The past few decades have witnessed the rapid growth of the atmospheric CO2 component. Electrochemical CO2 reduction (ECR) is expected to be a burgeoning strategy for excess CO2 treatment as well as energy conversion. Nevertheless, the low conversion efficiency and reaction selectivity towards a single component product limits the industrial application of ECR technology. Thus, electrocatalysts are critically important, and the precise design of electrocatalysts can not only improve the reaction efficiency, but also adjust the product selectivity and distribution. As potential heterogeneous catalysts for ECR application, crystalline porous materials (CPMs) possess periodic framework structures, and thus shows highly clear and tunable active sites. Herein, we developed two CPMs as electrocatalysts, namely CuII4-MFU-4l and CuBtz, whose secondary coordination spheres were designed to introduce hydrogen bond donors and proton relays to the ECR system, respectively, resulting in enhanced ECR performances for yielding hydrocarbons and carbon oxygenates. The results demonstrated that rational design of the secondary coordination sphere of the active sites can significantly influence the binding ability between the metal sites and intermediates, hence regulate the ECR performances.

Secondary coordination sphere design of porous copper-azolate catalysts for electrochemical CO2 reduction

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