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  Interaction of Hydrogen with Ceria: Hydroxylation, Reduction, and Hydride Formation on the Surface and in the Bulk

Li, Z., Werner, K., Chen, L., Jia, A., Qian, K., Zhong, J., You, R., Wu, L., Zhang, L., Pan, H., Wu, X.-P., Gong, X.-Q., Shaikhutdinov, S. K., Huang, W., & Freund, H.-J. (2020). Interaction of Hydrogen with Ceria: Hydroxylation, Reduction, and Hydride Formation on the Surface and in the Bulk. Chemistry – A European Journal. doi:10.1002/chem.202005374.

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アイテムのパーマリンク: https://hdl.handle.net/21.11116/0000-0007-A33B-F 版のパーマリンク: https://hdl.handle.net/21.11116/0000-0007-A33F-B
資料種別: 学術論文

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chem.202005374.pdf (出版社版), 3MB
ファイルのパーマリンク:
https://hdl.handle.net/21.11116/0000-0007-A33D-D
ファイル名:
chem.202005374.pdf
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application/pdf / [MD5]
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著作権日付:
2021
著作権情報:
The Author(s)

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作成者

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 作成者:
Li, Zhaorui1, 著者
Werner, Kristin2, 著者           
Chen, Lu3, 著者
Jia, Aiping1, 4, 著者
Qian, Kun1, 著者
Zhong, JianQiang2, 著者           
You, Rui1, 著者
Wu, Lihui5, 著者
Zhang, Liyuan1, 著者
Pan, Haibin5, 著者
Wu, Xin-Ping3, 著者
Gong, Xue-Qing3, 著者
Shaikhutdinov, Shamil K.2, 著者           
Huang, Weixin1, 6, 著者
Freund, Hans-Joachim2, 著者           
所属:
1Hefei National Laboratory for Physical Sciences at Microscale, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Key Laboratory of Materials for Energy Conversion and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, P. R. China, ou_persistent22              
2Chemical Physics, Fritz Haber Institute, Max Planck Society, ou_24022              
3Key Laboratory for Advanced Materials and Joint International Research Laboratory for Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, P.R. China., ou_persistent22              
4Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, P. R. China , ou_persistent22              
5 National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China, ou_persistent22              
6Dalian National Laboratory for Clean Energy, Dalian 116023, P. R. China, ou_persistent22              

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 要旨: The study reports on a first attempt to address the interplay between surface and bulk in hydride formation in ceria (CeO2) by combining experiment, using surface sensitive and bulk sensitive spectroscopic techniques on the two sample systems, i.e., CeO2(111) thin films and CeO2 powders, and theoretical calculations of CeO2(111) surfaces with oxygen vacancies (Ov) at the surface and in the bulk. We show that, on a stoichiometric CeO2(111) surface, H2 dissociates and forms surface hydroxyls (OH). On the pre‐reduced CeO2 samples, both films and powders, hydroxyls and hydrides (Ce‐H) are formed on the surface as well as in the bulk, accompanied by the Ce3+«Ce4+ redox reaction. As the Ov concentration increases, hydroxyl is destabilized and hydride becomes more stable. Surface hydroxyl is more stable than bulk hydroxyl, whereas bulk hydride is more stable than surface hydride. The surface hydride formation is the kinetically‐favorable process at relatively low temperatures, and the resulting surface hydride may diffuse into the bulk region and be stabilized therein. At higher temperatures, surface hydroxyls can react to produce water and create additional oxygen vacancies, increasing its concentration, which controls the H2/CeO2 interaction. The results demonstrate a large diversity of reaction pathways, which have to be taken into account for better understanding of reactivity of ceria‐based catalysts in a hydrogen‐rich atmosphere.

資料詳細

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言語: eng - English
 日付: 2020-12-172020-12-212020-12-23
 出版の状態: オンラインで出版済み
 ページ: 20
 出版情報: -
 目次: -
 査読: 査読あり
 識別子(DOI, ISBNなど): DOI: 10.1002/chem.202005374
 学位: -

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出版物 1

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出版物名: Chemistry – A European Journal
  その他 : Chem. – Eur. J.
  その他 : Chem. Eur. J.
種別: 学術雑誌
 著者・編者:
所属:
出版社, 出版地: Weinheim : Wiley-VCH
ページ: 20 巻号: - 通巻号: - 開始・終了ページ: - 識別子(ISBN, ISSN, DOIなど): ISSN: 0947-6539
CoNE: https://pure.mpg.de/cone/journals/resource/954926979058