邻位邻近是单原子铂催化剂析氢反应的主要活性描述符。

IF 36.3 1区材料科学 Q1 Engineering

Nano-Micro Letters Pub Date : 2026-05-04 DOI:10.1007/s40820-026-02201-z

Xue-Lu Chen, Yu-Yang Liu, Sudip Biswas, Yi Yang, Yi Shi, Chun-Gen Liu, Xing-Hua Xia

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引用次数: 0

摘要

在单原子催化剂（SACs）中，精确控制邻接位点的接近性和电子状态使得原子水平的内在催化性质调制成为可能。虽然电子结构对催化性能的影响已经很好地确立，但邻接位点邻近性的影响仍未得到充分探讨。在这里，我们报道了MoS2上的单原子铂催化剂（Pt- sac /MoS2），其中相邻Pt （Ptadj）位点的可控富集和Pt的氧化态都是通过电位下沉积的Cu原子的电位移来调节的。我们发现析氢反应（HER）活性主要受非键合Pt∙∙Pt接近程度而不是氧化状态的支配：在酸性条件下，PtSA-0.1/MoS2中富集的Ptadj位点的质量活性比PtSA-0.3/MoS2中分离的Pt （Ptiso）位点高41倍。原位红外光谱显示，Ptiso位点优先结合线性吸附的氢中间体（*HL），而Ptadj位点稳定桥式氢中间体（*HB），这表明邻接位点接近。密度泛函理论计算表明，相邻的Pt原子促进了三中心“Pt- h -Pt”键合中间体的形成，降低了H-H偶联势垒，加速了HER动力学。这些发现确立了邻接位点邻近性是SACs的主要活性描述符，并为下一代高性能电催化剂的设计提供了新的原则。

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Adjacent-Site Proximity as a Dominant Activity Descriptor in Single-Atom Pt Catalysts for Hydrogen Evolution Reaction

Highlights

Site-specific underpotential deposition strategy enables precise spatial control over atomic-level active sites, enriching adjacent Pt sites while tuning oxidation states
Adjacent-site proximity dominates hydrogen evolution reaction (HER) activity, with adjacent Pt sites deliver a 41-fold higher mass activity than isolated Pt sites.
Pt–H–Pt bridge intermediate at adjacent sites lowers the H–H coupling barrier and accelerates HER kinetics.

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来源期刊

Nano-Micro Letters NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

32.60

自引率

4.90%

发文量

981

审稿时长

1.1 months

期刊介绍： Nano-Micro Letters is a peer-reviewed, international, interdisciplinary, and open-access journal published under the SpringerOpen brand. Nano-Micro Letters focuses on the science, experiments, engineering, technologies, and applications of nano- or microscale structures and systems in various fields such as physics, chemistry, biology, material science, and pharmacy.It also explores the expanding interfaces between these fields. Nano-Micro Letters particularly emphasizes the bottom-up approach in the length scale from nano to micro. This approach is crucial for achieving industrial applications in nanotechnology, as it involves the assembly, modification, and control of nanostructures on a microscale.