Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation

Jimenez, Juan D.; Wen, Cun; Royko, Michael M.; Kropf, Arthur J.; Segre, Carlo; Lauterbach, Jochen

doi:10.1002/cctc.201901676

Title: Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO₂ Hydrogenation

Journal Article · Mon Dec 16 00:00:00 UTC 2019 · ChemCatChem

DOI: https://doi.org/10.1002/cctc.201901676 · OSTI ID:1763652

Jimenez, Juan D. ^[1]; Wen, Cun ^[1]; Royko, Michael M. ^[1]; Kropf, Arthur J. ^[2]; Segre, Carlo ^[3];

^[1]

Univ. of South Carolina, Columbia, SC (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Illinois Institute of Technology, Chicago, IL (United States). Center for Synchrotron Research and Instrumentation

Heterogeneous catalysts generally have a variety of active-site structures due to the innate heterogeneity of the surface,resulting in complicated correlations between activity and active-site structure. Single site heterogeneous cobalt catalysts with a uniform catalytic surface were utilized as a platform to probe surface sensitive reactions; in this case CO₂ hydrogenation. It was found that atomically isolated cobalt single sites, which exist solely in the tetrahedral Co²⁺ coordination, exclusively form CO under typical CO₂ methanation conditions,while cobalt clusters yielded the highest rate of CO₂ reactionand began to form methane. Utilizing the principles of Ostwald Ripening to probe the ensemble effects for CO₂ hydrogenation, the transition from atomic isolation to small clusters of atoms to nanoparticles was explored. Furthermore, the chemical structure of the cobalt was elucidated primarily via X-Ray Absorption Spectroscopy (XANES/EXAFS) and X-Ray Photoelectron Spectroscopy (XPS).

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1763652

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 3 Vol. 12; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 hydrogenation
CO2 methanation
Cobalt
Cobalt single-site catalysts
Ensemble effects
Ostwald Ripening
XAFS
XPS

Title: Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO2 Hydrogenation

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Title: Influence of Coordination Environment of Anchored Single-Site Cobalt Catalyst on CO₂ Hydrogenation