Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers

doi:10.1016/j.cjche.2020.09.058

Chinese Journal of Chemical Engineering ›› 2021, Vol. 35 ›› Issue (7): 247-255.DOI: 10.1016/j.cjche.2020.09.058

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Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers

Ming Luo^1,2, Lunzheng Zhou¹, Jianjun Cai³, Haiyan Zhang¹, Chao Wang¹

1. School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, China;
2. State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China;
3. School of Environmental Science and Engineering and Key Laboratory of Municipal Solid, Southern University of Science and Technology, Shenzhen 518055, China

Received:2020-07-16 Revised:2020-08-28 Online:2021-09-30 Published:2021-07-28
Contact: Ming Luo
Supported by:
This work was supported by the National Natural Science Foundation of China (51606087), Start-Up Foundation of Jiangsu University (15JDG157). Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2020-KF-07).

Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers

Ming Luo^1,2, Lunzheng Zhou¹, Jianjun Cai³, Haiyan Zhang¹, Chao Wang¹

1. School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, China;
2. State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China;
3. School of Environmental Science and Engineering and Key Laboratory of Municipal Solid, Southern University of Science and Technology, Shenzhen 518055, China

通讯作者: Ming Luo
基金资助:
This work was supported by the National Natural Science Foundation of China (51606087), Start-Up Foundation of Jiangsu University (15JDG157). Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2020-KF-07).

Abstract

Abstract: Chemical looping combustion (CLC) is an energy conversion technology with high efficiency and inherent separation of CO₂. The existence of sulfur in coal may affect the CO₂ purity and the performance of oxygen carrier due to the interactions between sulfur contaminants and oxygen carrier. The migration of sulfur in Beisu coal during the in-situ gasification chemical looping combustion (iG-CLC) process using two oxygen carriers (iron ore and CuO/SiO₂) was investigated respectively. The thermodynamic analysis results showed the formation of metal sulfides was thermodynamically favored at low temperatures and low oxygen excess coefficients, while they were obviously inhibited and the production of SO₂ was significantly promoted with an increase in temperature and oxygen excess coefficient. Moreover, part of sulfur was captured and fixed in the forms of alkali/alkaline earth metal sulfate due to the high amount of alkali/alkaline earth metal oxides in the coal ash or/and oxygen carrier. The experimental results showed that the sulfur in coal mainly released in the form of SO₂, and the sulfur conversion efficiency (X_S) in the reduction stage were 51.04% and 48.24% when using iron ore and CuO/SiO₂ respectively. The existence of metal sulfides was observed in the reduced oxygen carriers. The values of X_S in the reoxidation process reached 3.80% and 7.64% when using iron ore and CuO/SiO₂ respectively. The residue and accumulation of sulfur were also found on the surfaces of two oxygen carriers.

Key words: SO₂, Coal, Ironore, Copper-based, Chemicalloopingcombustion

摘要： Chemical looping combustion (CLC) is an energy conversion technology with high efficiency and inherent separation of CO₂. The existence of sulfur in coal may affect the CO₂ purity and the performance of oxygen carrier due to the interactions between sulfur contaminants and oxygen carrier. The migration of sulfur in Beisu coal during the in-situ gasification chemical looping combustion (iG-CLC) process using two oxygen carriers (iron ore and CuO/SiO₂) was investigated respectively. The thermodynamic analysis results showed the formation of metal sulfides was thermodynamically favored at low temperatures and low oxygen excess coefficients, while they were obviously inhibited and the production of SO₂ was significantly promoted with an increase in temperature and oxygen excess coefficient. Moreover, part of sulfur was captured and fixed in the forms of alkali/alkaline earth metal sulfate due to the high amount of alkali/alkaline earth metal oxides in the coal ash or/and oxygen carrier. The experimental results showed that the sulfur in coal mainly released in the form of SO₂, and the sulfur conversion efficiency (X_S) in the reduction stage were 51.04% and 48.24% when using iron ore and CuO/SiO₂ respectively. The existence of metal sulfides was observed in the reduced oxygen carriers. The values of X_S in the reoxidation process reached 3.80% and 7.64% when using iron ore and CuO/SiO₂ respectively. The residue and accumulation of sulfur were also found on the surfaces of two oxygen carriers.

关键词: SO₂, Coal, Ironore, Copper-based, Chemicalloopingcombustion

Ming Luo, Lunzheng Zhou, Jianjun Cai, Haiyan Zhang, Chao Wang. Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers[J]. Chinese Journal of Chemical Engineering, 2021, 35(7): 247-255.

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Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers

Migration of sulfur in in-situ gasification chemical looping combustion of Beisu coal with iron- and copper-based oxygen carriers

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