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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 40: Focus Session: Novel Approaches to Surface Plasmon Generated Charges and Heat for Photocatalysis II (joint session O/CPP)

CPP 40.5: Vortrag

Donnerstag, 21. März 2024, 11:45–12:00, MA 141

Atomic scale plasmonic catalysis — •Yicui Kang and Emiliano Cortés — Nanoinstitute Munich, LMU Muenchen, Germany

In the realm of plasmonic catalytic systems, much attention has been devoted to the plasmon-derived mechanisms1, yet the influence of nanoparticles (NPs) crystal facets has been sparsely investigated. In this work2, we study the plasmon-assisted electrocatalytic CO2RR using three different shapes of plasmonic Au nanocube (NC), rhombic dodecahedron (RD) and octahedron (OC) - with different exposed facets: {100}, {110} and {111}, respectively. Upon plasmon excitation, Au OCs and NCs exhibited nearly a doubling in the FE(CO) compared to non-illuminated response. In contrast, RDs showed nearly the same performance in dark or light conditions. Electromagnetic modeling showed higher electric field (EF) enhancement on OCs and NCs on the edges and corners, which in some degree contributes to the enhancement of CO production3. Large-scale atomistic simulations of the electronic structure revealed higher hot carrier abundance on OCs and NCs compared to RDs. Abundant hot carriers on edges facilitate molecular activation, leading to enhanced selectivity and activity. This observation is further supported by plasmon-assisted HER experiments. Our findings highlight the dominance of low coordinated sites over facets in plasmonic catalytic processes, providing valuable insights for designing more efficient catalysts for energy conversion and carbon neutralization. Ref1. ACS Energy Letters 7.2 (2022): 778-815 Ref2. Crystal Facet Effect in Plasmonic Catalysis. Revision (2023) Ref3. Angew.Chem.Int.Ed.61.44 (2022): e202212640

Keywords: plasmonic catalysis; facet effect; carbon dioxide reduction; hot carriers; hot carriers, low-coordinated sites