相邻 Pt 单原子和簇的协同酸析氢：了解它们的优越活性和机制,Inorganic Chemistry

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相邻 Pt 单原子和簇的协同酸析氢：了解它们的优越活性和机制
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-04-20 , DOI: 10.1021/acs.inorgchem.3c00680
Chao Wang ₁ , Hu Zang ₁ , Changjiang Liu ₁ , Jiahao Wang ₁ , Long Kuai _{2,

3} , Baoyou Geng _{1,

3}

Affiliation

析氢反应 (HER) 涉及两步基本反应，为建立双中心协同催化剂提供了机会。这项工作展示了碳负载的 Pt 单原子和团簇 (Pt _1+Cs -NPC) 作为酸性 HER 的有效催化剂，在 10 mA/cm 2 时表现出 12.5 mV/dec 的超低塔菲尔斜率和 24 mV 的过电^势具有 3.8 wt% 的超低铂含量。Pt 质量活度和转换频率 (TOF) 分别是商业 Pt/C 的 10.2 倍和 5.4 倍。密度泛函理论（DFT）研究表明，Pt团簇调节相邻Pt单原子的电子态结构，使得Pt _1处的ΔG _H*位点接近 0。此外，DFT 研究证实 Pt 团簇和相邻的 Pt 单原子可以协同催化 Tafel 步骤并降低形成 H-H 键的能垒。同时，铂簇降低了附近铂单原子位点对海洛夫斯基步的能垒，加速了与水合氢离子的反应。研究表明，铂簇和铂单原子复合负载结构对 HER 反应的 Volmer-Tafel 或 Volmer-Heyrovsky 反应路径表现出优异的活性。_{这项工作清楚地了解了 Pt 1+Cs} -NPC的协同效应，为开发高效的 HER 催化剂提供了指导。

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Synergistic Acid Hydrogen Evolution of Neighboring Pt Single Atoms and Clusters: Understanding Their Superior Activity and Mechanism

The hydrogen evolution reaction (HER) involves two-step elementary reactions, providing an opportunity to establish dual-site synergistic catalysts. This work demonstrates carbon-supported Pt single atoms and clusters (Pt_1+Cs-NPC) as an efficient catalyst for acidic HER, which exhibits an ultralow Tafel slope of 12.5 mV/dec and an overpotential of 24 mV at 10 mA/cm² with an ultralow platinum content of 3.8 wt %. The Pt mass activity and turnover frequency (TOF) are 10.2 times and 5.4 times that of commercial Pt/C, respectively. The density functional theory (DFT) study shows that the Pt cluster regulates the electronic state structure of the adjacent Pt single atom, so that the ΔG_H* at the Pt₁ site approaches 0. Moreover, the DFT study confirms that Pt clusters and neighboring Pt single atoms can synergistically catalyze the Tafel step and reduce the energy barrier in forming the H–H bond. At the same time, the platinum cluster reduces the energy barrier of the nearby platinum single-atom site to the Heyrovsky step and accelerates the reaction with hydrated hydrogen ions. Studies have shown that platinum clusters and platinum single-atom composite loading structures exhibit excellent activity for the Volmer–Tafel or Volmer–Heyrovsky reaction paths of HER reactions. This work provides a clear understanding of the synergistic effect of Pt_1+Cs-NPC, which provides guidance for developing efficient HER catalysts.

更新日期：2023-04-20

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