Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 17, Pages 9306-9310Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202100198
Keywords
catalytic hydrogenation; in situ spectroscopy; nanoparticles; SHINERS; single atoms
Categories
Funding
- NSFC [22021001, 21925404, 21972117, 21775127, 21991151]
- National Key Research and Development Program of China [2020YFB1505800, 2019YFA0705400]
- 111 Project [B17027]
- Natural Science Foundation of Fujian Province [2019J01030]
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The development of shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) has allowed for the characterization and in situ monitoring of Pd single-atom catalysts (SACs), revealing their unique catalytic properties and evolution processes. This new spectroscopic tool provides molecular insights into SACs and is particularly useful for studying solid-liquid interfaces.
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.
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