Modulating the Active Sites of VS₂ by Mn Doping for Highly Selective CO₂ Electroreduction to Methanol in a Flow Cell

Abstract

Methanol is a valuable liquid C 1 product in CO 2 electroreduction (CO 2 ER); however, it is hard to achieve high selectivity and a large current density simultaneously. In this work, we construct Mn 2+ -doped VS 2 multilayer nanowafers applied in a flow cell to yield methanol as a single liquid product to tackle this challenge. Mn doping adjusts the electronic structure of VS 2 and concurrently introduces sulfur vacancies, forming a critical *CO B intermediate and facilitating its sequential hydrogenation to methanol. The optimal Mn 4.8% -VS 2 exhibits methanol Faradic efficiencies of more than 60% over a wide potential range of −0.4 to −0.8 V in a flow cell, of which the maximal value is 72.5 ± 1.1% at −0.6 V along with a partial current density of 74.3 ± 1.1 mA cm −2 . This work opens an avenue to rationally design catalysts for engineering C 1 intermediates toward CO 2 ER to a single liquid methanol in a flow cell.