Oxide-derived Cu exhibits high C2+ selectivity, which shows excellent application prospects in CO2 reduction reaction (CO2RR) research and future industrialization. However, given the chaos of the surface morphology, there are still controversies about the catalytic mechanism. Here, what we do is oxygen doping or building irregular surfaces to reflect the surface morphology more realistically. We find the overflow of oxygen atoms to the upper layer and the left vacancy which causes the fracture of C-C bond. Based on the pretreated surface, the possible reaction sites were searched comprehensively and a limited number of sites are conductive to the occurrence of CO-CO coupling. The subsequent decreased energy barriers of ethylene and ethanol products indicate that the key reaction step of C2 product is C-C coupling. As for the selectivity of C2 products, it depends more on the surface characteristics of the catalyst. Finally, the energy barriers in the constraint molecular dynamics are lower than molecular dynamics results, which suggests that the spill-over process on Cu surface plays a great role in promoting the reaction. Consequently , surface reconstruction comes from residual oxygen or other experimental conditions, which causes the chaos of surface morphology to increase the diversity of reaction sites and the probability of spill-over effects.

Ab initio molecular dynamics of Cu surface morphology for CO2 reduction to C2 products

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