Abstract
More sustainable solutions are needed to produce chemicals and fuels, mainly to face rising demands and mitigate climate change. Light, as a reagent, has emerged as a route to activate small molecules, e.g., H2O, CO2, N2, and make complex chemicals in a process called photocatalysis. Several photosystems have been proposed, with plasmonic technology emerging as one the most promising technologies due to its high optical absorption and hot-carrier formation. However, the lifetime of hot carriers is unsuitable for direct use; therefore, they are normally coupled with suitable charge-accepting materials, such as semiconductors. Herein, a system is reported consisting of Au supported in p-Cu2O. The combination of p-Cu2O intrinsic photoactivity with the plasmonic properties of Au extended the system’s optical absorption range, increasing photocatalytic efficiency. More importantly, the system enabled us to study the underlying processes responsible for hot-hole transfer to p-Cu2O. Based on photocatalytic studies, it was concluded that most of the holes involved in aniline photo-oxidation come from hot-carrier injections, not from the PIRET process.
Highlights
The steadily rising consumption of energy and consumer products is becoming increasingly challenging
A step forward from power generation is the photocatalytic production of chemicals and fuels, known as photoredox catalysis and artificial photosynthesis, respectively
This study reports on charge transfer from a Au plasmon to a p-Cu2O semiconductor, the mechanisms and benefits of photocatalytic oxidation reactions
Summary
The steadily rising consumption of energy and consumer products is becoming increasingly challenging. The formation of the hot carriers on Au plasmons occurs via several processes, namely electronelectron (e-e) scattering, electron-phonon (e-ph) scattering and Landau damping [5] The latter dominates on small NPs and is based on the interaction of the collective oscillation with the natural boundaries of the NP. This indicates that the formally collective oscillation of the plasmon starts decaying and creates the separation of electron-hole pairs, which are highly non-thermalised and do not follow the Fermi–Dirac distribution Those carriers start to decay through e-e collisions, which results in the thermal equilibrium following the. The transfer of energy into the adjacent semiconductor forms electron-hole pairs in the material through relaxation of the surface plasmons’ resonance This mechanistical difference, the coupling of the electromagnetic field with the semiconductor, rather than direct injection of carriers or tunnelling, explains the rather low-distance. Even though this material shows good photocatalytic behaviour, its photo response and stability are challenges that need to be resolved, making it an ideal candidate for this study
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