environ­ ( ) ( ) ( ) ( )
Lignite → C C0 + CO C2+ + CH4 C4− + CO2 C4+ (g) + H2 O(g)
mental pollution. It has been reported that the migration and trans­ ( 2− )
+ H2 S S (g) + other substance
formation process of carbon during CLG is highly complex and consists
of three parts, as depicted in Fig. 16 [151]. The first part is the con­ (R3.4.1)
version of organic carbon to inorganic gaseous carbon (including CH4, C,
CO and CO2) through lignite gasification. Subsequently, mutual con­ 3.4.2.2. Reactions associated with the migration and conversion of carbon
( )
version of inorganic gaseous carbon is achieved. Finally, when the re­ C4− + Ca(OH)2 → CaCO3 C4+ (s) + H2 + CaO (R3.4.2)
action temperature exceeds 1073 K, a phase transition process of
inorganic carbon occurs. The process involves the conversion of gaseous C0 + 2Ca(OH)2 → C4+ (s) + H2 + CaO (R3.4.3)
inorganic carbon to solid inorganic carbon and the conversion of inor­
ganic carbon to gaseous carbon. Sulfur migration and transformation 2C0 + 2Ca(OH)2 → C4+ (s) + C4− + CaO (R3.4.4)
primarily involve two steps. The first step is the conversion of organic
sulfur to inorganic gaseous sulfur (H2S) through lignite gasification. C2+ + Ca(OH)2 → C4+ (s) + H2 (R3.4.5)
Subsequently, inorganic gaseous sulfur (H2S) is transformed into inor­
ganic solid sulfur (CaS). In-situ solidification of sulfur can be achieved C4+ (g) + Ca(OH)2 → C4+ (s) + H2 O (R3.4.6)
through the lignite–H2S–CaS reaction pathway.

11
L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

Fig. 15. Reaction pathway for the release of hydrogen and carbon capture [150].

Fig. 16. Migration route of carbon and sulfur in producing hydrogen through lignite CLG using carbide slag [151].

C0 + H2 O(g) → C2+ + H2 (R3.4.7) is very popular due to its high oxygen carrying capacity. Carbide slag has
the characteristics of OC, hydrogen carrier and in-situ carbon capture at
C2+ + H2 O(g) → C4+ (g) + H2 (R3.4.8) the same time due to Ca(OH)2. Industrial solid wastes (RM, LD slag and
carbide slag) react with CaO, which can capture the sulfur content and
CaO + C4+ (g)→C4+ (s) (R3.4.9) also promote the conversion of water gas through in-situ carbon capture.
This in turn promotes the production of H2. Due to poor reactivity,
3.4.2.3. Reactions associated with the migration and conversion of sulfur transition metals are often loaded to improve the reactivity of industrial
( ) solid wastes. The use of industrial solid waste as an OC in CLG process of
S2− (g) + Ca(OH)2 →CaS S2− (s) (R3.4.10) biomass and coal provides a new way for its resourcing.
Based on the current research status, the following suggestions for
4. Conclusions and prospects industrial solid waste are put forward. It does not need to be recycled in
the reaction process as the bulk solid waste using as the OC. Then, it is
Depending on the OC activity, industrial solid wastes such as RM, PG, necessary to consider the subsequent resource utilization ways of the
LD slag and carbide slag have been widely used in the CLG of biomass or slag from CLG to avoid turning solid waste into “solid waste” again.
coal. The advantage of RM and LD slag is that the Fe2O3 content pro­ Next, multiple solid wastes can be used as OC to promote the reaction
motes biomass or coal gasification. The active OC in PG is CaSO4, which

12
L. Peng et al. Journal of the Energy Institute 116 (2024) 101694

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