2026-04-13T05:26:47Zhttps://recercat.cat/oai/request

oai:recercat.cat:2072/4505312024-12-20T22:42:47Zcom_2072_300912com_2072_4427col_2072_301309

00925njm 22002777a 4500 dc Dattila, Federico author García-Muelas, Rodrigo author López, Núria author 2020-09-22 Copper catalysts are unique in CO2 reduction as they allow the formation of C2+ products. Depending on the catalysts’ synthesis, product distribution varies significantly: while Cu nanoparticles produce mainly methane and hydrogen, oxide-derived copper leads to ethylene and ethanol. Here, by means of ab initio molecular dynamics on oxygen-depleted models, we identified the ensembles controlling catalytic performance. Upon reconstruction and irrespective of the starting structure, recurrent patterns defined by their coordination and charges appear: metallic Cu0, polarized Cuδ+, and oxidic Cu+. These species combine to form 14 ensembles. Among them, 4-(6-)coordinated Cu adatoms and Cu3δ+O3 are responsible for tethering CO2, while metastable near-surface oxygens in fcc-(111) or (100)-like Cu domains promote C–C bond formation via glyoxylate species, thus triggering selective C2+ production at low onset potentials. Our work provides guidelines for modeling complex structural rearrangements under CO2 reduction conditions and devising new synthetic protocols toward an enhanced catalytic performance. http://hdl.handle.net/2072/450531 https://doi.org/10.1021/acsenergylett.0c01777 Active and Selective Ensembles in Oxide- Derived Copper Catalysts for CO2 Reduction