Regulating the Transfer of Photogenerated Carriers on CdS Nanorods by Conductive Bimetallic CuNi‐MOF for Highly Selective Photocatalytic Benzylamine Oxidation Integrated with H ₂ Production

ABSTRACT The simultaneous utilization of photoelectrons and holes to achieve the coupling of photocatalytic hydrogen evolution with the selective oxidation of organic substances holds significant importance. Yet, this strategy is often constrained by the inadequate charge separation efficiency of photocatalysts and the scarcity of sufficient catalytic active sites. Herein, a conductive bimetallic metal‐organic framework (MOF), Cu x Ni 1‐x ‐HHTP, was strategically integrated onto the surface of CdS nanorods, yielding a visible‐light‐responsive CdS@Cu x Ni 1‐x ‐HHTP core‐shell inorganic‐organic hybrid, which demonstrated exceptional performance and remarkable product selectivity in the photocatalytic dehydrogenative coupling of benzylamine. The incorporation of Cu x Ni 1‐x ‐HHTP endows the photocatalytic system with a plethora of accessible reactive sites. Moreover, the ultrafast spectroscopy research unveils that Cu 0.5 Ni 0.5 ‐HHTP exhibits robust capability for efficient photogenerated electron extraction, thereby effectively facilitating the spatial separation of photogenerated carriers during the photocatalytic process. Notably, when the CdS/Cu 0.5 Ni 0.5 ‐HHTP molar ratio was 1:2 in photocatalysts, the catalyst denoted as CdS@Cu 0.5 Ni 0.5 ‐HHTP‐2 demonstrated a remarkable hydrogen evolution rate of 29.79 mmol g − 1 h − 1 , accompanied by a benzylamine conversion rate of 58.39%, while maintaining high stability. This study introduces a strategy for integrating conductive bimetallic metal‐organic frameworks with inorganic semiconductors, enabling ultrafast photocarrier transfer and significantly enhancing photocatalytic efficiency.