One-Dimensional CdS/Carbon/Au Plasmonic Nanoarray Photoanodes via In Situ Reduction-Graphitization Approach toward Efficient Solar Hydrogen Evolution

Photoelectrochemical (PEC) hydrogen evolution has been acknowledged as a promising "green" technique to convert solar energy into clean chemical fuel. Photoanodes play a key role in determining the performance of PEC systems, spurring numerous efforts to develop advanced materials as well as structures to improve the photoconversion efficiency. In this work, we report the rational design of a plasmonic hierarchical nanorod array, composed of oriented one-dimensional (1D) CdS nanorods decorated with a uniformly wrapped graphite-like carbon (CPDA) layer and Au nanoparticles (Au NPs), as highly efficient photoanode materials. An interfacial in situ reduction-graphitization method has been conducted to prepare the CdS/CPDA/Au nanoarchitecture, where polydopamine (PDA) coating was used as a C source and a reductant. The CdS/CPDA/Au nanoarray photoanode demonstrates superior photoconversion efficiency with a photocurrent density of 8.74 mA/cm2 and an IPCE value (480 nm) of 30.2% (at 1.23 V vs RHE), under simulated sunlight irradiation, which are 12.7 and 13.5 times higher than pristine CdS. The significant enhancement of PEC performance is mainly benefited from the increase of the entire quantum yield and efficiency due to the formation of a Schottky rectifier, localized surface plasmon resonance (LSPR)-enhanced light absorption, and promoted hot-electron injection from interlayered graphene-like carbon. More importantly, thanks to the inhibited charge carrier recombination process and transferred oxidation reaction sites, the fabricated CdS/CPDA/Au photoelectrode exhibits lengthened electron lifetimes and better photostability, illustrating its wonderful potential for future PEC application.