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Distinct Crystal-Facet-Dependent Behaviors for Single-Atom Palladium-On-Ceria Catalysts: Enhanced Stabilization and Catalytic Properties
Hu, Botao1,2; Sun, Kaian1; Zhuang, Zewen1; Chen, Zheng3; Liu, Shoujie4; Cheong, Weng Chon5; Chen, Cheng6; Hu, Mingzhen7; Cao, Xing1; Ma, Junguo1; Tu, Renyong1; Zheng, Xusheng8; Xiao, Hai1; Chen, Xiao9; Cui, Yi10; Peng, Qing1; Chen, Chen1; Li, Yadong1
2022-04-21
Source PublicationAdvanced Materials
ISSN0935-9648
Volume34Issue:16
Other Abstract

High-performance, fully atomically dispersed single-atom catalysts (SACs) are promising candidates for next-generation industrial catalysts. However, it remains a great challenge to avoid the aggregation of isolated atoms into nanoparticles during the preparation and application of SACs. Here, the evolution of Pd species is investigated on different crystal facets of CeO, and vastly different behaviors on the single-atomic dispersion of surface Pd atoms are surprisingly discovered. In situ X-ray photoelectron spectroscopy (XPS), in situ near-ambient-pressure-XPS (NAP-XPS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and X-ray absorption spectroscopy (XAS) reveal that, in a reducing atmosphere, more oxygen vacancies are generated on the (100) facet of CeO, and Pd atoms can be trapped and thus feature atomic dispersion; by contrast, on the CeO (111) facet, Pd atoms will readily aggregate into clusters (Pd). Furthermore, Pd/CeO(100) gives a high selectivity of 90.3% for the catalytic N-alkylation reaction, which is 2.8 times higher than that for Pd/CeO(111). This direct evidence demonstrates the crucial role of crystal-facet effects in the preparation of metal-atom-on-metal-oxide SACs. This work thus opens an avenue for the rational design and targeted synthesis of ultrastable and sinter-resistant SACs.

KeywordCrystal-facets N-alkylation Reaction Oxygen Defects, Pd–ceo 2 Single-atom Catalysis
DOI10.1002/adma.202107721
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS SubjectChemistry, multidisciplinary;Chemistry, Physical;nanoScience & Nanotechnology;materials Science, Multidisciplinary;physics, Applied;physics, Condensed Matter
WOS IDWOS:000767033100001
Scopus ID2-s2.0-85126051339
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Cited Times [WOS]:3   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionDEPARTMENT OF PHYSICS AND CHEMISTRY
Corresponding AuthorPeng, Qing; Chen, Chen; Li, Yadong
Affiliation1.Department of Chemistry, Tsinghua University, Beijing, 100084, China
2.Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094, China
3.College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241000, China
4.Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031, China
5.Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, 999078, Macao
6.Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China
7.School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China
8.National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China
9.Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China
10.Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou, 215123, China
Recommended Citation
GB/T 7714
Hu, Botao,Sun, Kaian,Zhuang, Zewen,et al. Distinct Crystal-Facet-Dependent Behaviors for Single-Atom Palladium-On-Ceria Catalysts: Enhanced Stabilization and Catalytic Properties[J]. Advanced Materials,2022,34(16).
APA Hu, Botao,Sun, Kaian,Zhuang, Zewen,Chen, Zheng,Liu, Shoujie,Cheong, Weng Chon,Chen, Cheng,Hu, Mingzhen,Cao, Xing,Ma, Junguo,Tu, Renyong,Zheng, Xusheng,Xiao, Hai,Chen, Xiao,Cui, Yi,Peng, Qing,Chen, Chen,&Li, Yadong.(2022).Distinct Crystal-Facet-Dependent Behaviors for Single-Atom Palladium-On-Ceria Catalysts: Enhanced Stabilization and Catalytic Properties.Advanced Materials,34(16).
MLA Hu, Botao,et al."Distinct Crystal-Facet-Dependent Behaviors for Single-Atom Palladium-On-Ceria Catalysts: Enhanced Stabilization and Catalytic Properties".Advanced Materials 34.16(2022).
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