Polarized Cu-Bi site pairs for non-covalent to covalent interaction tuning toward N₂ photoreduction

• المؤلفون الرئيسيون: 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
• مؤلفون آخرون: School of Materials Science and Engineering
• التنسيق: مقال
• اللغة: English
• منشور في: 2022
• الموضوعات: Engineering::Materials; Altered Hydrogenation Pathways; Atomic Layers
• الوصول للمادة أونلاين: https://hdl.handle.net/10356/162503

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 CuOBi 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 NN. 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.