Chlorosome‐Like Molecular Aggregation of Chlorophyll Derivative on Ti3C2Tx MXene Nanosheets for Efficient Noble Metal‐Free Photocatalytic Hydrogen Evolution

Efficient photocatalytic hydrogen evolution reaction (HER) in the visible‐to‐near infrared region at a low cost remains a challenging issue. This work demonstrates the fabrication of organic‐inorganic composites by deposition of supramolecular aggregates of a chlorophyll derivative, namely, zinc methyl 3‐devinyl‐3‐hydroxymethyl‐pyropheophorbide a (Chl) on the surface of Ti3C2Tx MXene with 2D accordion‐like morphology. This composite material is employed as noble metal‐free catalyst in photocatalytic HER under the white light illumination, where Chl serves as a small molecule organic semiconductor component instead of ordinary inorganic and polymer organic semiconductors such as TiO2 and g‐C3N4, and Ti3C2Tx serves as a co‐catalyst. Different composition ratios of Chl/Ti3C2Tx are compared for their light‐harvesting ability, morphology, charge transfer efficiency, and photocatalytic performance. The best HER performance is found to be as high as 52 ± 5 µmol h−1 gcat−1 after optimization. Such a large HER activity is attributed to the efficient light harvesting followed by exciton transfer in Chl aggregates and the resultant charge separation at the interface of Chl/Ti3C2Tx.