Ligand engineering towards electrocatalytic urea synthesis on a molecular catalyst

Han Li, Leitao Xu, Shuowen Bo, Yujie Wang, Han Xu, Chen Chen (), Ruping Miao, Dawei Chen (), Kefan Zhang, Qinghua Liu, Jingjun Shen, Huaiyu Shao, Jianfeng Jia and Shuangyin Wang ()
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Han Li: Hunan University
Leitao Xu: Hunan University
Shuowen Bo: University of Science and Technology of China
Yujie Wang: Hunan University
Han Xu: Hunan University
Chen Chen: Hunan University
Ruping Miao: Hunan University
Dawei Chen: Hunan University
Kefan Zhang: Hunan University
Qinghua Liu: University of Science and Technology of China
Jingjun Shen: University of Macau
Huaiyu Shao: University of Macau
Jianfeng Jia: Shanxi Normal University
Shuangyin Wang: Hunan University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Electrocatalytic C-N coupling from carbon dioxide and nitrate provides a sustainable alternative to the conventional energy-intensive urea synthetic protocol, enabling wastes upgrading and value-added products synthesis. The design of efficient and stable electrocatalysts is vital to promote the development of electrocatalytic urea synthesis. In this work, copper phthalocyanine (CuPc) is adopted as a modeling catalyst toward urea synthesis owing to its accurate and adjustable active configurations. Combining experimental and theoretical studies, it can be observed that the intramolecular Cu-N coordination can be strengthened with optimization in electronic structure by amino substitution (CuPc-Amino) and the electrochemically induced demetallation is efficiently suppressed, serving as the origination of its excellent activity and stability. Compared to that of CuPc (the maximum urea yield rate of 39.9 ± 1.9 mmol h−1 g−1 with 67.4% of decay in 10 test cycles), a high rate of 103.1 ± 5.3 mmol h−1 g−1 and remarkable catalytic durability have been achieved on CuPc-Amino. Isotope-labelling operando electrochemical spectroscopy measurements are performed to disclose reaction mechanisms and validate the C-N coupling processes. This work proposes a unique scheme for the rational design of molecular electrocatalysts for urea synthesis.

Date: 2024
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DOI: 10.1038/s41467-024-52832-2

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