Regulating the Local Charge Distribution of Ni Active Sites for the Urea Oxidation Reaction
Regulating the Local Charge Distribution of Ni Active Sites for the Urea Oxidation Reaction
复制标题
尿素氧化反应镍活性位点局部电荷分布的调控
DOI：
10.1002/anie.202100610
复制
发表时间：
2021-03-30
影响因子：
16.6
通讯作者：
Zhang, Bo
中科院分区：
文献类型：
--
作者：
Wang, Liping;Zhu, Yajie;Zhang, Bo
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-WOx) with superior activity towards UOR. The Ni-WOx 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 Ni3+ sites with superior activity and thus accelerating the interfacial catalytic reaction. Moreover, when we integrated Ni-WOx into a CO2 flow electrolyzer, the cell voltage is reduced to 2.16 V accompanying with approximate to 98 % Faradaic efficiency towards carbon monoxide.
