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Regulating the Local Charge Distribution of Ni Active Sites for the Urea Oxidation Reaction
Author(s) -
Wang Liping,
Zhu Yajie,
Wen Yunzhou,
Li Shangyu,
Cui Chunyu,
Ni Fenglou,
Liu Yunxia,
Lin Haiping,
Li Youyong,
Peng Huisheng,
Zhang Bo
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202100610
Subject(s) - catalysis , oxygen evolution , anode , chemistry , inorganic chemistry , electrochemistry , dopant , faraday efficiency , nickel , carbon monoxide , electrolysis , materials science , electrode , doping , organic chemistry , optoelectronics , electrolyte
In electrochemical energy storage and conversion systems, the anodic oxygen evolution reaction (OER) accounts for a large proportion of the energy consumption. The electrocatalytic urea oxidation reaction (UOR) is one of the promising alternatives to OER, owing to its low thermodynamic potential. However, owing to the sluggish UOR kinetics, its potential in practical use has not been unlocked. Herein, we developed a tungsten‐doped nickel catalyst (Ni‐WO x ) with superior activity towards UOR. The Ni‐WO x catalyst exhibited record fast reaction kinetics (440 mA cm −2 at 1.6 V versus reversible hydrogen electrode) and a high turnover frequency of 0.11 s −1 , which is 4.8 times higher than that without W dopants. In further experiments, we found that the W dopant regulated the local charge distribution of Ni atoms, leading to the formation of Ni 3+ sites with superior activity and thus accelerating the interfacial catalytic reaction. Moreover, when we integrated Ni‐WO x into a CO 2 flow electrolyzer, the cell voltage is reduced to 2.16 V accompanying with ≈98 % Faradaic efficiency towards carbon monoxide.