Anchoring Sub‐Nanometer Pt Clusters on Crumpled Paper‐Like MXene Enables High Hydrogen Evolution Mass Activity

Platinum (Pt)‐based electrocatalysts are the benchmark catalysts for hydrogen evolution reaction (HER); however, they are limited by the scarcity and high price. Introducing an adequate substrate to disperse and anchor Pt‐based species is a feasible pathway to improve the utilization efficiency. Herein, a quick and continuous spray drying route is proposed to fabricate 3D crumpled Ti 3 C 2 T x MXene loaded with sub‐nanometer platinum clusters (Pt/MXene). The 3D crumpled structure inhibits the restacking of layered MXene nanosheets and guarantees the fully exposure of Pt clusters. The as‐prepared catalyst exhibits excellent HER performances comparable to commercial Pt/C, including a low overpotential of 34 mV to reach a current density of 10 mA cm −2 , a superior mass activity (1847 mA mg Pt −1 ), a small Tafel slope (29.7 mV dec −1 ), and a high turnover frequency (10.66 H 2 s −1 ). The improved activity of Pt/MXene can be attributed to the charge transfer from Pt clusters to MXene, which weakens the hydrogen adsorption, as evidenced by the density functional theory calculations. The present contribution proposes a novel strategy to anchor low‐mass‐loading sub‐nanometer precious metal clusters on crumpled MXene with fully exposed active sites for catalysis.