期刊
SMALL
卷 17, 期 27, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202004289
关键词
clusters; heterogeneous catalysis; interfaces; nanoparticles; operando; surface science
类别
资金
- Austrian Science Fund (FWF) [F4502/04-N16, W1243, I942-N17, I1041-N28, P 32772-N, I 4434-N]
- Shanghai University of Engineering Science (SUES)
Operando characterization of catalysts is essential for identifying the relevant structure, composition, and adsorbed species, often achieved through techniques such as X-ray absorption spectroscopy and infrared spectroscopy. Combining experimental results with density functional theory allows for thorough interpretation. Understanding restructuring, surface composition alterations, and metal/oxide interface effects on catalytic performance is crucial for rational design and improvement.
Operando characterization of working catalysts, requiring per definitionem the simultaneous measurement of catalytic performance, is crucial to identify the relevant catalyst structure, composition and adsorbed species. Frequently applied operando techniques are discussed, including X-ray absorption spectroscopy, near ambient pressure X-ray photoelectron spectroscopy and infrared spectroscopy. In contrast to these area-averaging spectroscopies, operando surface microscopy by photoemission electron microscopy delivers spatially-resolved data, directly visualizing catalyst heterogeneity. For thorough interpretation, the experimental results should be complemented by density functional theory. The operando approach enables to identify changes of cluster/nanoparticle structure and composition during ongoing catalytic reactions and reveal how molecules interact with surfaces and interfaces. The case studies cover the length-scales from clusters via nanoparticles to meso-scale aggregates, and demonstrate the benefits of specific operando methods. Restructuring, ligand/atom mobility, and surface composition alterations during the reaction may have pronounced effects on activity and selectivity. The nanoscale metal/oxide interface steers catalytic performance via a long ranging effect. Combining operando spectroscopy with switching gas feeds or concentration-modulation provides further mechanistic insights. The obtained fundamental understanding is a prerequisite for improving catalytic performance and for rational design.
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