Electrocatalytic hydrogen evolution reaction (HER) shows potential to transition from fossil fuels to green renewable energy. Designed for high efficiency and stability electrocatalyst in pH-universal electrolyte is of great significance but challenging. Herein, a novel electrocatalyst of two-dimensional (2D) MoTiCT MXene supported Pt/Ni(OH) (denoted as Pt/Ni(OH)/MoTiCT) is reported by hydrogen spillover effect for efficient HER in the full-pH range. The operando electrochemical characterization reveals that the hydrogen spillover phenomenon interactions between multi-functional catalytic sites, e.g. Pt, Ni(OH) and MoTiCT, are used to enhance HER performance and expedite HER kinetics. Moreover, theoretical calculation via density functional theory demonstrates the Pt/Ni(OH)/MoTiCT possess free energy of absorbed hydrogen close to zero (≈– 0.09 eV), which leads to optimal activity. As expected, the electrocatalyst necessitates the overpotential of 25, 33 and 36 mV at 10 mA cm in acidic, alkaline, and neutral conditions, respectively, which are outperforming Pt/C. This work furtherly demonstrates a new way to design a powerful electrocatalyst for pH-universal HER based hydrogen spillover phenomenon.

中文翻译：

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Pt/Ni(OH)2/Mo2TiC2TX 电催化剂中的氢气溢出改善了 pH 通用析氢反应

电催化析氢反应（HER）显示出从化石燃料向绿色可再生能源转变的潜力。设计在pH通用电解质中高效稳定的电催化剂具有重要意义但也具有挑战性。在此，报道了一种新型二维（2D）MoTiCT MXene负载Pt/Ni(OH)电催化剂（表示为Pt/Ni(OH)/MoTiCT），通过氢溢出效应在全pH范围内实现高效的HER。原位电化学表征表明，多功能催化位点（例如 Pt、Ni(OH)2 和 MoTiCT）之间的氢溢出现象相互作用可用于增强 HER 性能并加速 HER 动力学。此外，通过密度泛函理论的理论计算表明，Pt/Ni(OH)/MoTiCT 所吸收的氢的自由能接近于零（≈– 0.09 eV），这导致了最佳的活性。正如预期的那样，该电催化剂在酸性、碱性和中性条件下在 10 mA cm 下需要分别具有 25、33 和 36 mV 的过电势，这优于 Pt/C。这项工作进一步展示了一种针对基于 pH 通用 HER 的氢溢出现象设计强大电催化剂的新方法。