Continuous Coupling Mechanism for High Rate Electrosynthesis of Urea on Sulfur‐Coordinated Adjacent Copper Sites
Abstract
Abstract The co‐electrolysis of nitrate (NO 3 − ) and carbon dioxide (CO 2 ) to synthesize urea can satisfy the comprehensive needs of carbon footprint closure, waste valorization, and sustainable urea production. However, designing efficient electrocatalysts to promote the electrocatalytic C─N coupling process and achieve efficient urea production remains a challenge. Here, we design a copper (Cu)‐based coordination polymer catalyst, which can achieve the dual function of promoting C─N coupling and protonation through sulfur (S)‐coordinated adjacent Cu sites. Through the unique Continuous Coupling Mechanism (CCM) of low Gibbs free energy of reaction intermediates (*CO 2 + *NO to *CO 2 NO to *ONCO 2 NO), the resulting catalyst achieved ultra‐high Faradaic efficiency (FE) (84.9 ± 3.1%) and production rate (0.34 ± 0.012 mol h −1 g −1 ). Moreover, the FE and production rate of urea did not change noticeably during at least 90 cycles of testing.
Article Details
Authors (14)
Xiao Chen
Shuaiqiang Jia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Jianxin Zhai
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Jiapeng Jiao
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mengke Dong
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Cheng Xue
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Zhanghui Xia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Ting Deng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Hailian Cheng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Chunjun Chen
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Xueqing Xing
Beijing Synchrotron Radiation Facility
Haihong Wu
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mingyuan He
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,