Two-Dimensional Morphology Enhances Light-Driven H₂ Generation Efficiency in CdS Nanoplatelet-Pt Heterostructures

Light-driven H₂ generation using semiconductor nanocrystal heterostructures has attracted intense recent interest because of the ability to rationally improve their performance by tailoring their size, composition, and morphology. In zero- and one-dimensional nanomaterials, the lifetime of the photoinduced charge-separated state is still too short for H₂ evolution reaction, limiting the solar-to-H₂ conversion efficiency. Here we report that using two-dimensional (2D) CdS nanoplatelet (NPL)-Pt heterostructures, H₂ generation internal quantum efficiency (IQE) can exceed 40% at pH 8.8-13 and approach unity at pH 14.7. The near unity IQE at pH 14.7 is similar to those reported for 1D nanorods and can be attributed to the irreversible hole removal by OH^-. At pH < 13, the IQE of 2D NPL-Pt is significantly higher than those in 1D nanorods. Detailed time-resolved spectroscopic studies and modeling of the elementary charge separation and recombination processes show that, compared to 1D nanorods, 2D morphology extends charge-separated state lifetime and may play a dominant role in enhancing the H₂ generation efficiency. This work provides a new approach for designing nanostructures for efficient light-driven H₂ generation.