Durable and efficient urea electrosynthesis using carbon dioxide and nitrate over defect-rich In2O3 nanotubes

Electrochemical conversion of CO2 and NO3− waste (EC-CO2/NO3−) into valuable urea is a promising method for fertilizer production and environmental remediation, but its practical application is currently limited by the low efficiency of electrocatalytic processes. Here, we report a novel In2O3 nanot...

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Bibliographic Details
Published in:Green chemistry : an international journal and green chemistry resource : GC 2024, Vol.26 (11), p.6812-6821
Main Authors: Fang, Hongjun, Chen-Han, Kuo, Yang, Hongsheng, Wang, Ze, Feng, Xinzhen, Ji, Weijie, Chak-Tong Au
Format: Article
Language:English
Subjects:
Carbon dioxide
Catalysts
Chemical synthesis
Defects
Efficiency
Electrocatalysts
Electrochemistry
Environmental cleanup
Fourier transforms
Indium oxides
Infrared reflection
Infrared spectroscopy
Metal-organic frameworks
Nanotechnology
Nanotubes
Nitrates
Production methods
Urea
Ureas
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Summary:Electrochemical conversion of CO2 and NO3− waste (EC-CO2/NO3−) into valuable urea is a promising method for fertilizer production and environmental remediation, but its practical application is currently limited by the low efficiency of electrocatalytic processes. Here, we report a novel In2O3 nanotube (In2O3-NT) material derived from a metal–organic framework (MOF) which functions as an electrocatalyst for durable and efficient urea synthesis via EC-CO2/NO3−. The obtained In2O3-NT-500 with a porous structure and rich oxygen vacancies (Vo) is more conducive to the target reaction system, reaching a urea formation rate of 1441 μg mgcat−1 h−1 with a high faradaic efficiency of 60.3%, exhibiting the top-level performance toward urea synthesis via the current route. In situ attenuated total reflection Fourier transform infrared spectroscopy verified that In2O3-NT with enriched Vo could stabilize the *CO2NH2 intermediate, thus accelerating the rate-determining step (RDS). The DFT simulation demonstrated that the transformation of *COOHNH2 to *CONH2 is the RDS for urea formation. The defect-engineered In2O3-NT catalyst significantly lowers the energy barrier for this step, thus boosting the overall efficiency of urea synthesis. This work provides an example showing that the defect engineering of In2O3-NT is highly capable of activating CO2 and NO3− waste molecules for urea synthesis, and is conceptually versatile for other value-added chemical production methods.
ISSN:1463-9262
1463-9270
DOI:10.1039/d4gc01630k