Balancing sub‐reaction activity to boost electrocatalytic urea synthesis using a metal‐free electrocatalyst
Chen Chen,
Shuang Li,
Xiaorong Zhu,
Shuowen Bo,
Kai Cheng,
Nihan He,
Mengyi Qiu,
Chao Xie,
Dezhong Song,
Youzhen Liu,
Wei Chen,
Yafei Li,
Qinghua Liu,
Conggang Li,
Shuangyin Wang
Affiliations
Chen Chen
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Shuang Li
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Xiaorong Zhu
College of Chemistry and Materials Science Nanjing Normal University Nanjing China
Shuowen Bo
National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei China
Kai Cheng
Key Laboratory of Magnetic Resonance in Biological Systems, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan Collaborative Innovation Center of Chemistry for Life Sciences, Wuhan Institute of Physics and Mathematics Chinese Academy of Sciences Wuhan China
Nihan He
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Mengyi Qiu
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Chao Xie
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Dezhong Song
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Youzhen Liu
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Wei Chen
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Yafei Li
College of Chemistry and Materials Science Nanjing Normal University Nanjing China
Qinghua Liu
National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei China
Conggang Li
Key Laboratory of Magnetic Resonance in Biological Systems, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan Collaborative Innovation Center of Chemistry for Life Sciences, Wuhan Institute of Physics and Mathematics Chinese Academy of Sciences Wuhan China
Shuangyin Wang
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
Abstract Electrocatalytic urea synthesis via coupling of nitrate with CO2 is considered as a promising alternative to the industrial urea synthetic process. However, the requirement of sub‐reaction (NO3RR and CO2RR) activities for efficient urea synthesis is not clear and the related reaction mechanisms remain obscure. Here, the construction, breaking, and rebuilding of the sub‐reaction activity balance would be accompanied by the corresponding regulation in urea synthesis, and the balance of sub‐reaction activities was proven to play a vital role in efficient urea synthesis. With rational design, a urea yield rate of 610.6 mg h−1 gcat.−1 was realized on the N‐doped carbon electrocatalyst, superior to that of noble‐metal electrocatalysts. Based on the operando SR‐FTIR measurements, we proposed that urea synthesis arises from the coupling of *NO and *CO to generate the key intermediate of *OCNO. This work provides new insights and guidelines into urea synthesis from the aspect of activity balance.
