Journal
NANO-MICRO LETTERS
Volume 15, Issue 1, Pages -Publisher
SHANGHAI JIAO TONG UNIV PRESS
DOI: 10.1007/s40820-023-01080-y
Keywords
Metal-organic frameworks; Atomically dispersed catalyst; Hydrogen bond; Overall water splitting
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In this study, asymmetric structural evolution and a dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst were reported. Nitrogen-doped porous carbons, functionalized by atomically dispersed Co-Ni dual-metal sites with an unprecedented N8V4 structure, were obtained through the pyrolysis of Co/Ni-doped MAF-4/ZIF-8. This electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C-OH groups, which can form reversible hydrogen bonds with the oxygen evolution reaction intermediates, breaking the conventional scaling relationship.
The real structure and in situ evolution of catalysts under working conditions are of paramount importance, especially for bifunctional electrocatalysis. Here, we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst. Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co-Ni dual-metal sites with an unprecedented N8V4 structure, which can serve as an efficient bifunctional electrocatalyst for overall water splitting. More importantly, the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C-OH groups. Density functional theory calculations suggested that the flexible C-OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates, giving a bridge between elementary reactions to break the conventional scaling relationship.
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