Harnessing Wrinkles in Pt-Doped Pd Metallenes for Enhanced Hydrogen Evolution

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Abstract
Strain relaxation in atomically thin two-dimensional (2D) materials typically leads to geometric wrinkles or ripples. These intrinsic structural features can significantly influence the material’s electronic and mechanical properties, playing a crucial role in modifying catalytic behavior. Here, we report a strain-induced wrinkling strategy to construct synergistic active sites in Pt-doped Pd metallenes for efficient acidic hydrogen evolution reaction. Controlled Pt doping generates lattice mismatch and internal stress, driving spontaneous wrinkle formation. Characterization reveals that these wrinkled regions integrate electron transfer with localized strain effects, serving as efficient active sites. This geometry-electron synergy lowers the activation barrier, shifting reaction kinetics toward the efficient Volmer–Tafel pathway. Consequently, the optimized Pt5.0-Pd ML achieves an ultralow overpotential of 18 mV at 10 mA cm–2, significantly outperforming commercial benchmarks. This work highlights wrinkle engineering as a key strategy for tuning metallene catalytic performance, offering a rational design route for advanced 2D electrocatalysts.
Funding Information
  • East China University of Science and Technology
  • Science and Technology Commission of Shanghai Municipality (22ZR1415700)
  • Science and Technology Commission of Shanghai Municipality (24DX1400200)
  • Fundamental Research Funds for the Central Universities
  • National Natural Science Foundation of China (22376062)

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