Dual-Hole Excitons Activated Photoelectrolysis in Neutral Solution

II–VI semiconductors exhibit unique behaviors that can generate dual-holes (“heavy and light”), but the application in photocatalysis is still missing. Herein, an empirical utilization of light/heavy holes in a hybrid metal cluster-2D semiconductor nanoplatelets is reported. This hybrid material can boost the hole-transfer at the surface and suppress the recombination. Different roles are enacted by light-holes and heavy-holes, in which the light-holes with higher energy and mobility can facilitate the slow kinetics of water oxidation and further reduce the onset voltage, while the massive heavy-holes can increase the resulting photocurrent by about five times, achieving a photocurrent of 2 mA cm⁻² at 1.23 V versus RHE under AM 1.5 G illumination in nonsacrificial neutral solution. These strategies can be the solutions for photoelectrolysis and be beneficial for sustainable development in solar conversion.