Oxidation of Reduced Ceria by Incorporation of Hydrogen

Li, Zhaorui; Werner, Kristin; Qian, Kun; You, Rui; Płucienik, Agata; Jia, Aiping; Wu, Liang; Zhang, Liyuan; Pan, Haibin; Kuhlenbeck, Helmut; Shaikhutdinov, Shamil K.; Huang, Weixin; Freund, Hans‐Joachim

doi:10.1002/anie.201907117

Cited by 126 publications

(157 citation statements)

References 54 publications

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“…We have already shown that single Au atoms become charged upon adsorption on very thin MgO(001) films. Similar observations have been made for Au aggregates on a number of thin-film substrates [106]. We demonstrate this on Au aggregates adsorbed on alumina.…”

Section: Charge-transfer On and In Thin Oxide Filmssupporting

confidence: 88%

“…A case where such charge transfer is not an obvious option is illustrated by the interaction of hydrogen with reduced ceria [106]. We have discussed above the preparation and identification of oxygen vacancies in reduced ceria.…”

Section: Charge-transfer On and In Thin Oxide Filmsmentioning

confidence: 99%

“…The interaction of ceria with hydrogen has recently gained increasing interest, since it was reported that ceria may be used as a catalyst for selective hydrogenation of alkynes (triplebonded unsaturated hydrocarbons) to alkenes (double-bonded hydrocarbons) [107][108][109][110][111][112]. We have studied the interaction of H 2 with CeO 2 (111) crystalline films using XPS and electron energy loss spectroscopy [106]. Figure 17 shows Ce 3d spectra obtained at grazing emission before and after exposure of a reduced ceria film to 10 mbar of H 2 at 300 K. From the fit of the spectra we found that the amount of Ce 3+ at the surface considerably decreased upon reactions with H 2 thus indicating that hydrogen oxidizes CeO 2 (111), which sounds like a contradiction.…”

Section: Charge-transfer On and In Thin Oxide Filmsmentioning

confidence: 99%

“…The reduced CeO 2−x (111) film was then exposed to 10 mbar H 2 at 300 K for 15 min. The spectra were recorded in sequence from the bottom to the top, adapted with permission from Ref [106],. copyright by John Wiley and Sons (2019) (color online).…”

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Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

et al. 2020

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The review presents an overview of studies in the surface science of oxide and related surfaces with an emphasis of the studies performed in the authors' group. Novel instruments and technique developments, as well as their applications are reported, in an attempt to cover studies on model systems of increasing complexity, including some of the key ingredients of an industrially applied heterogeneous catalyst and its fabrication. The review is intended to demonstrate the power of model studies in understanding heterogeneous catalysis at the atomic level. The studies include those on supported nano-particles, both, prepared in vacuum and from solution, interaction of surfaces and the underlying bulk with molecules from the gas phase, strong metal support interaction, as well as the first attempt to include studies on reactions in confined spaces.

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Section: Charge-transfer On and In Thin Oxide Filmssupporting

confidence: 88%

Section: Charge-transfer On and In Thin Oxide Filmsmentioning

confidence: 99%

Section: Charge-transfer On and In Thin Oxide Filmsmentioning

confidence: 99%

mentioning

confidence: 99%

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Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

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“…Generally speaking, the existence of oxygen vacancy is accompanied by the change of valence of metal elements (the formation of low‐valent metal ions), so the existence and semi‐quantitative analysis of surface oxygen vacancies can be judged and calculated by XPS datum. [ 63 ]…”

Section: Characterization Of Oxygen Defects In Nanostructured Metal Omentioning

confidence: 99%

Oxygen Defects in Nanostructured Metal‐Oxide Gas Sensors: Recent Advances and Challenges^†

Ding

Liu

et al. 2020

Chin. J. Chem.

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Defect engineering has been the most promising strategy to modulate the surface microstructure and electronic structure of the metal oxides, which will govern the efficiency of a given oxide for the applications in heterogeneous catalysis, energy storage and conversion fields, and gas sensing. This review summarizes recent research advances on understanding the role of oxygen vacancies of the metal oxides in gas sensing. First, different strategies for oxygen vacancy productions are summarized and compared. Then, the proper characterization techniques for oxygen vacancy are introduced. Importantly, the structure-activity relationships between vacancy engineering and gas sensing ability are further illustrated coupling the experimental results and theoretical studies. Finally, the key challenges and prospects regarding defect engineering in gas sensing are highlighted. Wenjie Ding (left) obtained his bachelor degree from Beijing Forestry University in 2018. Currently, he is pursuing his master degree under the supervision of Associate Professor Jiajia Liu in Beijing Instituted of Technology, China. His current research interests mainly focus on the synthesis of nanomaterials for the application of gas sensing. Dr. Jiajia Liu (middle) received her PhD degree in 2010 from Department of Chemical & Biomolecular Engineering of National University of Singapore, Singapore. Currently, she is Associate Professor in School of Materials and Engineering, Beijing Institute of Technology, China. Her current research interest is the development of metal oxide nanostructures and their applications in sensor, catalysis, and optoelectronics. Jiatao Zhang (right) was born in 1975. He earned his PhD from the Department of Chemistry, Tsinghua University, in 2006. Currently, he is Xu Teli Professor in the School of Materials and Engineering, BIT. He was awarded the Excellent Young Scientist foundation of NSFC in 2013. He also serves as the director of Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications. His current research interest is inorganic chemistry of semiconductor-based hybrid nanostructures with novel optical, electronic properties for the applications in energy conversion and storage, catalysis, optoelectronics and biology.

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Distinct Crystal‐Facet‐Dependent Behaviors for Single‐Atom Palladium‐On‐Ceria Catalysts: Enhanced Stabilization and Catalytic Properties

Sun

Zhuang

et al. 2022

Advanced Materials

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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 CeO2, 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 CeO2, and Pd atoms can be trapped and thus feature atomic dispersion; by contrast, on the CeO2 (111) facet, Pd atoms will readily aggregate into clusters (Pdn). Furthermore, Pd1/CeO2(100) gives a high selectivity of 90.3% for the catalytic N‐alkylation reaction, which is 2.8 times higher than that for Pdn/CeO2(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.

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Oxidation of Reduced Ceria by Incorporation of Hydrogen

Cited by 126 publications

References 54 publications

Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

Oxygen Defects in Nanostructured Metal‐Oxide Gas Sensors: Recent Advances and Challenges^†

Distinct Crystal‐Facet‐Dependent Behaviors for Single‐Atom Palladium‐On‐Ceria Catalysts: Enhanced Stabilization and Catalytic Properties

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Oxidation of Reduced Ceria by Incorporation of Hydrogen

Cited by 126 publications

References 54 publications

Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

Chapter model systems in heterogeneous catalysis at the atomic level: a personal view

Oxygen Defects in Nanostructured Metal‐Oxide Gas Sensors: Recent Advances and Challenges†

Distinct Crystal‐Facet‐Dependent Behaviors for Single‐Atom Palladium‐On‐Ceria Catalysts: Enhanced Stabilization and Catalytic Properties

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Oxygen Defects in Nanostructured Metal‐Oxide Gas Sensors: Recent Advances and Challenges^†