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Updated: Oct 28, 2026

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Cation Vacancy-Modulated NiOOH for Electro-Oxidative Alcohol Dehydrogenation and Amide Synthesis Coupled With
Xun Pan1, Suhan Zhang2, Lingzhi Sun1
1Department of Thoracic Surgery, School of Chemical Science and Engineering, Shanghai Tongji Hospital, Tongji University, Shanghai, China.
Abstract:
Utilizing thermodynamically favorable biomass conversion to replace oxygen evolution reactions (OER) can achieve efficient H2 production under low energy consumption. However, this strategy has seldom been studied in the electrosynthesis of C-N oxidative coupling reactions (COR), mainly due to the challenge of simultaneously achieving efficient oxidation and coupling reaction. Herein, an electrochemical etching strategy was employed to prepare a V+-NiOOH catalyst rich in cation vacancies (V+), which succeeded in the electrosynthesis of benzamide from benzyl alcohol (BA) and NH3 at 1.50 V versus RHE, with 86% selectivity and 100% conversion. Synchrotron radiation analysis confirmed that the presence of V+ promoted the generation of high-valent Ni4+(t2g 6 eg 0) species and activated the lattice oxygen in Ni4+-Olat-Ni3+. Related in situ characterization and theoretical calculations explained the significant role of Ni4+-Olat-O∙ in catalyzing the oxidation of O-H and C-H bonds, and the dynamic reconstruction between Ni3+ and Ni4+ inhibited the poisoning effect of NH3 on the catalyst. Notably, by coupling with cathodic H2 production, an amide yield of 0.81 mmol h-1 was achieved under 200 mA, and the H2 production energy consumption was reduced by 24.1%. It provides important guidance for promoting green and efficient utilization of resources and energy.
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