期刊
ACS NANO
卷 16, 期 5, 页码 8213-8222出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c01956
关键词
electrocatalysis; C-N coupling; defect engineering; urea synthesis; indium oxyhydroxide
类别
资金
- National Natural Science Foundation of China [52101246]
- Fundamental Research Funds for the Central Universities [WK2310000099, 5710010721]
- Singapore MOE AcRF Tier 1 Grant [2020-T1-001-031]
- Singapore A*STAR project [A19D9a0096]
- Camille Dreyfus TeacherScholar Award
- Welch Foundation Award [F-1861]
- Users with Excellence program of Hefei Science Center of CAS [2020HSC-UE003]
Indium oxyhydroxide electrocatalyst with defect engineering has been developed for efficient synthesis of urea. By studying the catalytic mechanism, this design strategy may lead to the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications.
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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