Direct Neutron Spectroscopy Observation of Cerium Hydride Species on a Cerium Oxide Catalyst

Wu, Zili; Cheng, Yongqiang; Tao, Franklin; Daemen, Luke; Foo, Guo Shiou; Nguyen, Luan; Zhang, Xiaoyan; Beste, Ariana; Ramirez-Cuesta, Anibal J.

doi:10.1021/jacs.7b05492

Direct Neutron Spectroscopy Observation of Cerium Hydride Species on a Cerium Oxide Catalyst

Journal Article · Tue Jun 27 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b05492· OSTI ID:1376480

^[1]; Cheng, Yongqiang ^[2]; ^[3]; Daemen, Luke ^[2]; Foo, Guo Shiou ^[1]; Nguyen, Luan ^[3]; Zhang, Xiaoyan ^[3]; ^[4]; Ramirez-Cuesta, Anibal J. ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division. Center for Nanophase Materials Sciences
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Chemistry
Univ. of Tennessee, Oak Ridge, TN (United States). Joint Inst. for Computational Sciences

Ceria has recently shown intriguing hydrogenation reactivity in catalyzing alkyne selectively to alkenes. However, the mechanism of the hydrogenation reaction, especially the activation of H₂, remains experimentally elusive. In this paper, we report the first direct spectroscopy evidence for the presence of both surface and bulk Ce–H species upon H₂ dissociation over ceria via in situ inelastic neutron scattering spectroscopy. Combined with in situ ambient-pressure X-ray photoelectron spectroscopy, IR, and Raman spectroscopic studies, the results together point to a heterolytic dissociation mechanism of H₂ over ceria, leading to either homolytic products (surface OHs) on a close-to-stoichiometric ceria surface or heterolytic products (Ce–H and OH) with the presence of induced oxygen vacancies in ceria. Finally, the finding of this work has significant implications for understanding catalysis by ceria in both hydrogenation and redox reactions where hydrogen is involved.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Contributing Organization:: Univ. of Tennessee, Oak Ridge, TN (United States)

Grant/Contract Number:: AC05-00OR22725; SC0014561

OSTI ID:: 1376480

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 28 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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