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Synergy of Diatomic CuSb-HAB Catalyst with Methanol Oxidation to Promote Formamide Electrosynthesis
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DOI：10.1039/D6GC01944G.png)
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Abstract
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Electrochemical co-reduction of CO2 and NOx- to formamide (ECNF) provides a promising pathway for sustainable formamide synthesis; yet its electrocatalytic activity and selectivity remain unsatisfactory. Herein; a CuSb-HAB metal-organic framework catalyst; featuring Cu-Sb diatomic sites within a conductive hexaaminobenzene (HAB) matrix; is developed for highly efficient formamide synthesis from co-electrolysis of CO2 and NO2-. Theoretical calculations and in situ spectroscopic characterizations unravel the essential role of d-p hybridized Cu-Sb diatomic sites in synergistically stabilizing two key intermediates (*CHO and *NH2) and promoting their C-N coupling for formamide synthesis. Notably; a two-electrode MEA electrolyzer integrating cathodic ECNF with anodic methanol oxidation delivers the outstanding Faradaic efficiency of 61.21% and formamide yield rates of 777.9 mmol h-1 g-1; together with the exceptional electrolysis durability for over 200 h; representing one of the highest reported values.
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