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Study of sites and species during CO hydrogenation over silica-supported Co–Pd catalysts. Relation to performance in the process

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Abstract

Supported bimetallic catalysts of (Co + Pd)/SiO2 system were studied in carbon monoxide hydrogenation. Comparative analysis showed that depending on precursor treatment mode the catalysts ranged in different rows of activity in CO conversion and selectivity to methane. Samples of best performance were obtained after pretreatment in Ar flow. Highly selective catalysts were synthesized by reduction at 450 °C determining low metal dispersion, high extent of alloying, and agglomeration. A low H2,100C/COstrong adsorbed gas ratio was ascribed to a great amount of bimetallic particles and concerned with a diminished number of sites for multiply bonded CO species. Metal dispersion was low due to large Co particles, which enhanced CO dissociation and hydrogenation to CH4. In presence of bimetallic particles the reaction CO + 3H2 = CH4 + H2O was hampered. A decreased H2O formation influenced the WGS reaction. Catalyst samples activated at higher temperatures had better selectivity. During the process, formation of bidentate carbonate species was registered. It was supposed that palladium impeded creation of the latter species and following decomposition to CO2. Active catalyst samples were prepared by reduction at 300 °C leading to higher unreduced cobalt quota and metal dispersion, and decreased alloy particle formation. Higher H2,100C/COstrong ratio values were assigned to pure Co and Pd particle segregation, i.e. availability of sites for multiply bonded CO species favoring a higher activity in CO dissociation and further hydrogenation. A higher amount of CO species on these samples was conducive to CH4 formation, but also to CO2 production. The latter reaction was facilitated by unreduced cobalt.

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Data availability

All datasets for this study are included in the manuscript. They also are available in IC, BAS, Sofia, Bulgaria; IG, SAS, Kosice, Slovakia.

Code availability

Not applicable.

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Acknowledgements

Financial support by Bulgarian National Science Fund through contract KP-06-H29-9/14.12.2018 is greatly acknowledged. Research equipment of Distributed research infrastructure INFRAMAT (part of Bulgarian National Roadmap for Research Infrastructures) supported by Bulgarian Ministry of Education and Science was used in this investigation. The authors acknowledge English language text editing by Assoc. Prof. C. Bonev.

Funding

The research leading to these results received funding from Bulgarian National Science Fund under Grant Agreement No. KP-06-H29-9/2018.

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Authors and Affiliations

  1. Institute of Catalysis, Bulgarian Academy of Sciences, Acad. G. Bonchev St., Bldg. 11, 1113, Sofia, Bulgaria

    Maya Shopska, Hristo Kolev, Katerina Aleksieva, Iskra Shtereva, Krassimir Tenchev, Silviya Todorova & Georgi Kadinov

  2. Institute of Geotechnics, Slovak Academy of Sciences, Watsonova 45, 04001, Kosice, Slovakia

    Martin Fabian

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  1. Maya Shopska
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  2. Hristo Kolev
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  3. Katerina Aleksieva
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  6. Silviya Todorova
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  7. Martin Fabian
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  8. Georgi Kadinov
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Contributions

Conceptualization, writing—original draft preparation, visualization, project administration, funding acquisition [MS]; methodology [MS, ST, GK]; validation [MS, ST, HK, MF, KA, KT]; investigation [MS, HK, MF, KA, KT, ST, GK]; resources [MS, ST]; data curation [MS, ST, HK, MF, KA, KT]; writing—review and editing [GK]; supervision [GK].

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Correspondence to Maya Shopska.

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Shopska, M., Kolev, H., Aleksieva, K. et al. Study of sites and species during CO hydrogenation over silica-supported Co–Pd catalysts. Relation to performance in the process. Reac Kinet Mech Cat 134, 303–330 (2021). https://doi.org/10.1007/s11144-021-02067-9

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