High-performance water gas shift induced by asymmetric oxygen vacancies: Gold clusters supported by ceria-praseodymia mixed oxides
Junjie Shi,Günther Rupprechter,Junjie Shi,Hailian Li,Alexander Genest,Weixuan Zhao,Pengfei Qi,Tao Wang,Günther Rupprechter +8 more
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In this article, mixed ceria-praseodymia supported Au clusters for the water gas shift reaction (WGSR) were employed for tuning catalytic activity, beneficial for bifunctional catalysis by reducible oxide supported metal nanoparticles.Abstract:
Modifying and controlling sites at the metal/oxide interface is an effective way of tuning catalytic activity, beneficial for bifunctional catalysis by reducible oxide supported metal nanoparticles. We employed mixed ceria-praseodymia supported Au clusters for the water gas shift reaction (WGSR). Varying the Ce: Pr ratio (4:1, 2:1, 1:4) not only allows to control the number of oxygen vacancies but, even more important, their local coordination, with asymmetrically coordinated O# being most active for water activation. These effects have been examined by X-ray absorption near edge structure (XANES), extended X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, temperature programmed desorption/reduction (TPD/TPR), and density functional theory (DFT). Using the WGSR performance of Au/CeOx as reference, Au/Ce4Pr1Ox was identified to exhibit the highest activity, with a CO conversion of 75% at 300°, which is about 5-times that of Au/CeOx. Au/Ce4Pr1Ox also showed excellent stability, with the conversion still being 70% after 50 h time-on-stream at 300 °. Although a higher Pr content leads to more O vacancies, the catalytic activity showed a “volcano behavior”. Based on DFT, this was rationalized via the formation energy of oxygen vacancies, the binding energy of water, and the asymmetry of the O# site. The presented route of creating active vacancy sites should also be relevant for other heterogeneous catalytic systems.read more
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The Route from Green H2 Production through Bioethanol Reforming to CO2 Catalytic Conversion: A Review
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Static and Dynamic Quantification Tracking of Asymmetric Oxygen Vacancies in Copper-Ceria Catalysts with Superior Catalytic Activity
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TL;DR: In this paper , a series of Cu-Ce catalysts were prepared by regulating the synthesis method, ARCu/Ce (atomic ratios of Cu to Ce), and pH of precipitation, so as to investigate CO and VOCs oxidations.
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Journal ArticleDOI
Role of an Interface for Hydrogen Production Reaction over Size-Controlled Supported Metal Catalysts
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Leveraging Pt/Ce1-xLaxO2-δ To Elucidate Interfacial Oxygen Vacancy Active Sites for Aerobic Oxidation of 5-Hydroxymethylfurfural.
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TL;DR: In this paper , a series of La3+-doped three-dimensional ordered macroporous CeO2 (3D-Ce1-xLaxO2-δ) were synthesized and applied as supports for Pt nanoparticles.
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