Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

doi:10.1016/j.cjche.2022.02.009

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 116-123.DOI: 10.1016/j.cjche.2022.02.009

Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

Xiangzhao Hu¹, Junjie Sun¹, Wanzhen Zheng¹, Sixing Zheng¹, Yu Xie³, Xiang Gao¹, Bin Yang¹, Zhongjian Li¹, Lecheng Lei¹, Yang Hou^1,2,4

1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China;
2. Institute of Zhejiang University-Quzhou, Quzhou 324000, China;
3. Department of Material Chemistry, Nanchang Hangkong University, Nanchang 330063, China;
4. School of Biological and Chemical Engineering, Ningbo Technology University, Ningbo 315100, China

收稿日期:2021-09-11 修回日期:2022-02-13 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Yu Xie,E-mail:xieyu_121@163.com;Yang Hou,E-mail:yhou@zju.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (Nos. 21922811, 21878270, 22178308, and 21961160742), Jiangxi Province "double thousand plan" project (205201000020), the Zhejiang Provincial Natural Science Foundation of China (LR19B060002), the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang (2019R01006), Zhejiang Key Laboratory of Marine Materials and Protective Technologies (2020K10), Key Laboratory of Marine Materials and Related Technologies, CAS, and the Startup Foundation for Hundred-Talent Program of Zhejiang University.

Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

Xiangzhao Hu¹, Junjie Sun¹, Wanzhen Zheng¹, Sixing Zheng¹, Yu Xie³, Xiang Gao¹, Bin Yang¹, Zhongjian Li¹, Lecheng Lei¹, Yang Hou^1,2,4

1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China;
2. Institute of Zhejiang University-Quzhou, Quzhou 324000, China;
3. Department of Material Chemistry, Nanchang Hangkong University, Nanchang 330063, China;
4. School of Biological and Chemical Engineering, Ningbo Technology University, Ningbo 315100, China

Received:2021-09-11 Revised:2022-02-13 Online:2022-03-28 Published:2022-04-28
Contact: Yu Xie,E-mail:xieyu_121@163.com;Yang Hou,E-mail:yhou@zju.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (Nos. 21922811, 21878270, 22178308, and 21961160742), Jiangxi Province "double thousand plan" project (205201000020), the Zhejiang Provincial Natural Science Foundation of China (LR19B060002), the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang (2019R01006), Zhejiang Key Laboratory of Marine Materials and Protective Technologies (2020K10), Key Laboratory of Marine Materials and Related Technologies, CAS, and the Startup Foundation for Hundred-Talent Program of Zhejiang University.

摘要/Abstract

摘要： Electrochemical reduction of carbon dioxide (CO₂ER) into formate plays a crucial role in CO₂ conversion and utilization. However, it still faces the problems of high overpotential and poor catalytic stability. Herein, we report a hybrid CO₂ER electrocatalyst composed of layered bismuth sulfide (Bi₂S₃) and bismuth oxide (Bi₂O₃) supported on carrageenan derived carbon (Bi-CDC) prepared by a combined pyrolysis with hydrothermal treatment. In such 3D hybrid, layered Bi₂O₃ and Bi₂S₃ are uniformly grown on nanocarbon supports. Benefiting from strong synergistic effect between Bi₂O₃/Bi₂S₃ and nanocarbon, Bi-CDC-1:2 displays a high Faradic efficiency (FE) of >80% for formate production in the range of -0.9 V to -1.1 V with the maximum formate FE of 85.6% and current density of 14.1 mA·cm^-2 at -1.0 V. Further, a positive onset potential of -0.5 V, a low Tafel slope of 112.38 mV·dec^-1, and a slight performance loss during long-term CO₂ER tests are observed on Bi-CDC-1:2. Experimental results shows that the better CO₂ER performance of Bi-CDC-1:2 than that of Bi₂O₃ can be attributed to the strong interfacial interactions between nanocarbons and Bi₂O₃/Bi₂S₃. In situ ATR-FTIR measurements reveal that the rate-determining step in the CO₂ER is the formation of HCOO* intermediated. Compared with carbon support, Bi-CDC-1:2 can promote the production of HCOO* intermediate and thus promoting CO₂ER kinetic.

关键词: Nanomaterials, Catalyst, Selectivity, Bi₂S₃/Bi₂O₃, CO₂ electroreduction, Formate

Abstract: Electrochemical reduction of carbon dioxide (CO₂ER) into formate plays a crucial role in CO₂ conversion and utilization. However, it still faces the problems of high overpotential and poor catalytic stability. Herein, we report a hybrid CO₂ER electrocatalyst composed of layered bismuth sulfide (Bi₂S₃) and bismuth oxide (Bi₂O₃) supported on carrageenan derived carbon (Bi-CDC) prepared by a combined pyrolysis with hydrothermal treatment. In such 3D hybrid, layered Bi₂O₃ and Bi₂S₃ are uniformly grown on nanocarbon supports. Benefiting from strong synergistic effect between Bi₂O₃/Bi₂S₃ and nanocarbon, Bi-CDC-1:2 displays a high Faradic efficiency (FE) of >80% for formate production in the range of -0.9 V to -1.1 V with the maximum formate FE of 85.6% and current density of 14.1 mA·cm^-2 at -1.0 V. Further, a positive onset potential of -0.5 V, a low Tafel slope of 112.38 mV·dec^-1, and a slight performance loss during long-term CO₂ER tests are observed on Bi-CDC-1:2. Experimental results shows that the better CO₂ER performance of Bi-CDC-1:2 than that of Bi₂O₃ can be attributed to the strong interfacial interactions between nanocarbons and Bi₂O₃/Bi₂S₃. In situ ATR-FTIR measurements reveal that the rate-determining step in the CO₂ER is the formation of HCOO* intermediated. Compared with carbon support, Bi-CDC-1:2 can promote the production of HCOO* intermediate and thus promoting CO₂ER kinetic.

Key words: Nanomaterials, Catalyst, Selectivity, Bi₂S₃/Bi₂O₃, CO₂ electroreduction, Formate

Xiangzhao Hu, Junjie Sun, Wanzhen Zheng, Sixing Zheng, Yu Xie, Xiang Gao, Bin Yang, Zhongjian Li, Lecheng Lei, Yang Hou. Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate[J]. 中国化学工程学报, 2022, 43(3): 116-123.

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Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

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