Identifying and tailoring C-N coupling site for efficient urea synthesis over diatomic Fe-Ni catalyst

Xiaoran Zhang; Xiaorong Zhu; Shuowen Bo; Chen Chen; Mengyi Qiu; Xiaoxiao Wei; Nihan He; Chao Xie; Wei Chen; Jianyun Zheng; Pinsong Chen; San Ping Jiang; Yafei Li; Qinghua Liu; Shuangyin Wang

doi:10.1038/s41467-022-33066-6

Identifying and tailoring C-N coupling site for efficient urea synthesis over diatomic Fe-Ni catalyst

Nat Commun. 2022 Sep 10;13(1):5337. doi: 10.1038/s41467-022-33066-6.

Authors

Xiaoran Zhang^#^{1

2}, Xiaorong Zhu^#³, Shuowen Bo^#⁴, Chen Chen⁵, Mengyi Qiu¹, Xiaoxiao Wei¹, Nihan He¹, Chao Xie¹, Wei Chen¹, Jianyun Zheng⁶, Pinsong Chen², San Ping Jiang^{7

8}, Yafei Li³, Qinghua Liu⁴, Shuangyin Wang⁹

Affiliations

¹ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, People's Republic of China.
² WA School of Mines: Minerals, Energy & Chemical Engineering, Curtin University, Perth, WA, 6102, Australia.
³ College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, Jiangsu, People's Republic of China.
⁴ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, People's Republic of China.
⁵ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, People's Republic of China. chenc@hnu.edu.cn.
⁶ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, People's Republic of China. jyzheng@hnu.edu.cn.
⁷ WA School of Mines: Minerals, Energy & Chemical Engineering, Curtin University, Perth, WA, 6102, Australia. s.jiang@curtin.edu.au.
⁸ Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan, 528216, People's Republic of China. s.jiang@curtin.edu.au.
⁹ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, People's Republic of China. shuangyinwang@hnu.edu.cn.

^# Contributed equally.

Abstract

Electrocatalytic urea synthesis emerged as the promising alternative of Haber-Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe-Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe-Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C-N coupling thermodynamically and kinetically. The performance for urea synthesis up to an order of magnitude higher than those of single-atom and isolated diatomic electrocatalysts, a high urea yield rate of 20.2 mmol h^-1 g^-1 with corresponding Faradaic efficiency of 17.8% has been successfully achieved. A total Faradaic efficiency of about 100% for the formation of value-added urea, CO, and NH₃ was realized. This work presents an insight into synergistic catalysis towards sustainable urea synthesis via identifying and tailoring the atomic site configurations.

Abstract

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