Hot Electrons Induced by Localized Surface Plasmon Resonance in Ag/g-C(3)N(4) Schottky Junction for Photothermal Catalytic CO(2) Reduction

利用Ag/gC₃N₄肖特基结中局域表面等离子体共振诱导的热电子进行光热催化CO₂还原

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Abstract

Converting carbon dioxide (CO(2)) into high-value-added chemicals using solar energy is a promising approach to reducing carbon dioxide emissions; however, single photocatalysts suffer from quick the recombination of photogenerated electron-hole pairs and poor photoredox ability. Herein, silver (Ag) nanoparticles featuring with localized surface plasmon resonance (LSPR) are combined with g-C(3)N(4) to form a Schottky junction for photothermal catalytic CO(2) reduction. The Ag/g-C(3)N(4) exhibits higher photocatalytic CO(2) reduction activity under UV-vis light; the CH(4) and CO evolution rates are 10.44 and 88.79 µmol·h(-1)·g(-1), respectively. Enhanced photocatalytic CO(2) reduction performances are attributed to efficient hot electron transfer in the Ag/g-C(3)N(4) Schottky junction. LSPR-induced hot electrons from Ag nanoparticles improve the local reaction temperature and promote the separation and transfer of photogenerated electron-hole pairs. The charge carrier transfer route was investigated by in situ irradiated X-ray photoelectron spectroscopy (XPS). The three-dimensional finite-difference time-domain (3D-FDTD) method verified the strong electromagnetic field at the interface between Ag and g-C(3)N(4). The photothermal catalytic CO(2) reduction pathway of Ag/g-C(3)N(4) was investigated using in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS). This study examines hot electron transfer in the Ag/g-C(3)N(4) Schottky junction and provides a feasible way to design a plasmonic metal/polymer semiconductor Schottky junction for photothermal catalytic CO(2) reduction.

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