Synergistic Effect of Plasmonic Gold Nanoparticles Decorated Carbon Nanotubes in Quantum Dots/TiO2 for Optoelectronic Devices

Abstract 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.