Show simple item record

dc.contributor.authorPustovarenko, Alexey
dc.contributor.authorDikhtiarenko, Alla
dc.contributor.authorBavykina, Anastasiya
dc.contributor.authorGevers, Lieven
dc.contributor.authorRamirez, Adrian
dc.contributor.authorRusskikh, Artem
dc.contributor.authorTelalovic, Selvedin
dc.contributor.authorAguilar, Antonio
dc.contributor.authorHazemann, Jean Louis
dc.contributor.authorOuld-Chikh, Samy
dc.contributor.authorGascon, Jorge
dc.date.accessioned2020-04-09T10:37:03Z
dc.date.available2020-04-09T10:37:03Z
dc.date.issued2020-04-03
dc.identifier.citationPustovarenko, A., Dikhtiarenko, A., Bavykina, A., Gevers, L. E., Ramirez, A., Russkikh, A., … Gascon, J. (2020). Metal Organic Framework Derived Synthesis of Cobalt Indium Catalysts for the Hydrogenation of CO2 to methanol. ACS Catalysis. doi:10.1021/acscatal.0c00449
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.doi10.1021/acscatal.0c00449
dc.identifier.urihttp://hdl.handle.net/10754/662470
dc.description.abstractMethanol synthesis by means of direct CO2 hydrogenation has the potential to contribute to climate change mitigation by turning the most important greenhouse gas into a commodity. However, for this process to become industrially relevant, catalytic systems with improved activity, selectivity and stability are required. Here we explore the potential of metal-organic frameworks (MOF) as precursors for synthesis of Co3O4-supported In2O3 oxide composites for the direct CO2 hydrogenation to methanol. Stepwise pyrolytic-oxidative decomposition of indium-impregnated ZIF-67(Co) MOF affords the formation of a nanostructured In2O3@Co3O4 reticulated shell composite material able to reach a maximum methanol production rate of 0.65 gMeOH·gcat-1·h-1 with selectivity as high as 87% over 100 h on stream. Textural characteristics of the sacrificial ZIF-67(Co) matrix and In-loading were found to be important variables for optimizing the catalyst performance such as induction time, methanol productivity and selectivity. The structural investigation on the catalytic system reveals that the catalyst undergoes reorganization under reaction conditions, transforming from a Co3O4 with amorphous In2O3 shell into Co3InC0.75 covered by a layer consisting of a mixture of amorphous CoOx and In2O3 oxides. Structural reorganization is responsible for the observed induction period, while the amorphous mixed cobalt indium oxide shell is responsible for the high methanol yield and selectivity. Additionally, these results demonstrate the tunable performance of MOF-derived In2O3@Co3O4 catalyst as a function of the reaction conditions which allows to establish a reasonable trade-off between high methanol yield and selectivity in a wide temperature and pressure window.
dc.description.sponsorshipThe authors gratefully acknowledge the European Synchrotron Radiation Facility (Grenoble, France) for provision of beamtime (CH 5572) for XAS experiments carried out on the FAME beamline (BM30B) and support of their staff.
dc.description.sponsorshipFunding for this work was provided by King Abdullah University of Science and Technology (KAUST).
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/acscatal.0c00449
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.0c00449.
dc.titleMetal Organic Framework Derived Synthesis of Cobalt Indium Catalysts for the Hydrogenation of CO2 to methanol
dc.typeArticle
dc.contributor.departmentChemical Engineering Program
dc.contributor.departmentChemical Science
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentKing Abdullah University of Science and Technology, KAUST Catalysis Center (KCC), Advanced Catalytic Materials, Thuwal 23955, Saudi Arabia.
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Catalysis
dc.rights.embargodate2021-04-03
dc.eprint.versionPost-print
dc.contributor.institutionNéel, UPR2940 CNRS, University of Grenoble Alpes, F-38000 Grenoble, France.
kaust.personDikhtiarenko, Alla
kaust.personBavykina, Anastasiya
kaust.personGevers, Lieven
kaust.personRamirez, Adrian
kaust.personRusskikh, Artem
kaust.personTelalovic, Selvedin
kaust.personOuld-Chikh, Samy
kaust.personGascon, Jorge
refterms.dateFOA2020-04-09T10:38:47Z
dc.date.published-online2020-04-03
dc.date.published-print2020-05-01


Files in this item

Thumbnail
Name:
Mmetal organic.pdf
Size:
12.54Mb
Format:
PDF
Description:
Accepted manuscript

This item appears in the following Collection(s)

Show simple item record