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Dual-atom catalysts (DACs) have attracted considerable interest since they utilize adjacent metal centers in the metal(I)–metal(II) dimer structure to achieve functionality complementarity and more flexible active sites compared to single-atom catalysts (SACs). Herein, we report that the synergistic effect and electron redistribution effect in the Pt1Ru1 dimer can simultaneously accelerate the H2 generation and improve the catalyst’s activity. The as-developed Pt1Ru1/NMHCS-A exhibits a quite low overpotential (η10) of 22 mV to drive a current density of 10 mA cm–2, a large mass activity of 3.49 A mg–1 at 50 mV overpotential, a high turnover frequency (TOF) of 74.14 H2 s–1 at 200 mV overpotential, and a slight increment of 3 mV for η10 after 10,000 consecutive cyclic voltammetry (CV) cycles in 0.5 M H2SO4 solution, greatly outperforming the commercial 20 wt % Pt/C benchmark and nanoparticle counterparts. The detailed spectroscopic investigations and theoretical calculations confirm the formation of a C1–Pt–Ru–N2 coordination structure in Pt1Ru1/NMHCS-A and reveal the electron redistribution effect of Ru on the Pt atom. With the Ru atom tuning the electron redistribution, the Pt atom acting as the active site shows strong abilities to adsorb and reduce the proton, thus leading to the optimal HER activity. Our work provides constructive guidance for the fabrication of metal(I)–metal(II) dimers and the precise regulation of their electronic structures to achieve excellent catalytic activities.
Zhao et al. (Mon,) studied this question.