Tandem atomically dispersed metal catalysts to promote flow-line electrocatalytic CO2RR

Atomically dispersed metal catalysts (ADMCs), featuring attractive electronic/geometric configuration and excellent catalytic performance, have emerged a novel class of heterogenous catalysts. However, the linear limitations of ADMCs for complex catalytic reactions, such as the electrocatalytic carbon dioxide reduction reaction (ECO2RR) for C2+ products, constrain the further improvement of the catalytic performance. Hence, we proposed a tandem ADMCs (T-ADMCs) model for the first time, which is inspired by the tandem catalysis observed in the multienzyme catalytic cycles of biocatalytic systems. The coupled multistep reactions occurring at the adjacent sites in T-ADMCs may promote flow-line ECO2RR and optimize the overall catalytic performance. This perspective overviews the recent research advances on T-ADMCs for ECO2RR and highlights the advancing orientation of T-ADMCs. Reaction mechanisms based on CO, formic acid, and acetaldehyde intermediates on T-ADMCs are proposed. The activity-promoting effects of tandem catalyst are elucidated, including the regulation of electronic structure via long-range interaction, breaking of linear scaling relationship, and modulation of local microenvironment through intralayer or interlayer diffusion. The challenges, opportunities, and further development of T-ADMCs and reaction mechanisms under realistic electrocatalytic environment are proposed. This work sheds new light on the design of high-performance T-ADMCs.