Publication date: 15th December 2025
Dimethyl carbonate (DMC) is a widely used and versatile organic platform chemical with growing applications in energy storage, polymer synthesis, and sustainable chemical manufacturing [1]. Industrial DMC production primarily proceeds via methanol oxycarbonylation and methylnitrite carbonylation, which rely on high-pressure conditions and complex catalytic cycles [2]. In contrast, the direct electrochemical carbonylation of methanol presents an electrified, low-temperature alternative that aligns well with sustainable energy conversion goals towards high-value compounds. Nevertheless, this approach remains limited by challenges in selectivity and catalyst stability due to a lack of established mechanistic understanding in non-aqueous environments.
This study aims to address this knowledge gap by employing a combination of in situ spectroscopic, microscopic, and computational methods. Using in situ scanning tunneling microscopy (STM) and in situ Raman spectroscopy on well-defined single-crystal electrodes, we directly probe the interface and monitor product evolution under controlled electrochemical conditions. By systematically studying product distribution as a function of surface facet orientation and catalyst composition, we aim to identify key structure–reactivity relationships that govern selective methanol carbonylation. Integrated density functional theory (DFT) calculations provide atomic-scale insights into the energetics and reaction pathways underlying DMC formation.
By linking model surfaces and their respective product distributions, we aim to establish a mechanistic framework allowing for the rational design of tailored nanoparticle catalysts for direct electrochemical carbonylation of alcohols.
Pioneer Center for Accelerating P2X Materials Discovery (CAPeX), DNRF grant number P3
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