Authors
Xiaowen Gu, Yu Liang, Pengcheng Zhao, Xinye Zhang, Wei Liu, Chenyu Cui, Zihao Xing, Shangqian Zhu, Jinfa Chang
Published in
Angewandte Chemie (International ed. in English). Oct 24, 2026. Epub Oct 24, 2026.
Abstract
Direct ethanol fuel cells (DEFCs) are hampered by sluggish C─C bond cleavage and CO poisoning during ethanol electrooxidation on Pd catalysts. Selective oxidation to acetate through the C2 pathway circumvents CO formation, yet achieving near-exclusive C2 selectivity remains challenging. Herein, we report a nitrogen-doping-induced expansion strategy that converts bulk 2H-MoS2 into a metastable 1T-rich MoS2-x support (NTMSx) with enlarged interlayer spacing and abundant sulfur vacancies. Conductive 1T domains preferentially anchor Pd nanoparticles, creating an "island-sea" architecture that fosters pronounced electronic metal-support interaction (EMSI). Electron transfer from NTMSx to Pd generates electron-rich Pd sites that weaken CO adsorption, while sulfur vacancies enhance hydroxyl adsorption. These synergistic effects steer ethanol electrooxidation toward the C2-4e pathway and suppress CO formation. DFT calculations confirm favorable energetics for the C2 pathway on Pd/NTMSx. The catalyst delivers a high current density and 95.7% Faradaic efficiency for acetate of high added value, with no detectable CO intermediates and outstanding durability. In DEFCs, it achieves a maximum power density of 0.68 W cm-2 and operates stably for over 500 h. This work establishes confined interfacial anchoring on phase-engineered metal dichalcogenides as a rational design principle for achieving high pathway selectivity in multielectron electrocatalysis.
PMID:
42920342
Bibliographic data and abstract were imported from PubMed on 24 Oct 2026.
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