Asymmetric Associate Configuration of Nb Single Atoms Coupled Bi–O Vacancy Pairs Boosting CO<sub>2</sub> Photoreduction
Precisely designing the atomic coordination structure of the catalytic center is highly desired to lower the energy barrier of CO2 photoreduction. The present work shows that engineering Nb single atom coupled Bi–O vacancy pairs (VBi–O) into Bi24O31Br10 (BOB) atomic layers can create a preferential local asymmetric structure. This configuration can result in a stronger local polarization electric field and thus prolong the carrier lifetime, as proved by ultrafast transient absorption spectroscopy. Meantime, this unique Nb SA-VBi–O associate favors the formation of strong chemical interaction between key *COOH intermediate and catalytic center, thus lowering the energy barrier of the rate-limiting step. Benefiting from these features, a high CO generation rate of 76.4 μmol g–1 h–1 for CO2 photoreduction can be achieved over Nb SA-VBi–O BOB atomic layers in pure water, roughly 5.4 and 92.7 times higher than those of BOB atomic layers or bulk BOB, respectively. This work discloses an important paradigm for designing single atom coupled defect associates to optimize photocatalysis performance.
Authors
- Wei Jiang (ORCID: https://orcid.org/0000-0001-5663-9119)
- Xingzhong Cao (ORCID: https://orcid.org/0000-0001-5011-5912)
- Ran Long (ORCID: https://orcid.org/0000-0003-4845-9120)
- Peng Zhou (ORCID: https://orcid.org/0000-0001-8034-8282)
- Jun Di (ORCID: https://orcid.org/0000-0002-6232-6466)
- Hongwei Shou (ORCID: https://orcid.org/0000-0002-1012-5814)
- Yao Wu (ORCID: https://orcid.org/0000-0003-0443-8571)
- Jun Xiong (ORCID: https://orcid.org/0000-0002-0596-7232)
- Peng Zhang (ORCID: https://orcid.org/0000-0001-9505-3858)
- Zheng Liu (ORCID: https://orcid.org/0000-0002-8825-7198)
- Li Song (ORCID: https://orcid.org/0000-0003-0585-8519)
- Hailong Chen (ORCID: https://orcid.org/0000-0002-3456-7836)
Institutions
- Jiangsu University (CN)
- University of Science and Technology of China (CN)
- Nanyang Technological University (SG)
- Chinese Academy of Sciences (CN)
- Peking University (CN)
- Nanjing University of Science and Technology (CN)
- Institute of High Energy Physics (CN)
- National Synchrotron Radiation Laboratory (CN)
- Institute of Physics (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2024-11-18
- DOI
- https://doi.org/10.1021/acscatal.4c04407
- Citations
- 21
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 2.46
Funders
- Ministry of Education - Singapore
- National Natural Science Foundation of China
- Fundamental Research Funds for the Central Universities