澳大利亚新南威尔士大学Liming Dai团队揭示了原子分散金属氮活性中心上增强电化学CO2还原的质子捕获策略。相关研究成果于2021年2月18日发表在《德国应用化学》。

电催化剂在加速涉及多电子和质子转移的缓慢电化学CO2还原（ECR）过程中起着关键作用。

研究人员开发了一种质子捕获策略，通过加速邻近原子分散和氮配位单镍（Ni‐Nx）活性中心的过渡金属纳米颗粒（NPs）催化的水离解反应，加速质子转移到后者，以促进中间质子化步骤，最终完成整个ECR过程。该加速质子化过程在实验上得到了充分的证明。像差校正扫描透射电子显微镜和X射线吸收光谱以及理论计算表明，Ni NPs加速了吸附H（Had）的产生并转移到相邻的Ni-Nx位置，从而促进中间质子化和整个ECR过程。

开发的质子捕获策略对于设计和制备各种高性能的催化剂是通用的，甚至可以用于ECR以外的各种电化学反应。

附：英文原文

Title: Proton capture strategy for enhancing electrochemical CO2 reduction on atomically dispersed metal‐nitrogen active sites

Author: Xinyue Wang, Xiahan Sang, Chung-Li Dong, Siyu Yao, Ling Shuai, Jianguo Lu, Bin Yang, Zhongjian Li, Lecheng Lei, Ming Qiu, Liming Dai, Yang Hou

Issue&Volume: 2021-02-18

Abstract: Electrocatalysts play a key role in accelerating the sluggish electrochemical CO2 reduction (ECR) involving multi‐electron and proton transfer. Herein, we develop a proton capture strategy via accelerating the water dissociation reaction catalyzed by transition metal nanoparticles (NPs) adjacent to atomically dispersed and nitrogen coordinated single nickel (Ni‐Nx) active sites to accelerate the proton transfer to the latter for boosting the intermediate protonation step, and hence the whole ECR process. This accelerated protonation process is amply demonstrated experimentally. Aberration‐corrected scanning transmission electron microscopy and X‐ray absorption spectroscopy, together with theoretical calculations, reveals that Ni NPs accelerate the adsorbed H (Had) generation and transfer to the adjacent Ni‐Nx sites for boosting the intermediate protonation and the overall ECR processes. This proton capture strategy is universal to design and prepare for various high‐performance catalysts for diverse electrochemical reactions even beyond ECR.

DOI: 10.1002/anie.202100011

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202100011