Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt1–Pdn–(Ni,Co)(OH)x

• DOI: 10.1021/jacs.4c12665
• Publication Date: 2025-01-14T04:23:57Z
• Authors: An Pei; Ruikuan Xie; Lihua Zhu; Fengshun Wu; Zinan Huang; Yongyu Pang; Yu-Chung Chang; Guoliang Chai; Chih-Wen Pao; Qingsheng Gao; Congxiao Shang; Guang Li; Jinyu Ye; Huaze Zhu; Zhiqing Yang; Zhengxiao Guo
• Keywords: Cell voltage

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.