Reaction characteristics investigation of CeO2-enhanced CaSO4 oxygen carrier with lignite

doi:10.1016/j.cjche.2021.02.016

中国化学工程学报 ›› 2022, Vol. 42 ›› Issue (2): 319-328.DOI: 10.1016/j.cjche.2021.02.016

Reaction characteristics investigation of CeO₂-enhanced CaSO₄ oxygen carrier with lignite

Baowen Wang¹, Zhongyuan Cai¹, Heyu Li¹, Yanchen Liang¹, Tao Jiang¹, Ning Ding², Haibo Zhao³

1. Research Institute for Coal Clean and Efficient Utilization, College of Electric Power, North China University of Water Resources and Electric Power, Zhengzhou 450045, China;
2. Hebei Ji-Yan Energy Science and Technology Research Institute, Shijiazhuang 050000,China;
3. State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

收稿日期:2020-08-08 修回日期:2021-02-05 出版日期:2022-02-28 发布日期:2022-03-30
通讯作者: Baowen Wang,E-mail:david-wn@163.com
基金资助:
This work is supported by the National Natural Science Foundation of China (Nos. 51776073, 51906083), Key Research & Development program of Henan Province (No.162102210233), North China University of Water Resources and Electric Power Innovative Project (Nos. 2019XA014, 2019XB058), Scientific Research & Development Project of Ji-Yan Energy Science and Technology Research Institute (NKY2020-05).

Reaction characteristics investigation of CeO₂-enhanced CaSO₄ oxygen carrier with lignite

Baowen Wang¹, Zhongyuan Cai¹, Heyu Li¹, Yanchen Liang¹, Tao Jiang¹, Ning Ding², Haibo Zhao³

1. Research Institute for Coal Clean and Efficient Utilization, College of Electric Power, North China University of Water Resources and Electric Power, Zhengzhou 450045, China;
2. Hebei Ji-Yan Energy Science and Technology Research Institute, Shijiazhuang 050000,China;
3. State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

Received:2020-08-08 Revised:2021-02-05 Online:2022-02-28 Published:2022-03-30
Contact: Baowen Wang,E-mail:david-wn@163.com
Supported by:
This work is supported by the National Natural Science Foundation of China (Nos. 51776073, 51906083), Key Research & Development program of Henan Province (No.162102210233), North China University of Water Resources and Electric Power Innovative Project (Nos. 2019XA014, 2019XB058), Scientific Research & Development Project of Ji-Yan Energy Science and Technology Research Institute (NKY2020-05).

摘要/Abstract

摘要： Calcium sulfate (CaSO₄) has been verified as a promising oxygen carrier (OC) in the chemical looping combustion (CLC) for its high oxygen capacity, abundant reserve and low cost, but its low reactivity and deleterious sulfur species emission from the side reactions of CaSO₄ should be well considered for its wide application in CLC. In order to promote the reactivity of CaSO₄ and increase its potential to inhibit the gaseous sulfur emission, a CeO₂-enhanced CaSO₄ OC mixed OC of core-shell structure was prepared using the combined template synthesis method. Reaction characteristics of the prepared CaSO₄-CeO₂ mixed OC with a typical lignite was first conducted and systematically investigated, and an improved reactivity of the prepared CaSO₄-CeO₂ mixed OC was demonstrated than its single component CaSO₄ or CeO₂ due to the fast transfer and exchange of oxygen from the CaSO₄ substrate to coal via the doped CeO₂. Furthermore, the solid products formed from the mixed CaSO₄-CeO₂ OC with the selected coal were collected and analyzed. Especially, evolution and redistribution of the sulfur species of different forms were focused. At the latter reaction stage of YN reaction with the CaSO₄-CeO₂ mixed OC, the SO₂ emitted from the side reactions of CaSO₄ was greatly diminished and the doped CeO₂ was proven effective to directionally fix the SO₂ released to turn into different solid sulfur compounds, which were determined as Ce₂O₂S, Ce₂S₃ and Ce₂(SO₄)₃·5H₂O and formed through the different pathways. In addition, good regeneration of the reduced CaSO₄-CeO₂ mixed OC could be reached in spite of the unavoidable interaction between the included minerals in coal and the reduced mixed OC. Overall, the combined template method-made CaSO₄-CeO₂ mixed OC reported herein was not only endowed with enhanced reactivity for coal conversion, but also owned the potential to directionally fix the gaseous sulfur emission, which is quite applicable as OC for simultaneous decarbonatization and desulfurization in the real CLC process.

关键词: Coal combustion, CO₂ capture, Chemical looping combustion, CaSO₄ mixed oxygen carrier, Template combined synthesis method, Sulfur evolution

Abstract: Calcium sulfate (CaSO₄) has been verified as a promising oxygen carrier (OC) in the chemical looping combustion (CLC) for its high oxygen capacity, abundant reserve and low cost, but its low reactivity and deleterious sulfur species emission from the side reactions of CaSO₄ should be well considered for its wide application in CLC. In order to promote the reactivity of CaSO₄ and increase its potential to inhibit the gaseous sulfur emission, a CeO₂-enhanced CaSO₄ OC mixed OC of core-shell structure was prepared using the combined template synthesis method. Reaction characteristics of the prepared CaSO₄-CeO₂ mixed OC with a typical lignite was first conducted and systematically investigated, and an improved reactivity of the prepared CaSO₄-CeO₂ mixed OC was demonstrated than its single component CaSO₄ or CeO₂ due to the fast transfer and exchange of oxygen from the CaSO₄ substrate to coal via the doped CeO₂. Furthermore, the solid products formed from the mixed CaSO₄-CeO₂ OC with the selected coal were collected and analyzed. Especially, evolution and redistribution of the sulfur species of different forms were focused. At the latter reaction stage of YN reaction with the CaSO₄-CeO₂ mixed OC, the SO₂ emitted from the side reactions of CaSO₄ was greatly diminished and the doped CeO₂ was proven effective to directionally fix the SO₂ released to turn into different solid sulfur compounds, which were determined as Ce₂O₂S, Ce₂S₃ and Ce₂(SO₄)₃·5H₂O and formed through the different pathways. In addition, good regeneration of the reduced CaSO₄-CeO₂ mixed OC could be reached in spite of the unavoidable interaction between the included minerals in coal and the reduced mixed OC. Overall, the combined template method-made CaSO₄-CeO₂ mixed OC reported herein was not only endowed with enhanced reactivity for coal conversion, but also owned the potential to directionally fix the gaseous sulfur emission, which is quite applicable as OC for simultaneous decarbonatization and desulfurization in the real CLC process.

Key words: Coal combustion, CO₂ capture, Chemical looping combustion, CaSO₄ mixed oxygen carrier, Template combined synthesis method, Sulfur evolution

Baowen Wang, Zhongyuan Cai, Heyu Li, Yanchen Liang, Tao Jiang, Ning Ding, Haibo Zhao. Reaction characteristics investigation of CeO₂-enhanced CaSO₄ oxygen carrier with lignite[J]. 中国化学工程学报, 2022, 42(2): 319-328.

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Reaction characteristics investigation of CeO₂-enhanced CaSO₄ oxygen carrier with lignite

Reaction characteristics investigation of CeO₂-enhanced CaSO₄ oxygen carrier with lignite

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