Wang Xinyue, Sang Xiahan, Dong Chung-Li, Yao Siyu, Shuai Ling, Lu Jianguo, Yang Bin, Li Zhongjian, Lei Lecheng, Qiu Ming, Dai Liming, Hou Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070, China.
Angew Chem Int Ed Engl. 2021 May 17;60(21):11959-11965. doi: 10.1002/anie.202100011. Epub 2021 Apr 12.
Electrocatalysts play a key role in accelerating the sluggish electrochemical CO reduction (ECR) involving multi-electron and proton transfer. We now develop a proton capture strategy by accelerating the water dissociation reaction catalyzed by transition-metal nanoparticles (NPs) adjacent to atomically dispersed and nitrogen-coordinated single nickel (Ni-N ) active sites to accelerate proton transfer to the latter for boosting the intermediate protonation step, and thus the whole ECR process. Aberration-corrected scanning transmission electron microscopy, X-ray absorption spectroscopy, and calculations reveal that the Ni NPs accelerate the adsorbed H (H ) generation and transfer to the adjacent Ni-N 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.
电催化剂在加速涉及多电子和质子转移的缓慢电化学CO还原（ECR）过程中起着关键作用。我们现在开发了一种质子捕获策略，通过加速由与原子分散且氮配位的单镍（Ni-N）活性位点相邻的过渡金属纳米颗粒（NPs）催化的水离解反应，来加速质子向后者的转移，以促进中间质子化步骤，进而推动整个ECR过程。像差校正扫描透射电子显微镜、X射线吸收光谱和计算结果表明，Ni NPs加速了吸附态H（H ）的生成并将其转移到相邻的Ni-N位点，以促进中间质子化和整个ECR过程。这种质子捕获策略对于设计和制备用于各种电化学反应（甚至超越ECR）的高性能催化剂具有通用性。
