Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction

The inefficient charge separation and lack of active sites have been regarded as the main obstacles limiting the CO2 photoreduction efficiency. It is highly desirable but challenging to create a local polarization field to accelerate charge separation and build reactive sites for CO2 reduction dynam...

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Main Authors: Di, Jun, Chen, Chao, Zhu, Chao, Long, Ran, Chen, Hailong, Cao, Xingzhong, Xiong, Jun, Weng, Yuxiang, Song, Li, Li, Shuzhou, Li, Huaming, Xiong, Yujie, Liu, Zheng
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2022
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Online Access:https://hdl.handle.net/10356/160219
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1602192022-07-15T08:17:26Z Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction Di, Jun Chen, Chao Zhu, Chao Long, Ran Chen, Hailong Cao, Xingzhong Xiong, Jun Weng, Yuxiang Song, Li Li, Shuzhou Li, Huaming Xiong, Yujie Liu, Zheng School of Materials Science and Engineering Engineering::Materials Reactive Sites Photocatalysis The inefficient charge separation and lack of active sites have been regarded as the main obstacles limiting the CO2 photoreduction efficiency. It is highly desirable but challenging to create a local polarization field to accelerate charge separation and build reactive sites for CO2 reduction dynamics. Herein, atomic level bismuth-oxygen vacancy pairs are engineered into Bi24O31Br10 (BOB) atomic layers to create a local polarization field. It facilitates photogenerated electrons to migrate from BOB to vacancy pair sites and favors the activation of CO2 molecules. Simultaneously, it works as reactive sites to tune the non-covalent interaction of intermediates and optimizes the reaction process. The vacancy pairs tuned surface atomic structures enable the formation of a highly stable Bi−C−O−Bi intermediate state and consecutive Bi−C−O intermediate, thus changing the rate-determining step from CO* formation to COOH* formation. Benefiting from these features, the VBiO-BOB delivers a 20.9-fold CO2 photoreduction activity enhancement relative to highly crystalline BOB in pure water with highly stability. This work provides new insights for the design of a vacancy pair to create local polarization and tune the non-covalent interaction. Ministry of Education (MOE) This work was supported by Singapore Ministry of Education AcRF Tier 2 (MOE2019-T2-2-105), AcRF Tier 1 RG4/17 and RG161/19. National Key R&D Program of China (2017YFA0207301), NSFC (21725102, U1832156). 2022-07-15T08:17:26Z 2022-07-15T08:17:26Z 2021 Journal Article Di, J., Chen, C., Zhu, C., Long, R., Chen, H., Cao, X., Xiong, J., Weng, Y., Song, L., Li, S., Li, H., Xiong, Y. & Liu, Z. (2021). Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction. Advanced Energy Materials, 11(41), 2102389-. https://dx.doi.org/10.1002/aenm.202102389 1614-6832 https://hdl.handle.net/10356/160219 10.1002/aenm.202102389 2-s2.0-85115872427 41 11 2102389 en MOE2019-T2-2-105 RG4/17 RG161/19 Advanced Energy Materials © 2021 Wiley-VCH GmbH. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Materials
Reactive Sites
Photocatalysis
spellingShingle Engineering::Materials
Reactive Sites
Photocatalysis
Di, Jun
Chen, Chao
Zhu, Chao
Long, Ran
Chen, Hailong
Cao, Xingzhong
Xiong, Jun
Weng, Yuxiang
Song, Li
Li, Shuzhou
Li, Huaming
Xiong, Yujie
Liu, Zheng
Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
description The inefficient charge separation and lack of active sites have been regarded as the main obstacles limiting the CO2 photoreduction efficiency. It is highly desirable but challenging to create a local polarization field to accelerate charge separation and build reactive sites for CO2 reduction dynamics. Herein, atomic level bismuth-oxygen vacancy pairs are engineered into Bi24O31Br10 (BOB) atomic layers to create a local polarization field. It facilitates photogenerated electrons to migrate from BOB to vacancy pair sites and favors the activation of CO2 molecules. Simultaneously, it works as reactive sites to tune the non-covalent interaction of intermediates and optimizes the reaction process. The vacancy pairs tuned surface atomic structures enable the formation of a highly stable Bi−C−O−Bi intermediate state and consecutive Bi−C−O intermediate, thus changing the rate-determining step from CO* formation to COOH* formation. Benefiting from these features, the VBiO-BOB delivers a 20.9-fold CO2 photoreduction activity enhancement relative to highly crystalline BOB in pure water with highly stability. This work provides new insights for the design of a vacancy pair to create local polarization and tune the non-covalent interaction.
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Di, Jun
Chen, Chao
Zhu, Chao
Long, Ran
Chen, Hailong
Cao, Xingzhong
Xiong, Jun
Weng, Yuxiang
Song, Li
Li, Shuzhou
Li, Huaming
Xiong, Yujie
Liu, Zheng
format Article
author Di, Jun
Chen, Chao
Zhu, Chao
Long, Ran
Chen, Hailong
Cao, Xingzhong
Xiong, Jun
Weng, Yuxiang
Song, Li
Li, Shuzhou
Li, Huaming
Xiong, Yujie
Liu, Zheng
author_sort Di, Jun
title Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
title_short Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
title_full Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
title_fullStr Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
title_full_unstemmed Surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for CO₂ photoreduction
title_sort surface local polarization induced by bismuth-oxygen vacancy pairs tuning non-covalent interaction for co₂ photoreduction
publishDate 2022
url https://hdl.handle.net/10356/160219
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