Bio-inspired engineering of BiSPPy composite for the efficient electrocatalytic reduction of carbon dioxide
Using surface-engineered chemical composites to enhance the binding energy of reaction intermediates and the conductivity is an attractive route to achieve a high partial current density and increased yield of the target products. Herein, conductive polymer polypyrrole (PPy) was used to regulate the...
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Published in | Energy & environmental science Vol. 16; no. 9; pp. 3885 - 3898 |
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Main Authors | , , , , , , , , |
Format | Journal Article |
Published |
13.09.2023
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Online Access | Get full text |
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Abstract | Using surface-engineered chemical composites to enhance the binding energy of reaction intermediates and the conductivity is an attractive route to achieve a high partial current density and increased yield of the target products. Herein, conductive polymer polypyrrole (PPy) was used to regulate the electronic structure of Bi
2
S
3
and facilitate the activation of CO
2
molecules to enhance the CO
2
electroreduction activity. The constructed electrocatalyst with a unique 3D hierarchical urchin-like nanoflower morphology was composed of Bi
2
S
3
nanowire assemblies with rich S vacancies
via
PPy modification, featuring an improved electron-transfer ability and outstanding formate faradaic efficiency of 91.18% and partial current density of 56.95 mA cm
2
, as well as good stability at a moderate potential in an H-type cell. More importantly, it could deliver current densities exceeding 300 mA cm
2
without compromising the selectivity of formate in a flow-cell reactor. A possible reaction mechanism for formate formation related to HCO
3
was proposed based on the
in situ
ATR-IR spectra, which could bring a new scientific understanding of CO
2
reduction. DFT calculations further demonstrated that the optimized electronic structure, boosted adsorption and activation of CO
2
, and protonation process contributed to a reduced formation energy for the formate intermediate *OCHO, leading to the enhanced performance. More impressively, ZnCO
2
batteries equipped with Bi
2
S
3
PPy displayed a maximum power density of 2.4 mW cm
2
and a superior cycle stability of >110 h. This study underlines the effectiveness of designing composite electrocatalysts to improve the CO
2
RR performance and thus provides a viable path toward carbon neutrality.
Using surface-engineered chemical composites to enhance the binding energy of reaction intermediates and the conductivity is an attractive route to achieve a high partial current density and increased yield of the target products. |
---|---|
AbstractList | Using surface-engineered chemical composites to enhance the binding energy of reaction intermediates and the conductivity is an attractive route to achieve a high partial current density and increased yield of the target products. Herein, conductive polymer polypyrrole (PPy) was used to regulate the electronic structure of Bi
2
S
3
and facilitate the activation of CO
2
molecules to enhance the CO
2
electroreduction activity. The constructed electrocatalyst with a unique 3D hierarchical urchin-like nanoflower morphology was composed of Bi
2
S
3
nanowire assemblies with rich S vacancies
via
PPy modification, featuring an improved electron-transfer ability and outstanding formate faradaic efficiency of 91.18% and partial current density of 56.95 mA cm
2
, as well as good stability at a moderate potential in an H-type cell. More importantly, it could deliver current densities exceeding 300 mA cm
2
without compromising the selectivity of formate in a flow-cell reactor. A possible reaction mechanism for formate formation related to HCO
3
was proposed based on the
in situ
ATR-IR spectra, which could bring a new scientific understanding of CO
2
reduction. DFT calculations further demonstrated that the optimized electronic structure, boosted adsorption and activation of CO
2
, and protonation process contributed to a reduced formation energy for the formate intermediate *OCHO, leading to the enhanced performance. More impressively, ZnCO
2
batteries equipped with Bi
2
S
3
PPy displayed a maximum power density of 2.4 mW cm
2
and a superior cycle stability of >110 h. This study underlines the effectiveness of designing composite electrocatalysts to improve the CO
2
RR performance and thus provides a viable path toward carbon neutrality.
Using surface-engineered chemical composites to enhance the binding energy of reaction intermediates and the conductivity is an attractive route to achieve a high partial current density and increased yield of the target products. |
Author | Wu, Yiji Li, Chengjin Zhou, Xiaoxia Liu, Zhengzheng Fu, Zhengqian Lv, XiMeng Zhang, Lifang Zheng, Gengfeng Chen, Hangrong |
AuthorAffiliation | Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Faculty of Chemistry and Materials Science Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences Fudan University Laboratory of Advanced Materials School of Chemistry and Materials Science Shanghai institute of Ceramics State Key Laboratory of High Performance Ceramics and Superfine Microstructure Chinese Academy of Science |
AuthorAffiliation_xml | – name: School of Chemistry and Materials Science – name: State Key Laboratory of High Performance Ceramics and Superfine Microstructure – name: Fudan University – name: Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Faculty of Chemistry and Materials Science – name: Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences – name: Shanghai institute of Ceramics – name: Laboratory of Advanced Materials – name: Chinese Academy of Science |
Author_xml | – sequence: 1 givenname: Chengjin surname: Li fullname: Li, Chengjin – sequence: 2 givenname: Zhengzheng surname: Liu fullname: Liu, Zhengzheng – sequence: 3 givenname: Xiaoxia surname: Zhou fullname: Zhou, Xiaoxia – sequence: 4 givenname: Lifang surname: Zhang fullname: Zhang, Lifang – sequence: 5 givenname: Zhengqian surname: Fu fullname: Fu, Zhengqian – sequence: 6 givenname: Yiji surname: Wu fullname: Wu, Yiji – sequence: 7 givenname: XiMeng surname: Lv fullname: Lv, XiMeng – sequence: 8 givenname: Gengfeng surname: Zheng fullname: Zheng, Gengfeng – sequence: 9 givenname: Hangrong surname: Chen fullname: Chen, Hangrong |
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