journal article·2022-05-24

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

Chade Lv, Carmen Lee, Lixiang Zhong, Hengjie Liu, Jiawei Liu, Lan Yang, Chunshuang Yan, Wei Yu, Huey Hoon Hng, Zeming Qi, Li Song, Shuzhou Li, Kian Ping Loh, Qingyu Yan, Guihua Yu

ACS Nano· Volume 16· Issue 5
Publisher page

Abstract

Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C–N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation–Fourier transform infrared spectroscopy showcases that *CO2NH2 protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO2NH2 intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications.
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Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Electrocatalysts for Energy Conversion · Covalent Organic Framework Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150001, China

School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore

National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China

Department of Chemistry, National University of Singapore, Singapore 117543, Singapore

Materials Science and Engineering Program, Walker Department of Mechanical Engineering, Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States

Funding

Welch Foundation · Agency for Science, Technology and Research · Ministry of Education - Singapore · Camille and Henry Dreyfus Foundation · Central University Basic Research Fund of China · National Natural Science Foundation of China · Hefei Science Center, Chinese Academy of Sciences

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