Nature-inspired design of molybdenum-selenium dual-single-atom electrocatalysts for CO2 reduction

Sun, Yu, Fang, Zhuang, Tan, Wu, Zeng, Zhuang, Pan, Chen (2022) Nature-inspired design of molybdenum-selenium dual-single-atom electrocatalysts for CO2 reduction. Adv Mater () e2206478

http://dx.doi.org/10.1002/adma.202206478

Electrochemical CO2 reduction (ECR) is becoming an increasingly important technology for achieving carbon neutrality. Inspired by the structure of naturally occurring Mo-dependent enzymes capable of activating CO2 , we demonstrate here a heteronuclear Mo-Se dual-single-atom electrocatalyst (MoSA-SeSA) for ECR into CO with a Faradaic efficiency of above 90% over a broad potential window from -0.4 to -1.0 V versus reversible hydrogen electrode. Both operando characterization and theoretical simulation results verify that MoSA acts as central atoms that directly interact with ECR feedstock and intermediates, whereas the SeSA adjacent to MoSA modulates the electronic structure of MoSA through the long-range electron delocalization for inhibiting MoSA poisoning caused by strong CO adsorption. In addition, the SeSAs far from MoSA help suppress the competing hydrogen evolution side reaction and accelerate the CO2 transport by repelling H2 O. Our work provides new insight into the precise regulation and in-depth understanding of multisite synergistic catalysis at the atomic scale. This article is protected by copyright. All rights reserved.This article is protected by copyright. All rights reserved.