Metal Organic Framework Derived Synthesis of Cobalt Indium Catalysts for the Hydrogenation of CO2 to methanol
Type
ArticleAuthors
Pustovarenko, AlexeyDikhtiarenko, Alla
Bavykina, Anastasiya
Gevers, Lieven
Ramirez, Adrian
Russkikh, Artem
Telalovic, Selvedin
Aguilar, Antonio
Hazemann, Jean Louis
Ould-Chikh, Samy

Gascon, Jorge

KAUST Department
Chemical Engineering ProgramChemical Science
KAUST Catalysis Center (KCC)
King Abdullah University of Science and Technology, KAUST Catalysis Center (KCC), Advanced Catalytic Materials, Thuwal 23955, Saudi Arabia.
Physical Science and Engineering (PSE) Division
Date
2020-04-03Online Publication Date
2020-04-03Print Publication Date
2020-05-01Embargo End Date
2021-04-03Permanent link to this record
http://hdl.handle.net/10754/662470
Metadata
Show full item recordAbstract
Methanol 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.Citation
Pustovarenko, 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.0c00449Sponsors
The 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.Funding for this work was provided by King Abdullah University of Science and Technology (KAUST).
Publisher
American Chemical Society (ACS)Journal
ACS CatalysisAdditional Links
https://pubs.acs.org/doi/10.1021/acscatal.0c00449ae974a485f413a2113503eed53cd6c53
10.1021/acscatal.0c00449