Oxygen Vacancy-Mediated Selective C–N Coupling toward Electrocatalytic Urea Synthesis

2022/06/24 by Xiaoxiao Wei, Xiaojian Wen, Yingying Liu +12 · 4 citations
Chemical Engineering · Chemistry · Energy · #Advanced Photocatalysis Techniques #Ammonia Synthesis and Nitrogen Reduction #Catalytic Cross-Coupling Reactions

paper · doi:10.1021/jacs.2c03452

openalex publication_date 2022/06/24 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/30

Abstract

The electrocatalytic C–N coupling for one-step urea synthesis under ambient conditions serves as the promising alternative to the traditional urea synthetic protocol. However, the hydrogenation of intermediate species hinders the efficient urea synthesis. Herein, the oxygen vacancy-enriched CeO 2 was demonstrated as the efficient electrocatalyst with the stabilization of the crucial intermediate of *NO via inserting into vacant sites, which is conducive to the subsequent C–N coupling process rather than protonation, whereas the poor selectivity of C–N coupling with protonation was observed on the vacancy-deficient catalyst. The oxygen vacancy-mediated selective C–N coupling was distinguished and validated by the in situ sum frequency generation spectroscopy. The introduction of oxygen vacancies tailors the common catalyst carrier into an efficient electrocatalyst with a high urea yield rate of 943.6 mg h –1 g –1, superior than that of partial noble-metal-based electrocatalysts. This work provides novel insights into the catalyst design and developments of coupling systems.

Citations

• How a century of ammonia synthesis changed the world
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Cited by

• Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys
• Designing Efficient Nitrate Reduction Electrocatalysts by Identifying and Optimizing Active Sites of Co-Based Spinels
• Carbon Dioxide and Nitrate Electrocatalytic C-N Coupling for Sustainable Production of Urea
• Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites

Related

• A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions
• Recent Advances in Urea Electrocatalysis: Applications, Materials and Mechanisms †
• Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites
• Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst
• Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis