Abstract
Copper-based materials are promising electrocatalysts for CO(2) reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO(2) reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO(2) reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C(2+) products. We achieve a 40-fold enhancement in the ratio of C(2+) to the competing CH(4) compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO(2) reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier-a rate-limiting step in CO(2) reduction to multi-carbon products.