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Surface engineering of palladium nanocatalysts via galvanically doping Au atom to modulate electrosynthesis of dimethyl carbonate
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DOI：10.1016/j.jelechem.2026.120062.png)
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Abstract
En 中文
Electrochemical synthesis of dimethyl carbonate (DMC) from carbon dioxide (CO2) and methanol (CH3OH) provides a greener and more sustainable route than the conventional industrial method of oxidative carbonylation of methanol. Palladium (Pd) nanocatalysts have shown high efficacy in the cathodic coupling of CO2 and CH3OH to form DMC in a bromide-containing electrolyte. In this study, we report a strategy to enhance the DMC performance of Pd nanocatalysts via surface modification with Au atoms using the galvanic replacement reaction. Experimental results demonstrate that the DMC performance can be significantly improved by controlling the content and dispersion of Au atoms during galvanic replacement. The optimized catalyst achieves a Faradaic efficiency for DMC (FEDMC) of 56.1% at a current density of 20 mA/cm2, substantially surpassing 29.3% of pristine Pd nanocatalysts under identical conditions. Through XPS, CV, and HR-TEM analyses, it reveals that the enhanced DMC performance of the Pd nanocatalysts modified by galvanic replacement of Au atoms originates from an electron-modulation effect induced by the Au atoms, which is governed by both their content and dispersion. Notably, the optimized catalyst integrates two tandem catalytic zones that operate in concert, significantly accelerating the DMC formation.
Keywords:
Dimethyl carbonate
Electrochemical synthesis
Palladium nanocatalysts
Au-atom modulation
Galvanic replacement
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