物理化学学报 >> 2025, Vol. 41 >> Issue (2): 100013.doi: 10.3866/PKU.WHXB202309036

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近常压X射线光电子能谱研究固-气和固-液界面

刘崇静1,2,†, 夏雨健1,†, 张鹏军1, 魏世强1, 曹登丰1,3, 圣蓓蓓1, 褚勇衡1, 陈双明1,*(), 宋礼1,3, 刘啸嵩1,*()   

  1. 1 中国科学技术大学国家同步辐射实验室, 中国科学院纳米科学卓越中心, 合肥 230026
    2 中国科学技术大学核科学技术学院, 合肥 230027
    3 合肥综合性国家科学中心能源研究院, 合肥 230031
  • 收稿日期:2023-09-20 修回日期:2023-10-17 录用日期:2023-10-23 发布日期:2023-12-20
  • 通讯作者: Email: csmp@ustc.edu.cn (陈双明)xsliu19@ustc.edu.cn (刘啸嵩)
  • 作者简介:

    †These authors contributed equally to this work.

  • 基金资助:
    国家重点研发计划(2019YFA0405601); 中国科学院青年创新促进会(2022457); 国家自然科学基金(12322515); 国家自然科学基金(U2032113); 国家自然科学基金(22075264); 国家自然科学基金(12205303); 中央高校基本科研基金(WK2060000039); 中央高校基本科研基金(WK2310000108)

Understanding Solid-Gas and Solid-Liquid Interfaces through Near Ambient Pressure X-Ray Photoelectron Spectroscopy

Chongjing Liu1,2, Yujian Xia1, Pengjun Zhang1, Shiqiang Wei1, Dengfeng Cao1,3, Beibei Sheng1, Yongheng Chu1, Shuangming Chen1,*(), Li Song1,3, Xiaosong Liu1,*()   

  1. 1 National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
    2 School of Nuclear Science and Technology, University of Science and Technology of China, Hefei 230027, China
    3 Institute of Energy, Hefei Comprehensive Nation Science Center, Hefei 230031, China
  • Received:2023-09-20 Revised:2023-10-17 Accepted:2023-10-23 Published:2023-12-20
  • Contact: Email: csmp@ustc.edu.cn (Shuangming Chen)xsliu19@ustc.edu.cn (Xiaosong Liu)
  • Supported by:
    the National Key Research and Development Program of China(2019YFA0405601); the Youth Innovation Promotion Association of CAS(2022457); the National Natural Science Foundation of China(12322515); the National Natural Science Foundation of China(U2032113); the National Natural Science Foundation of China(22075264); the National Natural Science Foundation of China(12205303); the Fundamental Research Funds for the Central Universities(WK2060000039); the Fundamental Research Funds for the Central Universities(WK2310000108)

摘要:

材料表面是能量储存和转化反应发生的直接场所,因此,真实反应条件下材料的表面化学和结构在理解反应机理方面起着关键作用。X射线光电子能谱是一种表面敏感技术,已经成为研究材料表面复杂成分和电子结构的主要工具之一。传统的X射线光电子能谱受限于真空条件,这限制了对原位条件下固-气和固-液界面的研究。但随着真空差分技术和静电透镜系统的引入,X射线光电子能谱不再局限于超高真空条件。结合同步辐射光源的优势,近常压X射线光电子能谱(NAP-XPS)展现出更先进的特点。在近年来,NAP-XPS迅速成为研究各种固-气和固-液界面的重要工具。通过NAP-XPS和一些先进的光谱学和显微镜技术,研究人员可以获得原子尺度的界面信息,这使得他们能够更深入地了解这些界面的性质。本文对近年来代表性的NAP-XPS研究进展进行了简要回顾,以阐明其在固-气和固-液界面研究领域中引发的新认识。最后,文章还讨论了关于NAP-XPS技术的挑战和前景,希望可以激发新的研究思路。

关键词: 近常压, X射线光电子能谱, 同步辐射, 能源材料, 固-气界面, 固-液界面

Abstract:

The surface of energy material is the direct place where energy storage and conversion reactions occur. Thus, the surface chemistry and the structure of the material under real reaction conditions are the key descriptors to clarify the reaction mechanism. However, such surfaces are usually immersed in gaseous or liquid environments under real reaction conditions, so it is not a simple task to identify the real physical and chemical properties of the interface under in situ conditions. X-ray photoelectron spectroscopy (XPS), as a surface-sensitive technique, is one of the main techniques for studying complex composition and electronic structure of material surfaces. However, due to the limited mean free path of photoelectrons in gas, liquid and solid media, the traditional XPS is confined to vacuum conditions, which poses a significant obstacle for studying solid-gas and solid-liquid interfaces under in situ conditions. With the introduction of differentially pumped analyzers and electrostatic lenses system, this limitation no longer restricts XPS only suitable for ultra-high vacuum conditions. With the active development of synchrotron radiation sources worldwide, near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) offers advanced features combined with the benefits of synchrotron radiation sources. Compared to traditional X-ray source, synchrotron radiation sources have significantly higher photon flux and much smaller spot size, which enables more electrons to escape to the electron analyzer, therefore can effectively improve the signal-to-noise ratio and the maximum working pressure, and the continuous wavelength tunability of synchrotron radiation makes experimental measurements more flexible and provides more information on the surface reaction. Over the years, NAP-XPS has rapidly emerged as an influential tool for investigating various solid-gas and solid-liquid interfaces, reflecting the importance of understanding reaction mechanisms and structure-performance relationship of materials under conditions closer to practical reacting conditions, particularly in heterogeneous catalysis. Information at atomic scale can be delivered with surface and interface sensitivity by NAP-XPS in conjunction with several advanced spectroscopy and microscopy techniques. In this paper, we provide a concise overview of recent notable advancements in NAP-XPS to showcase the novel insights generated by research on solid-gas and solid-liquid interfaces in cutting-edge scientific fields. This demonstrates how the knowledge gained from NAP-XPS studies can contribute to a fundamental understanding of reaction mechanisms at a molecular level. Finally, we discuss new challenges and prospects to ensure a comprehensive understanding of this technique and, hopefully, inspire fresh ideas.

Key words: Near ambient pressure, X-ray photoelectron spectroscopy, Synchrotron radiation, Energy material, Solid-gas interface, Solid-liquid interface