Tuning Intermediates Adsorption and C─N Coupling for Efficient Urea Electrosynthesis Via Doping Ni into Cu

Author:

Zhang Yangyang12,Zhao Yajun1,Sendeku Marshet Getaye3,Li Fuhua2,Fang Jinjie1,Wang Yuan1,Zhuang Zhongbin1,Kuang Yun13,Liu Bin4ORCID,Sun Xiaoming1

Affiliation:

1. State Key Lab of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China

2. School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 62 Nanyang Drive Singapore 639798 Singapore

3. Ocean Hydrogen Energy R&D Center Research Institute of Tsinghua University in Shenzhen Shenzhen 518057 P. R. China

4. Department of Materials Science and Engineering City University of Hong Kong China Hong Kong SAR 999077 P. R. China

Abstract

AbstractSimultaneous electrochemical reduction of nitrite and carbon dioxide (CO2) under mild reaction conditions offers a new sustainable and low‐cost approach for urea synthesis. However, the development of urea electrosynthesis thus far still suffers from low selectivity due to the high energy barrier of *CO formation and the subsequent C─N coupling. In this work, a highly active dendritic Cu99Ni1 catalyst is developed to enable the highly selective electrosynthesis of urea from co‐reduction of nitrite and CO2, reaching a urea Faradaic efficiency (FE) and production rate of 39.8% and 655.4 µg h−1 cm−2, respectively, at −0.7 V versus reversible hydrogen electrode (RHE). In situ Fourier‐transform infrared spectroscopy (FT‐IR) measurements together with density functional theory (DFT) calculations demonstrate that Ni doping into Cu can significantly enhance the adsorption energetics of the key reaction intermediates and facilitate the C─N coupling. This work not only provides a new strategy to design efficient electrocatalysts for urea synthesis but also offers deep insights into the mechanism of C─N coupling during the co‐reduction of nitrite and CO2.

Funder

National Natural Science Foundation of China

Fundamental Research Funds for the Central Universities

Publisher

Wiley

Subject

General Materials Science,General Chemistry

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