Solar-driven Plasmonic Catalysis

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This project addresses the major challenges associated with precise manipulation of interfaces for atom/charge transfer in catalysis and energy conversion, where high priority goals include visible-light plasmonic catalysis and high selectivity in e.g. CO2 conversion to MeOH. A range of new binary and ternary catalytic materials prepared from polyoxometalate-stabilised metal nanoparticles (POM@MNP) and polymeric carbon nitride (PCN) will build on previous work of the remarkable synergy in POM@Ru thermal, photo- and electro-catalysis.Underpinning the project is the synthesis of heterometal-substituted polyoxometalates (POMs) as tunable, single-atom, molecular metal oxide catalysts. These will be used to prepare POM@AuNP and POM@CuNP binary systems in order to precisely locate reactive metal sites (e.g. Ti, Zr, V, Cr, Mn, Fe, Co, Ni, Zn) at the metal-oxide/metal interface. Ternary materials obtained by supporting these POM@MNP on PCN will provide additional functionality derived from the photo- and electro-active PCN. POM/MNP interfaces will be analysed by high resolution electron microscopy and the distribution of NPs on PCN will be determined using electron tomography. Thermal and photocatalytic experiments will be studied by time-resolved spectroscopy and supplemented by studies of ultrafast charge extraction dynamics. Charge transfer at POM/MNP, POM/PCN, MNP/PCN and POM@MNP/PCN interfaces will be key to exploiting the unique photo physics of the new binary and ternary materials for visible light plasmonic catalysis. Fine tuning the properties of these multicomponent catalysts will require a deeper understanding of these systems, and this will be aided by DFT computational modelling studies.Precise manipulation of interfaces at the atomic level will improve activity and selectivity and enable catalyst design for new processes, providing better capabilities for CO2 utilisation and related energy conversion and storage.