Wei Jie, Qin Si-Na, Yang Ji, Ya Han-Long, Huang Wei-Hsiang, Zhang Hua, Hwang Bing Joe, Tian Zhong-Qun, Li Jian-Feng
College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces,iChEM, College of Chemistry and Chemical Engineering, Fujian Key Laboratory of Advanced Materials, College of Energy, Xiamen University, Xiamen, 361005, China.
Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei, 10607, Taiwan.
Angew Chem Int Ed Engl. 2021 Apr 19;60(17):9306-9310. doi: 10.1002/anie.202100198. Epub 2021 Mar 17.
Developing advanced characterization techniques for single-atom catalysts (SACs) is of great significance to identify their structural and catalytic properties. Raman spectroscopy can provide molecular structure information, and thus, the technique is a promising tool for catalysis. However, its application in SACs remains a great challenge because of its low sensitivity. We develop a highly sensitive strategy that achieves the characterization of the structure of SACs and in situ monitoring of the catalytic reaction processes on them by shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) for the first time. Using the strategy, Pd SACs on different supports were identified by Raman spectroscopy and the nucleation process of Pd species from single atoms to nanoparticles was revealed. Moreover, the catalytic reaction processes of the hydrogenation of nitro compounds on Pd SACs were monitored in situ, and molecular insights were obtained to uncover the unique catalytic properties of SACs. This work provides a new spectroscopic tool for the in situ study of SACs, especially at solid-liquid interfaces.
开发用于单原子催化剂（SACs）的先进表征技术对于识别其结构和催化性能具有重要意义。拉曼光谱可以提供分子结构信息，因此该技术是一种很有前景的催化工具。然而，由于其灵敏度较低，它在SACs中的应用仍然是一个巨大的挑战。我们首次开发了一种高灵敏度策略，通过壳层隔离纳米粒子增强拉曼光谱（SHINERS）实现了对SACs结构的表征以及对其上催化反应过程的原位监测。利用该策略，通过拉曼光谱鉴定了不同载体上的钯单原子催化剂，并揭示了钯物种从单原子到纳米粒子的成核过程。此外，原位监测了硝基化合物在钯单原子催化剂上的催化加氢反应过程，并获得了分子层面的见解以揭示单原子催化剂独特的催化性能。这项工作为单原子催化剂的原位研究提供了一种新的光谱工具，特别是在固液界面处。
