Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction
The role of vacancy associates in photocatalytic CO2 reduction is an open question. Herein, the Nb─O vacancy associates (VNb─O ) are engineered into niobic acid (NA) atomic layers to tailor the CO2 photoreduction performance. The intrinsic charge compensation from O to Nb around Nb─O vacancy associa...
| Main Authors: | , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/177911 |
| _version_ | 1826118805923823616 |
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| author | Di, Jun Chen, Chao Wu, Yao Chen, Hao Xiong, Jun Long, Ran Li, Shuzhou Song, Li Jiang, Wei Liu, Zheng |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Di, Jun Chen, Chao Wu, Yao Chen, Hao Xiong, Jun Long, Ran Li, Shuzhou Song, Li Jiang, Wei Liu, Zheng |
| author_sort | Di, Jun |
| collection | NTU |
| description | The role of vacancy associates in photocatalytic CO2 reduction is an open question. Herein, the Nb─O vacancy associates (VNb─O ) are engineered into niobic acid (NA) atomic layers to tailor the CO2 photoreduction performance. The intrinsic charge compensation from O to Nb around Nb─O vacancy associates can manipulate the active electronic states, leading to the asymmetric electron redistribution. These local symmetry breaking sites show a charge density gradient, forming a localized polarization field to polarize nonpolar CO2 molecules and tune the noncovalent interaction of reaction intermediates. This unique configuration contributes to the 9.3 times increased activity for photocatalytic CO2 reduction. Meantime, this VNb─O NA also shows excellent photocatalytic activity for NO3 - -NH4 + synthesis, with NH4 + formation rate up to 3442 µmol g-1 h-1 . This work supplies fresh insights into the vacancy associate design for electron redistribution and noncovalent interaction tuning in photocatalysis. |
| first_indexed | 2024-10-01T04:49:30Z |
| format | Journal Article |
| id | ntu-10356/177911 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:49:30Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1779112024-06-03T04:19:21Z Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction Di, Jun Chen, Chao Wu, Yao Chen, Hao Xiong, Jun Long, Ran Li, Shuzhou Song, Li Jiang, Wei Liu, Zheng School of Materials Science and Engineering Engineering Asymmetric electron redistribution Noncovalent interaction The role of vacancy associates in photocatalytic CO2 reduction is an open question. Herein, the Nb─O vacancy associates (VNb─O ) are engineered into niobic acid (NA) atomic layers to tailor the CO2 photoreduction performance. The intrinsic charge compensation from O to Nb around Nb─O vacancy associates can manipulate the active electronic states, leading to the asymmetric electron redistribution. These local symmetry breaking sites show a charge density gradient, forming a localized polarization field to polarize nonpolar CO2 molecules and tune the noncovalent interaction of reaction intermediates. This unique configuration contributes to the 9.3 times increased activity for photocatalytic CO2 reduction. Meantime, this VNb─O NA also shows excellent photocatalytic activity for NO3 - -NH4 + synthesis, with NH4 + formation rate up to 3442 µmol g-1 h-1 . This work supplies fresh insights into the vacancy associate design for electron redistribution and noncovalent interaction tuning in photocatalysis. Ministry of Education (MOE) This work was sup-ported by the National Natural Science Foundation of China (Grant Nos.22378206, 22205108), the Jiangsu Specially Appointed Professorship, the Fundamental Research Funds for the Central Universities (Grant No.30922010302), the Singapore Ministry of Education AcRF Tier 2 (GrantNos. MOE2019-T2-2-105 and MOE-MOET2EP10121-0006), AcRF Tier 1(Grant No. RG7/21). 2024-06-03T04:19:21Z 2024-06-03T04:19:21Z 2024 Journal Article Di, J., Chen, C., Wu, Y., Chen, H., Xiong, J., Long, R., Li, S., Song, L., Jiang, W. & Liu, Z. (2024). Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction. Advanced Materials, e2401914-. https://dx.doi.org/10.1002/adma.202401914 0935-9648 https://hdl.handle.net/10356/177911 10.1002/adma.202401914 38436110 2-s2.0-85187720599 e2401914 en MOE2019-T2-2-105 MOE-MOET2EP10121-0006 RG7/21 Advanced Materials © 2024 Wiley-VCH GmbH. All rights reserved. |
| spellingShingle | Engineering Asymmetric electron redistribution Noncovalent interaction Di, Jun Chen, Chao Wu, Yao Chen, Hao Xiong, Jun Long, Ran Li, Shuzhou Song, Li Jiang, Wei Liu, Zheng Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title | Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title_full | Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title_fullStr | Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title_full_unstemmed | Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title_short | Asymmetric electron redistribution in niobic-oxygen vacancy associates to tune noncovalent interaction in CO2 photoreduction |
| title_sort | asymmetric electron redistribution in niobic oxygen vacancy associates to tune noncovalent interaction in co2 photoreduction |
| topic | Engineering Asymmetric electron redistribution Noncovalent interaction |
| url | https://hdl.handle.net/10356/177911 |
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