In Situ Elucidation of the Active State of Co–CeOx Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

Zhang, Feng; Liu, Zongyuan; Zhang, Shuhao; Akter, Nusnin; Palomino, Robert M.; Vovchok, Dimitriy; Orozco, Ivan; Salazar, David; Rodriguez, Jose A.; Llorca, Jordi; Lee, Jaeha; Kim, DoHeui; Xu, Wenqian; Frenkel, Anatoly I.; Li, Yuanyuan; Kim, Taejin; Senanayake, Sanjaya D.

doi:10.1021/acscatal.7b03640

Title: In Situ Elucidation of the Active State of Co–CeO_x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

Journal Article · Mon Mar 12 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b03640· OSTI ID:1462401

Zhang, Feng ^[1];

^[2]; Zhang, Shuhao ^[1]; Akter, Nusnin ^[1]; Palomino, Robert M. ^[2];

^[3]; Orozco, Ivan ^[3]; Salazar, David ^[2];

^[4];

^[5]; Lee, Jaeha ^[6];

^[6]; Xu, Wenqian ^[7];

^[8]; Li, Yuanyuan ^[1];

^[1];

^[2]

Stony Brook Univ., NY (United States). Materials Science and Chemical Engineering Dept.
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Stony Brook Univ., NY (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Stony Brook Univ., NY (United States). Dept. of Chemistry
Technical Univ. of Catalonia, Barcelona (Spain). Inst. of Energy Technologies, Dept. of Chemical Engineering and Barcelona Research Center in Multiscale Science and Engineering
Seoul National Univ. (Korea, Republic of). School of Chemical and Biological Engineering, Inst. of Chemical Processes
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division
Stony Brook Univ., NY (United States). Materials Science and Chemical Engineering Dept.; Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry

The activation of methane and its dry reforming with CO2 was systematically studied over a series (2-30 wt %) of CO2 (similar to 5 nm in size) loaded CeO2 catalysts, with an effort to elucidate the interplay between Co and CeO2 during the catalytic process using in situ methods. The results of in situ time-resolved X-ray diffraction (TR-XRD) show a strong interaction of methane with the CoOx-CeO2 systems at temperatures between 200 and 350 degrees C. The hydrogen produced by the dissociation of C H bonds in methane leads to a full reduction of Co oxide, Co3O4 -> CoO -> Co, and a partial reduction of ceria with the formation of some Ce3+. Upon the addition of CO2, a catalytic cycle for dry reforming of methane (DRM) was achieved on the CoOx-CeO2 powder catalysts at temperatures below 500 degrees C. A 10 wt % Co-CeO2 catalyst was found to possess the best catalytic activity among various cobalt loading catalysts, and it exhibits a desirable stability for the DRM with a accumulation. The phase transitions and the nature of active components in the catalyst were investigated under reaction conditions by in situ time-resolved XRD and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). These studies showed dynamic evolutions in the chemical composition of the catalysts under reaction conditions. CO2 attenuated the reducing effects of methane. Under optimum CO- and H-2-producing conditions, both XRD and AP-XPS indicated that the active phase involved a majority of metallic Co with a small amount of CoO, both supported on a partially reduced ceria (Ce3+/Ce4+). We identified the importance of dispersing Co, anchoring it onto the ceria surface sites, and then utilizing the redox properties of CeO2 for activating and then oxidatively converting methane while inhibiting coke formation. Furthermore, a synergistic effect between cobalt and ceria and likely the interfacial sitee are essential to successfully close the catalytic cycle.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 1462401

Alternate ID(s):: OSTI ID: 1473677

Report Number(s):: BNL-207864-2018-JAAM

Journal Information:: ACS Catalysis, Vol. 8, Issue 4; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 62 works

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Title: In Situ Elucidation of the Active State of Co–CeOx Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

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Title: In Situ Elucidation of the Active State of Co–CeO_x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt