Hybrid Oxide Coatings Generate Stable Cu Catalysts for CO2 Electroreduction

Abstract Hybrid organic/inorganic materials have contributed to solve many challenges in different areas of science. 1–5 One of the biggest challenges for a more sustainable society is to have active and stable catalysts which enable the transition from fossil to renewable feedstocks, reduce energy consumption, and minimize the environmental footprint. Herein, we synthesize novel hybrid materials where an amorphous oxide coating with embedded organic ligands surrounds metallic nanocrystals. We demonstrate that the hybrid coating is a powerful mean to create electrocatalysts stable against structural reconstruction during the CO 2 electroreduction. These electrocatalysts consists of copper nanocrystals encapsulated in a hybrid organic/inorganic alumina shell. This shell locks a fraction of the copper surface into a reduction resistant Cu 2+ state, which inhibits those redox processes responsible for the structural reconstruction of copper. The electrocatalyst activity is preserved, which would not be possible with a conventional dense alumina coating. Varying the shell thickness and the coating morphology yields fundamental insights into the stabilization mechanism and emphasizes the importance of the Lewis acidity of the shell in relation to the retention of catalyst structure. The synthetic tunability of the chemistry developed herein opens new avenues for the design of stable electrocatalysts and beyond.