Restructuring of Cu2O to Cu2O@Cu-Metal-Organic Framework for the Selective Electrochemical Reduction of CO2.

Electrochemical reduction of carbon dioxide to hydrocarbons, driven by renewable power sources, is a fascinating and clean way to remedy greenhouse gas emission as a result of over-dependence on fossil fuels and produce value-added fine chemicals. The Cu-based catalysts feature unique superiorities, nevertheless, achieving high hydrocarbons selectivity is still inhibited and remains great challenges. In this study, we report on a tailor-made multifunction-coupled Cu-metal-organic frameworks (Cu-MOF) electrocatalyst by time-resolved controllable restruction from Cu2O to Cu2O@Cu-MOF. The restructured electrocatalyst features a time-responsive behavior, and is equipped with high specific surface area for strong adsorption capacity of CO2 and abundant active sites for high electrocatalysis activity based on the as-produced MOF on the surface of Cu2O, as well as accelerated charge transfer derived from Cu2O core in comparison with Cu-MOF. These intriguing characteristics finally lead to a prominent performance towards hydrocarbons, with a high hydrocarbon Faradaic efficiency (FE) of 79.4%, particularly, the CH4 FE as high as 63.2% (at -1.71 V). This work presents a novel & efficient strategy to configure the MOF-based materials in energy and catalysis fields, with a focus on big surface area, high adsorption ability as well as much more exposed active sites.