Reversible low-temperature redox activity and selective oxidation catalysis derived from the concerted activation of multiple metal species on Cr and Rh-incorporated ceria catalysts

Satoru Ikemoto; Xiubing Huang; Satoshi Muratsugu; Shoko Nagase; Takanori Koitaya; Hirosuke Matsui; Gen-ichi Yokota; Takatoshi Sudoh; Ayako Hashimoto; Yuanyuan Tan; Susumu Yamamoto; Jiayi Tang; Iwao Matsuda; Jun Yoshinobu; Toshihiko Yokoyama; Shinpei Kusaka; Ryotaro Matsuda; Mizuki Tada

doi:10.1039/C9CP04625A

Reversible low-temperature redox activity and selective oxidation catalysis derived from the concerted activation of multiple metal species on Cr and Rh-incorporated ceria catalysts†

Satoru Ikemoto,^a Xiubing Huang,

^b Satoshi Muratsugu,

*^ac Shoko Nagase,^a Takanori Koitaya,

^cd Hirosuke Matsui,

^a Gen-ichi Yokota,^a Takatoshi Sudoh,^a Ayako Hashimoto,

^ce Yuanyuan Tan,^b Susumu Yamamoto,

^f Jiayi Tang,^g Iwao Matsuda,

^f Jun Yoshinobu,

^f Toshihiko Yokoyama,

^d Shinpei Kusaka,

^h Ryotaro Matsuda

^h and Mizuki Tada

*^ab

Author affiliations

* Corresponding authors

^a Department of Chemistry, Graduate School of Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8602, Japan
E-mail: smuratsugu@chem.nagoya-u.ac.jp
Fax: +81-52-788-6093
Tel: +81-52-788-6093

^b Research Center for Materials Science (RCMS) & Integrated Research Consortium on Chemical Sciences (IRCCS), Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8602, Japan
E-mail: mtada@chem.nagoya-u.ac.jp
Fax: +81-52-788-6200
Tel: +81-52-788-6200

^c Japan Science and Technology Agency (JST), Precursory Research for Embryonic Science and Technology (PRESTO), 4-1-8 Honcho, Kawaguchi 332-0012, Japan

^d Department of Materials Molecular Science, Institute for Molecular Science, Myodaiji-cho, Okazaki, Aichi 444-8585, Japan

^e In-situ Characterization Technique Development Group, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba 305-0047, Japan

^f The Institute for Solid State Physics, The University of Tokyo, 5-1-5, Kashiwanoha, Kashiwa, Chiba 277-8581, Japan

^g Graduate School of Engineering, University of Hyogo, 2167, Shosha, Himeji, Hyogo 671-2280, Japan

^h Department of Chemistry and Biotechnology, Graduate School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8602, Japan

Abstract

The ceria-based catalyst incorporated with Cr and a trace amount of Rh (Cr_0.19Rh_0.06CeO_z) was prepared and the reversible redox performances and oxidation catalysis of CO and alcohol derivatives with O₂ at low temperatures (<373 K) were investigated. In situ X-ray absorption fine structure (XAFS), ambient-pressure X-ray photoelectron spectroscopy (AP-XPS), high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM)-EDS/EELS and temperature-programmed reduction/oxidation (TPR/TPO) revealed the structures and redox mechanisms of three metals in Cr_0.19Rh_0.06CeO_z: dispersed Rh^3+δ species (<1 nm) and Cr^6−γO_3−x nanoparticles (∼1 nm) supported on CeO₂ in Cr_0.19Rh_0.06CeO_z were transformed to Rh nanoclusters, Cr(OH)₃ species and CeO_2−x with two Ce³⁺-oxide layers at the surface in a concerted activation manner of the three metal species with H₂.

Physical Chemistry Chemical Physics

Reversible low-temperature redox activity and selective oxidation catalysis derived from the concerted activation of multiple metal species on Cr and Rh-incorporated ceria catalysts†

Abstract

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Reversible low-temperature redox activity and selective oxidation catalysis derived from the concerted activation of multiple metal species on Cr and Rh-incorporated ceria catalysts

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