Optimizing Surface State Electrons of Topological Semi‐Metal by Atomic Doping for Enhanced Hydrogen Evolution Reaction

Abstract

AbstractTopological materials carrying topological surface states (TSSs) have extraordinary carrier mobility and robustness, which provide a new platform for searching for efficient hydrogen evolution reaction (HER) electrocatalysts. However, the majority of these TSSs originate from the sp band of topological quantum catalysts rather than the d band. Here, based on the density functional theory calculation, it is reported a topological semimetal Pd3Sn carrying TSSs mainly derived from d orbital and proposed that optimizing surface state electrons of Pd3Sn by introduction heteroatoms (Ni) can promote hybridization between hydrogen atoms and electrons, thereby reducing the Gibbs free energy (ΔGH) of adsorbed hydrogen and improving its HER performance. Moreover, this is well verified by electrocatalytic experiment results, the Ni‐doped Pd3Sn (Ni0.1Pd2.9Sn) show much lower overpotential (−29 mV vs RHE) and Tafel slope (17 mV dec−1) than Pd3Sn (−39 mV vs RHE, 25 mV dec−1) at a current density of 10 mA cm−2. Significantly, the Ni0.1Pd2.9Sn nanoparticles exhibit excellent stability for HER. The electrocatalytic activity of Ni0.1Pd2.9Sn nanoparticles is superior to that of commercial Pt. This work provides an accurate guide for manipulating surface state electrons to improve the HER performance of catalysts.