Premium
Turning on Zn 4s Electrons in a N 2 ‐Zn‐B 2 Configuration to Stimulate Remarkable ORR Performance
Author(s) -
Wang Jing,
Li Hongguan,
Liu Shuhu,
Hu Yongfeng,
Zhang Jing,
Xia Meirong,
Hou Yanglong,
Tse John,
Zhang Jiujun,
Zhao Yufeng
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202009991
Subject(s) - delocalized electron , catalysis , chemistry , transition metal , atom (system on chip) , electron configuration , zinc , metal , electrocatalyst , crystallography , inorganic chemistry , nanotechnology , materials science , electrochemistry , organic chemistry , ion , computer science , embedded system , electrode
A zinc‐based single‐atom catalyst has been recently explored with distinguished stability, of which the fully occupied Zn 2+ 3d 10 electronic configuration is Fenton‐reaction‐inactive, but the catalytic activity is thus inferior. Herein, we report an approach to manipulate the s‐band by constructing a B,N co‐coordinated Zn‐B/N‐C catalyst. We confirm both experimentally and theoretically that the unique N 2 ‐Zn‐B 2 configuration is crucial, in which Zn + (3d 10 4s 1 ) can hold enough delocalized electrons to generate suitable binding strength for key reaction intermediates and promote the charge transfer between catalytic surface and ORR reactants. This exclusive effect is not found in the other transition‐metal counterparts such as M‐B/N‐C (M=Mn, Fe, Co, Ni and Cu). Consequently, the as‐obtained catalyst demonstrates impressive ORR activity, along with remarkable long‐term stability in both alkaline and acid media. This work presents a new concept in the further design of electrocatalyst.