Authors: Naohiro Fujinuma, Natalie Page, Anna G Boddy, Joshua Rivkind, Lindsey Tomlinson, Erik P Hoy, Samuel E Lofland
Published: 2024-09-18
Source: Full article
AbstractThis study reports ambient electrosynthesis of dimethyl carbonate with a palladium–gold catalyst. Material screening identifies a region of intermediate‐catalyst binding energy that facilitates interfacial electron and proton transfers for selective carbonylation, achieving a distinct maximum of 92% faradaic efficiency to dimethyl carbonate. Structural and electrochemical analyses suggest that the alloying of palladium and gold effectively modulates the CO* binding energy to the catalytic surface, in accord with subsequent computational studies. With an extended heterogeneous–homogeneous catalytic environment with a halide redox mediator, a remarkable partial current density of 52 mA cm−2 is observed for dimethyl carbonate for 100 h of continuous operation.