journal article·2022-09Open access

Polarized Cu–Bi Site Pairs for Non‐Covalent to Covalent Interaction Tuning toward N2 Photoreduction

Jun Di, Chao Chen, Yao Wu, Yunxuan Zhao, Chao Zhu, Yi Zhang, Changda Wang, Hailong Chen, Jun Xiong, Manzhang Xu, Jiexiang Xia, Jiadong Zhou, Yuxiang Weng, Li Song, Shuzhou Li, Wei Jiang, Zheng Liu

Advanced Materials· Volume 34· Issue 37

Abstract

Abstract A universal atomic layer confined doping strategy is developed to prepare Bi24O31Br10 materials incorporating isolated Cu atoms. The local polarization can be created along the CuOBi atomic interface, which enables better electron delocalization for effective N2 activation. The optimized Cu‐Bi24O31Br10 atomic layers show 5.3× and 88.2× improved photocatalytic nitrogen fixation activity than Bi24O31Br10 atomic layer and bulk Bi24O31Br10, respectively, with the NH3 generation rate reaching 291.1 µmol g−1 h−1 in pure water. The polarized Cu–Bi site pairs can increase the non‐covalent interaction between the catalyst's surface and N2 molecules, then further weaken the covalent bond order in NN. As a result, the hydrogenation pathways can be altered from the associative distal pathway for Bi24O31Br10 to the alternating pathway for Cu‐Bi24O31Br10. This strategy provides an accessible pathway for designing polarized metal site pairs or tuning the non‐covalent interaction and covalent bond order.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Advanced Photocatalysis Techniques · Ammonia Synthesis and Nitrogen Reduction · Copper-based nanomaterials and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research Center Nanjing University of Science and Technology Nanjing 210094 P. R. China

School of Materials Science and Engineering Nanyang Technological University Singapore 639798 Singapore

Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China

School of Chemistry and Chemical Engineering Institute for Energy Research Jiangsu University Zhenjiang 212013 P. R. China

National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230029 P. R. China

Laboratory of Soft Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 P. R. China

School of Electrical and Electronic Engineering and The Photonics Institute Nanyang Technological University Singapore 639798 Singapore

CINTRA CNRS/NTU/THALES UMI 3288 Research Techno Plaza Singapore Singapore

Funding

Nanjing University of Science and Technology · Fundamental Research Funds for the Central Universities

References (31)

Show source-provided references
1. 10.1126/science.abg237110.1126/science.abg2371 ↗
2. 10.1038/s41929-018-0092-710.1038/s41929-018-0092-7 ↗
3. 10.1002/anie.20220093710.1002/anie.202200937 ↗
4. 10.1016/j.nanoen.2020.10542910.1016/j.nanoen.2020.105429 ↗
5. 10.1039/C9MH01668F10.1039/C9MH01668F ↗
6. 10.1021/jacs.0c1334210.1021/jacs.0c13342 ↗
7. 10.1002/anie.20201019210.1002/anie.202010192 ↗
8. 10.1002/adma.20200818010.1002/adma.202008180 ↗
9. 10.1002/anie.20210400110.1002/anie.202104001 ↗
10. 10.1021/acsami.6b0812910.1021/acsami.6b08129 ↗
11. 10.1002/aenm.20200219910.1002/aenm.202002199 ↗
12. 10.1002/anie.20190864010.1002/anie.201908640 ↗
13. 10.1002/adma.20170177410.1002/adma.201701774 ↗
14. 10.1021/jacs.0c0509710.1021/jacs.0c05097 ↗
15. 10.1038/nmat175210.1038/nmat1752 ↗
16. 10.1021/acs.nanolett.1c0038310.1021/acs.nanolett.1c00383 ↗
17. 10.1021/jacs.1c0803310.1021/jacs.1c08033 ↗
18. 10.1039/C4CS00236A10.1039/C4CS00236A ↗
19. 10.1002/adma.20170454810.1002/adma.201704548 ↗
20. 10.1002/aenm.20210238910.1002/aenm.202102389 ↗
21. 10.1038/s41467-019-10392-w10.1038/s41467-019-10392-w ↗
22. 10.1021/jacs.7b0045210.1021/jacs.7b00452 ↗
23. 10.1002/anie.20201359410.1002/anie.202013594 ↗
24. 10.1002/aenm.20190197310.1002/aenm.201901973 ↗
25. 10.1038/s41563-019-0344-110.1038/s41563-019-0344-1 ↗
26. 10.1002/anie.20191243910.1002/anie.201912439 ↗
27. 10.1002/adma.20170382810.1002/adma.201703828 ↗
28. 10.1002/adma.20180757610.1002/adma.201807576 ↗
29. 10.1021/jacs.5b0310510.1021/jacs.5b03105 ↗
30. 10.1038/s41929-019-0241-710.1038/s41929-019-0241-7 ↗
31. 10.1002/adma.20200789110.1002/adma.202007891 ↗