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Selective Glycine Electrosynthesis via C-N Coupling Enabled by Synergistic Mott-Schottky Heterojunction and Oxygen
Guangkuo Xu1, Chengyuan Dong1,2, Xiangcheng Cai1
1State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian, China.
Abstract:
Glycine, an indispensable amino acid essential for diverse biological processes, remains challenging to synthesize directly via electrosynthesis from simple carbon and nitrogen precursors. Herein, we report a highly efficient electrochemical route for glycine production through the reductive coupling of oxalic acid (H2C2O4) with hydroxylamine (NH2OH) or nitrate (NO3 -) over a Mott-Schottky Sn/SnO2 heterojunction catalyst enriched with oxygen vacancies. When employing H2C2O4 and NH2OH as feedstocks, a remarkable Faradaic efficiency (FE) of 91.6% for glycine is achieved at -0.7 V versus RHE, alongside a high yield of 135 mmol gcat. -1 h-1. To the best of our knowledge, this represents one of the best performances ever reported in this system. The catalyst also shows strong substrate versatility, enabling efficient glycine formation when NO3 - (in situ reduced to NH2OH) couples with glyoxylic acid or H2C2O4. Mechanistic studies indicate that the Mott-Schottky heterojunction significantly promotes the co-adsorption of H2C2O4 and NH2OH, while oxygen vacancies facilitate the hydrogenation of oxime intermediates to glycine. This study highlights the profound synergistic interplay between Mott-Schottky heterojunctions and oxygen vacancy defects in precisely modulating active sites and accelerating reaction kinetics, thereby offering a sustainable strategy for the green electrosynthesis of amino acids.
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