Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

Liu, Lichen; Meira, Debora M.; Arenal, Raul; Concepcion, Patricia; Puga, Alberto V.; Corma, Avelino

doi:10.1021/acscatal.9b04214

Title: Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

Journal Article · Fri Oct 25 00:00:00 EDT 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b04214· OSTI ID:1578205

Liu, Lichen ^[1]; Meira, Debora M. ^[2];

^[3];

^[1]; Puga, Alberto V. ^[1];

^[1]

Polytechnic Univ. of Valencia (UPV) (Spain)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Canadian Light Sources, Inc., Saskatoon, SK (Canada)
Univ. de Zaragoza (Spain); ARAID Foundation. Zaragoza (Spain)

Identification of active sites in heterogeneous metal catalysts is critical for understanding the reaction mechanism at the molecular level and for designing more efficient catalysts. Because of their structural flexibility, subnanometric metal catalysts, including single atoms and clusters with a few atoms, can exhibit dynamic structural evolution when interacting with substrate molecules, making it difficult to determine the catalytically active sites. Here, Pt catalysts containing selected types of Pt entities (from single atoms to clusters and nanoparticles) have been prepared, and their evolution has been followed, while they were reacting in a variety of heterogeneous catalytic reactions, including selective hydrogenation reactions, CO oxidation, dehydrogenation of propane, and photocatalytic H2 evolution reaction. By in situ X-ray absorption spectroscopy, in situ IR spectroscopy, and high-resolution electron microscopy techniques, we will show that some characterization techniques carried out in an inadequate way can introduce confusion on the interpretation of coordination environment of highly dispersed Pt species. Finally, the combination of catalytic reactivity and in situ characterization techniques shows that, depending on the catalyst–reactant interaction and metal–support interaction, singly dispersed metal atoms can rapidly evolve into metal clusters or nanoparticles, being the working active sites for those abovementioned heterogeneous reactions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC); European Research Council (ERC); Severo Ochoa Program; Ministry of Economic Affairs and Digital Transformation of Spain (MINECO); European Social Fund; European Union (EU); European Regional Development Fund

Grant/Contract Number:: AC02-06CH11357; ERC-AdG-2014-671093; SEV-2016-0683; MAT2016-79776-P; E13_17R-FEDER-UE; 823717; CTQ2015-74138-JIN,

OSTI ID:: 1578205

Journal Information:: ACS Catalysis, Vol. 9, Issue 12; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Title: Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

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