Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction

An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO(2)RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO(2)RR performance of two-dimensional transition metal carbide class of materials. Our results indicate a maximum methane (CH4) current density of -421.63 mA/cm(2) and a CH4 faradic efficiency of 82.7% +/- 2% for di-tungsten carbide (W2C) nanoflakes in a hybrid electrolyte of 3 M potassium hydroxide and 2 M choline-chloride. Powered by a triple junction photovoltaic cell, we demonstrate a flow electrolyzer that uses humidified CO2 to produce CH4 in a 700-h process under one sun illumination with a CO2RR energy efficiency of about 62.3% and a solar-to-fuel efficiency of 20.7%. Density functional theory calculations reveal that dissociation of water, chemisorption of CO2 and cleavage of the C-O bond-the most energy consuming elementary steps in other catalysts such as copper-become nearly spontaneous at the W2C surface. This results in instantaneous formation of adsorbed CO-an important reaction intermediate-and an unlimited source of protons near the tungsten surface sites that are the main reasons for the observed superior activity, selectivity, and small potential. It is of high interests to develop new catalysts for selective CO2 electroreduction. Here the authors investigate two-dimensional transition metal carbides for CO2 to methane conversion with superior activity, selectivity and low overpotentials.

Automated summary

The study investigates the performance of two-dimensional transition metal carbides in electrochemical CO2 reduction to methane, demonstrating superior activity, selectivity, and low overpotentials. The findings suggest potential for developing new catalysts for selective CO2 electroreduction processes.