One‐Step Dual‐Ligand Co‐Embedding for MIL‐125‐Based Photocatalysts Toward Efficient Hydrogen Evolution

In photocatalysis, metal organic frameworks (MOFs) offer vast prospects owing to their exceptional structural and functional properties. Titanium‐based MOFs, in particular, have garnered attention for their stability and tunable band structure. However, conventional synthesis strategies for Ti‐MOFs face limitations, often requiring multi‐step reactions, tunable incorporation, or energy‐intensive processes. This study proposes a one‐step co‐embedding strategy for ligands, verified by direct experimental evidence. By adjusting the ratio of H 2 BDC and H 2 BDC‐NH 2 ligands, functionalized MOFs (NM (X)) were successfully synthesized in a single step. The FTIR peak at 1340 cm −1 confirmed the successful intergration of NH 2 ‐H 2 BDC ligands, validating the one‐step protocol. Photoelectrochemical measurements showed that the dual‐ligand materials exhibited enhanced visible‐light absorption, higher photocurrent density, and smaller EIS arc radius, indicating efficient charge separation. Under simulated solar irradiation, all NM (X) samples showed improved photocatalytic hydrogen evolution. Our work demonstrates that the one‐step dual‐ligand co‐embedding strategy is a feasible and controllable method for preparing Ti‐based MOFs. The resulting materials achieve significantly enhanced photocatalytic performance through rational dual‐ligand co‐embedding and ratio regulation. This strategy opens a novel and efficient avenue for optimizing the preparation and application of high‐performance Ti‐based MOF photocatalysts.