Symbiotically Reinforced Bimetallic Photocatalysis in Conjugated Metal−Organic Framework Nanosheets

Abstract Compared to monometallic counterparts, bimetallic two‐dimensional conjugated metal‐organic framework (2D c‐MOF) nanosheets possess preferable metal tunability and synergistic effect for performance optimization, yet rarely developed in photocatalytic hydrogen evolution to date. In this study, a feasible post‐synthetic strategy of second metal installation (SMI) is proposed and applied to construct a crystalline bimetallic 2D c‐MOF nanosheet, HTHATN‐Ni‐Pt‐NS. HTHATN‐Ni‐Pt‐NS exhibits high electrical conductivity and efficient hydrogen evolution with the rate of 47.2 mmol g⁻¹ h⁻¹, which is 13.5‐fold higher than that of pristine HTHATN‐Ni‐NS without Pt^II decoration under visible light irradiation. Experimental and theoretical analysis reveal that introduction of low amount of Pt^II provides catalytically active metal sites and optimizes the ΔG_H* value of Ni^II centers, thus resulting in the enhanced performance of proton reduction. This study represents the first example of symbiotic bimetallic centers in MOF nanosheets highlighting SMI strategy as an efficient approach to construct photocatalysts.