Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets
Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets
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单原子 Pt 修饰的 VS2 纳米片增强电催化析氢活性
DOI：
10.1021/acsnano.9b10048
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发表时间：
2020
期刊：
影响因子：
17.1
通讯作者：
Zhang Wenjing
中科院分区：
文献类型：
--
作者：
Zhu Jingting;Cai Lejuan;Yin Xinmao;Wang Zhuo;Zhang Linfei;Ma Haibin;Ke Yuxuan;Du Yonghua;Xi Shibo;Wee Andrew T. S.;Chai Yang;Zhang Wenjing
通过修饰催化剂中的贵金属来增强催化活性，为促进电催化析氢反应（HER）的应用提供了机会。然而，目前关于催化材料中贵金属结构的调控及其对析氢反应的影响的系统研究还很少。在此，报道了通过经济有效的光热方法将具有不同结构的 Pt 催化剂（包括单原子（SA）、簇和纳米粒子）很好地可控地锚定在 VS2 纳米片上，并研究了它们的 HER 性能。最高效的 Pt 修饰 VS2 催化剂（同时具有 Pt SA 和簇）在 10 mA cm–2 下可提供 77 mV 的过电势，接近 Pt/C (48 mV)。然而，Pt 的最佳质量活度（归一化为 Pt 含量）仅从 SA Pt 修饰的 VS2 中获得（即 200 mV 时的 22.88 A mgPt-1），并且比 Pt/C（1.87 A mgPt-1）大 12 倍，这归因于 Pt 利用率的大大提高。此外，理论模拟表明，Pt SA 修饰使 H* 的吸附自由能更接近热中性值，改善了电荷转移动力学，显着增强了 HER 活性。这项工作提供了一种基于 Pt 结构和 VS2 协同作用制备所需催化剂的途径，并揭示了增强催化活性的内在机制，这对于 HER 应用非常重要。
Enhancing catalytic activity by decorating noble metals in catalysts provides an opportunity for promoting the electrocatalytic hydrogen evolution reaction (HER) application. However, there are few systematic studies on regulating the structures of noble metals in catalytic materials and investigating their influence on HER. Herein, Pt catalysts with different structures including single atoms (SAs), clusters, and nanoparticles well-controllably anchored on VS2nanosheets through a cost-effective optothermal method are reported, and their HER performance is studied. The most efficient Pt-decorated VS2catalyst (with both Pt SAs and clusters) delivers an overpotential of 77 mV at 10 mA cm–2, close to that of Pt/C (48 mV). However, the optimal mass activity of Pt (normalizing to Pt content) is obtained from only SA Pt-decorated VS2(i.e., 22.88 A mgPt–1at 200 mV) and is 12 times greater than that of the Pt/C (1.87 A mgPt–1), attributed to the greatly enhanced Pt utilization. Additionally, the theoretical simulations reveal that Pt SA decoration makes the adsorption free energy of H* closer to the thermoneutral value and improves the charge-transfer kinetics, significantly enhancing HER activity. This work offers a pathway to prepare the desired catalyst based on synergy of Pt structures and VS2and reveals the intrinsic mechanism for enhancing catalytic activity, which is important for HER applications.