Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt1–Pdn–(Ni,Co)(OH)x
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DOI:
10.1021/jacs.4c12665
Publication Date:
2025-01-14T04:23:57Z
AUTHORS (16)
ABSTRACT
Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H2 generation, avoiding its costly and risky distribution issues, but this "ME-to-H2" electric conversion suffers from high voltage (energy consumption) competitive oxygen evolution reaction. Herein, we demonstrate that synergistic cofunctional Pt1Pdn/(Ni,Co)(OH)x catalyst with Pt single atoms (Pt1) Pd nanoclusters (Pdn) anchored on OH-vacancy(VOH)-rich (Ni,Co)(OH)x nanoparticles create triadic active sites, allowing methanol-enhanced low-voltage generation. For MOR, OH* preferentially adsorbed Pdn then interacts the intermediates (such as *CHO or *CHOOH) favorably neighboring Pt1 assistance of bonding surface (Ni,Co)(OH)x. The enhanced selectivity *CHOOH pathway, instead *CO, sustains MOR activity to practically current density. HER, Pt1, Pdn, OH-vacancy sites an "acid–base" microenvironment facilitate water adsorption splitting, forming H* species *OH at vacancy, promote efficient asymmetric via Tafel mechanism. triadic-site synergy opens new avenues design synthesis highly stable catalysts "on-site-on-demand" production, here facilitated by methanol.
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