Hydrogen Production on a Hybrid Photocatalytic System Composed of Ultrathin CdS Nanosheets and a Molecular Nickel Complex

The production of clean and renewable hydrogen through water splitting by using solar energy has received much attention due to the increasing global energy demand. We report an economic and artificial photosynthetic system free of noble metals, consisting of ultrathin CdS nanosheets as a photosensitizer and nickel‐based complex as a molecular catalyst. Emission quenching and flash photolysis studies reveal that this hybrid system allows for effective electron transfer from the excited CdS nanosheets to the nickel‐based complex to generate reduced intermediate species for efficient hydrogen evolution. Notably, the unique morphological and structural features of the ultrathin CdS nanosheets contribute to the highly efficient photocatalytic performance. As a consequence, the resulting system shows exceptional activity and stability for photocatalytic hydrogen evolution in aqueous solution with a turnover number (TON) of about 28 000 versus catalyst and a lifetime of over 90 h under visible light irradiation.