Recent Progress in Two-Dimensional Materials for Electrocatalytic CO2 Reduction

Electrocatalytic CO2 reduction (ECR) is an attractive approach to convert atmospheric CO2 to value-added chemicals and fuels. However, this process is still hindered by sluggish CO2 reaction kinetics and the lack of efficient electrocatalysts. Therefore, new strategies for electrocatalyst design should be developed to solve these problems. Two-dimensional (2D) materials possess great potential in ECR because of their unique electronic and structural properties, excellent electrical conductivity, high atomic utilization and high specific surface area. In this review, we summarize the recent progress on 2D electrocatalysts applied in ECR. We first give a brief description of ECR fundamentals and then discuss in detail the development of different types of 2D electrocatalysts for ECR, including metal, graphene-based materials, transition metal dichalcogenides (TMDs), metal-organic frameworks (MOFs), metal oxide nanosheets and 2D materials incorporated with single atoms as single-atom catalysts (SACs). Metals, such as Ag, Cu, Au, Pt and Pd, graphene-based materials, metal-doped nitric carbide, TMDs and MOFs can mostly only produce CO with a Faradic efficiencies (FE) of 80~90%. Particularly, SACs can exhibit FEs of CO higher than 90%. Metal oxides and graphene-based materials can produce HCOOH, but the FEs are generally lower than that of CO. Only Cu-based materials can produce high carbon products such as C2H4 but they have low product selectivity. It was proposed that the design and synthesis of novel 2D materials for ECR should be based on thorough understanding of the reaction mechanism through combined theoretical prediction with experimental study, especially in situ characterization techniques. The gap between laboratory synthesis and large-scale production of 2D materials also needs to be closed for commercial applications.