A General Strategy for Engineering Single-Metal Sites on 3D Porous N, P Co-Doped Ti₃C₂T_X MXene

Abstract

Two-dimensional (2D) MXenes have been developed to stabilize single atoms via various methods, such as vacancy reduction and heteroatom-mediated interactions. However, anchoring single atoms on 3D porous MXenes to further increase catalytic active sites and thus construct electrocatalysts with high activity and stability remains unexplored. Here, we reported a general synthetic strategy for engineering single-metal sites on 3D porous N, P codoped Ti3C2TX nanosheets. Through a “gelation-and-pyrolysis” process, a series of atomically dispersed metal catalysts (Pt, Ir, Ru, Pd, and Au) supported by N, P codoped Ti3C2TX nanosheets with 3D porous structure can be obtained and serve as efficient catalysts for the electrochemical hydrogen evolution reaction (HER). As a result of the favorable electronic and geometric structure of N­(O), P-coordinated metal atoms optimizing catalytic intermediates adsorption and 3D porous structure exposing the active surface sites and facilitating charge/mass transfer, the as-synthesized Pt SA-PNPM catalyst shows ∼20-fold higher activity than the commercial Pt/C catalyst for electrochemical HER over a wide pH range