Two-in-one redox photocatalysis: Cooperative hydrogen evolution and benzaldehyde production via 2D MoS2 cocatalyst-loaded hydrangea-like Zn3In2S6

By harnessing the power of MoS2 as a cocatalyst to enhance electron transfer and charge carrier separation, a groundbreaking two-in-one redox photocatalytic system was developed. This innovative system integrated 2D MoS2 nanosheets onto hydrangea-like Zn3In2S6 nanosheets, forming a 2D/3D heterostructure that established a stable and intimate interface. This unique architecture significantly improved cooperative photocatalytic performance, enabling the simultaneous production of hydrogen and benzaldehyde under light irradiation ≥420 nm. Notably, the system achieved remarkable yields of hydrogen (41.9 mmol g−1 h−1) and benzaldehyde (38.9 mmol g−1 h−1), surpassing the pristine Zn3In2S6 by 22.4 times. An impressive electron-hole pair utilization rate of approximately 93% was attained, underscoring the high efficiency of this two-in-one redox system. Additionally, the targeted 10 wt%-MoS2 loaded Zn3In2S6 (10MZ) nanohybrids at 400 nm obtained an apparent quantum yield (AQY) value of 17.66% without sacrificial agents or noble metals. The exceptional performance was attributed to improved charge carrier separation and reduced recombination, facilitated by cocatalyst integration and evidenced via photoluminescence, photoelectrochemical and Kelvin probe force microscopy measurements. This work highlighted the critical role of two-in-one redox-functioning heterojunctions in optimizing electron-hole pair utilization, offering a promising approach for sustainable energy production and organic synthesis. By demonstrating the potential for efficient, simultaneous generation of valuable chemicals and fuels, this research paves the way for the development of next-generation photocatalytic systems.