Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction
A universal atomic layer confined doping strategy is developed to prepare Bi24 O31 Br10 materials incorporating isolated Cu atoms. The local polarization can be created along the CuOBi atomic interface, which enables better electron delocalization for effective N2 activation. The optimized Cu-Bi24...
Saved in:
Main Authors: | , , , , , , , , , , , , , , , , |
---|---|
Other Authors: | |
Format: | Article |
Language: | English |
Published: |
2022
|
Subjects: | |
Online Access: | https://hdl.handle.net/10356/162503 |
Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
Institution: | Nanyang Technological University |
Language: | English |
id |
sg-ntu-dr.10356-162503 |
---|---|
record_format |
dspace |
spelling |
sg-ntu-dr.10356-1625032022-11-11T06:36:16Z Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction Di, Jun Chen, Chao Wu, Yao Zhao, Yunxuan Zhu, Chao Zhang, Yi Wang, Changda Chen, Hailong Xiong, Jun Xu, Manzhang Xia, Jiexiang Zhou, Jiadong Weng, Yuxiang Song, Li Li, Shuzhou Jiang, Wei Liu, Zheng School of Materials Science and Engineering School of Electrical and Electronic Engineering The Photonics Institute CNRS International NTU THALES Research Alliances Engineering::Materials Altered Hydrogenation Pathways Atomic Layers A universal atomic layer confined doping strategy is developed to prepare Bi24 O31 Br10 materials incorporating isolated Cu atoms. The local polarization can be created along the CuOBi atomic interface, which enables better electron delocalization for effective N2 activation. The optimized Cu-Bi24 O31 Br10 atomic layers show 5.3× and 88.2× improved photocatalytic nitrogen fixation activity than Bi24 O31 Br10 atomic layer and bulk Bi24 O31 Br10 , 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 NN. As a result, the hydrogenation pathways can be altered from the associative distal pathway for Bi24 O31 Br10 to the alternating pathway for Cu-Bi24 O31 Br10 . This strategy provides an accessible pathway for designing polarized metal site pairs or tuning the non-covalent interaction and covalent bond order. Ministry of Education (MOE) Submitted/Accepted version This work was supported by Singapore Ministry of Education AcRF Tier 2 (MOE2019-T2-2-105), AcRF Tier 1 RG4/17, RG161/19, Fundamental Research Funds for the Central Universities (Project 30922010302) and Start-Up Grant (Project AE89991/397) from Nanjing University of Science and Technology. 2022-10-26T07:45:29Z 2022-10-26T07:45:29Z 2022 Journal Article Di, J., Chen, C., Wu, Y., Zhao, Y., Zhu, C., Zhang, Y., Wang, C., Chen, H., Xiong, J., Xu, M., Xia, J., Zhou, J., Weng, Y., Song, L., Li, S., Jiang, W. & Liu, Z. (2022). Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction. Advanced Materials, 34(37), 2204959-. https://dx.doi.org/10.1002/adma.202204959 0935-9648 https://hdl.handle.net/10356/162503 10.1002/adma.202204959 35863016 2-s2.0-85135805729 37 34 2204959 en MOE2019-T2-2-105 RG4/17 RG161/19 Advanced Materials © 2022 Wiley-VCH GmbH. All rights reserved. This is the peer reviewed version of the following article: Di, J., Chen, C., Wu, Y., Zhao, Y., Zhu, C., Zhang, Y., Wang, C., Chen, H., Xiong, J., Xu, M., Xia, J., Zhou, J., Weng, Y., Song, L., Li, S., Jiang, W. & Liu, Z. (2022). Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction. Advanced Materials, 34(37), 2204959-, which has been published in final form at https://doi.org/10.1002/adma.202204959. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. application/pdf |
institution |
Nanyang Technological University |
building |
NTU Library |
continent |
Asia |
country |
Singapore Singapore |
content_provider |
NTU Library |
collection |
DR-NTU |
language |
English |
topic |
Engineering::Materials Altered Hydrogenation Pathways Atomic Layers |
spellingShingle |
Engineering::Materials Altered Hydrogenation Pathways Atomic Layers Di, Jun Chen, Chao Wu, Yao Zhao, Yunxuan Zhu, Chao Zhang, Yi Wang, Changda Chen, Hailong Xiong, Jun Xu, Manzhang Xia, Jiexiang Zhou, Jiadong Weng, Yuxiang Song, Li Li, Shuzhou Jiang, Wei Liu, Zheng Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
description |
A universal atomic layer confined doping strategy is developed to prepare Bi24 O31 Br10 materials incorporating isolated Cu atoms. The local polarization can be created along the CuOBi atomic interface, which enables better electron delocalization for effective N2 activation. The optimized Cu-Bi24 O31 Br10 atomic layers show 5.3× and 88.2× improved photocatalytic nitrogen fixation activity than Bi24 O31 Br10 atomic layer and bulk Bi24 O31 Br10 , 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 NN. As a result, the hydrogenation pathways can be altered from the associative distal pathway for Bi24 O31 Br10 to the alternating pathway for Cu-Bi24 O31 Br10 . This strategy provides an accessible pathway for designing polarized metal site pairs or tuning the non-covalent interaction and covalent bond order. |
author2 |
School of Materials Science and Engineering |
author_facet |
School of Materials Science and Engineering Di, Jun Chen, Chao Wu, Yao Zhao, Yunxuan Zhu, Chao Zhang, Yi Wang, Changda Chen, Hailong Xiong, Jun Xu, Manzhang Xia, Jiexiang Zhou, Jiadong Weng, Yuxiang Song, Li Li, Shuzhou Jiang, Wei Liu, Zheng |
format |
Article |
author |
Di, Jun Chen, Chao Wu, Yao Zhao, Yunxuan Zhu, Chao Zhang, Yi Wang, Changda Chen, Hailong Xiong, Jun Xu, Manzhang Xia, Jiexiang Zhou, Jiadong Weng, Yuxiang Song, Li Li, Shuzhou Jiang, Wei Liu, Zheng |
author_sort |
Di, Jun |
title |
Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
title_short |
Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
title_full |
Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
title_fullStr |
Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
title_full_unstemmed |
Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction |
title_sort |
polarized cu-bi site pairs for non-covalent to covalent interaction tuning toward n₂ photoreduction |
publishDate |
2022 |
url |
https://hdl.handle.net/10356/162503 |
_version_ |
1751548487738064896 |