Here, a facile approach to enhance the performance of solar‐driven photoelectrochemical (PEC) water splitting is described by means of the synergistic effects of a hybrid network of plasmonic Au nanoparticles (NPs) decorated on multiwalled carbon nanotubes (CNTs). The device based on TiO2–Au:CNTs hybrid network sensitized with colloidal CdSe/(CdSexS1?x)5/(CdS)1 core/alloyed shell quantum dots (QDs) yields a saturated photocurrent density of 16.10?± 0.10?mA cm?2 [at 1.0?V vs reversible hydrogen electrode (RHE)] under 1 sun illumination (AM 1.5G, 100?mW cm?2), which is ≈26% higher than the control device. The in‐depth mechanism behind this significant improvement is revealed through a combined experimental and theoretical analysis for QDs/TiO2–Au:CNTs hybrid network and demonstrates the multifaceted impact of plasmonic Au NPs and CNTs: i) hot‐electron injection from Au NPs into CNTs and TiO2; ii) near‐field enhancement of the QDs absorption and carrier generation/separation processes by the plasmonic Au NPs; iii) enhanced photoinjected electron transport due to the highly directional pathways offered by CNTs. These results provide fundamental insights on the properties of QDs/TiO2–Au:CNTs hybrid network, and highlights the possibility to improve the performance of other solar technologies.
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