Photocatalytic water-splitting into H2 in conventional procedures often requires sacrificial agents to consume unutilized holes to boost the reaction. Herein, we cast off the dependence on the addition of sacrificial agents and develop a dual-functional photocatalyst CdS/Ni@NC for coupling H2 evolution with value-added benzyl alcohol (BA) oxidation in anaerobic aqueous solution, wherein CdS/Ni@NC was synthesized by in-situ anchoring of CdS nanoparticles (NPs) onto NMOF-Ni ultrathin nanosheets-derived nitrogen-doped wrinkled graphitic carbon layers encapsulated metallic Ni NPs (Ni@NC). The optimized photocatalyst CdS/Ni@NC(5) achieves a high visible-light-driven H2 evolution rate of 1881 μmol·g−1·h−1 and a benzaldehyde (BAD) yield of 3254.2 μmol·g−1·h−1, with nearly 100 % selectivity over a 6 h period, which are 32.6 and 10.5 folds of that for CdS alone, respectively. Further in-depth experimental characterizations reveal that the hierarchical Ni@NC serves as an ideal support to enable high dispersion of CdS NPs, thus improving light absorption and facilitating full contact with reactants. Besides, the widely distributed Ni NPs, effectively shielded by nitrogen-doped wrinkled graphitic carbon layers, can not only promote photogenerated charge transfer for enhanced H2 production but also facilitate the cleavage of the Cα–H bond in BA, contributing to achieving high aldehyde selectivity. This study, integrating carbonized ultrathin nanosheets NMOF-Ni with CdS to synergistically enhance surface redox reactions, holds significant promise for advancing the development of high-performance photocatalysts for integrated production of solar hydrogen and value-added solar chemicals.
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