电合成
材料科学
氨
极化(电化学)
纳米技术
表面改性
电化学
化学工程
物理化学
有机化学
电极
化学
工程类
作者
Hongbo Wang,Chenyang Zhang,B. Liu,Wenqing Li,Changzhong Jiang,Zunjian Ke,Dong He,Xiangheng Xiao
标识
DOI:10.1002/adma.202401032
摘要
Abstract Electrocatalytic N 2 reduction reaction (NRR) to synthesize ammonia is a sustainable reaction that is expected to replace Haber Bosch process. Laminated Bi 2 WO 6 has great potential as an NRR electrocatalyst, however, the effective activity requires that the inert substrate is fully activated. Here, we succeeded for the first time in activating the Bi 2 WO 6 basal planes with NRR activity through Ti doping. The introduction of Ti successfully tunes the surface potential distribution and enhances the N 2 adsorption. The subsequently strong hybrid coupling of d(Ti)‐p(N) orbitals fills the electronic state of N 2 antibonding molecular orbital, which greatly weakens the bonding strength of N≡N bonds. Further, in situ SR‐FTIR spectrum and theoretical calculations showed that surface potential polarization enhanced the adsorption of HNN* by Bi‐Ti dual‐metal sites, which is beneficial for the subsequent activation hydrogenation process. The Ti‐Bi 2 WO 6 nanosheets achieved 11.44% Faradaic efficiency (‐0.2 V), a NH 3 yield rate of 23.14 µg mg −1 h −1 ( 15 N calibration), and satisfactory stability in 0.1 M HCl environment. The mutual assistance of theory and experiment can help understand and develop of excellent two‐dimensional (2D) materials for the NRR. This article is protected by copyright. All rights reserved
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