Pt–Fe Nanoparticles Dispersed on Mesoporous Silica as Selective Catalysts for Dehydrogenation of Isobutane

Alberto Rodriguez Gomez; Samy Ould-Chikh; Wilson Henao; Giovanni Agostini; Gonzalo Prieto; Jorge Gascon

doi:10.1021/acsanm.3c03572

Pt–Fe Nanoparticles Dispersed on Mesoporous Silica as Selective Catalysts for Dehydrogenation of Isobutane

Alberto Rodriguez Gomez, Samy Ould-Chikh, Wilson Henao, Giovanni Agostini, Gonzalo Prieto, Jorge Gascon

Research output: Contribution to journal › Article › peer-review

Abstract

A series of catalysts composed of Pt–Fe nanoparticles supported on mesoporous silica SBA-15 (ca. 7 nm pore diameter) have been prepared by ultrasound-assisted coimpregnation of the metal precursors and evaluated in the nonoxidative dehydrogenation of isobutane. Prereduced catalytic systems were characterized by STEM-HAADF + EDS mapping and XAS to determine the chemical environment of the highly dispersed platinum active sites on the iron host matrix. While the monometallic platinum (nanoparticles) supported on SBA-15 material presented a rapid catalyst deactivation under reaction conditions, coordinatively unsaturated Pt–Fe (Pt ≪ Fe) sites located in the mesopores of SBA-15 showed a high steady-state activity (43% conversion) and selectivity (96% to isobutylene) in the dehydrogenation of isobutane at 550 °C for several hours. Temperature-programmed reduction profiles determined not only the substantially higher reducibility of FeOx species with doping amounts of platinum in the as-prepared (calcined) catalysts but also the detrimental structural changes undergone after consecutive reaction–regeneration cycles. Finally, reactivation under controlled conditions allows to minimize irreversible catalyst deactivation after successive cycles.

Original language	English (US)
Journal	ACS Applied Nano Materials
DOIs	https://doi.org/10.1021/acsanm.3c03572
State	Published - Oct 2 2023

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10.1021/acsanm.3c03572

https://repository.kaust.edu.sa/bitstream/10754/694853/1/Rodriguez-Gomez%20et%20al_manuscript.pdf

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@article{6d8828c793f748588c7e97a2ffdb5b7b,

title = "Pt–Fe Nanoparticles Dispersed on Mesoporous Silica as Selective Catalysts for Dehydrogenation of Isobutane",

abstract = "A series of catalysts composed of Pt–Fe nanoparticles supported on mesoporous silica SBA-15 (ca. 7 nm pore diameter) have been prepared by ultrasound-assisted coimpregnation of the metal precursors and evaluated in the nonoxidative dehydrogenation of isobutane. Prereduced catalytic systems were characterized by STEM-HAADF + EDS mapping and XAS to determine the chemical environment of the highly dispersed platinum active sites on the iron host matrix. While the monometallic platinum (nanoparticles) supported on SBA-15 material presented a rapid catalyst deactivation under reaction conditions, coordinatively unsaturated Pt–Fe (Pt ≪ Fe) sites located in the mesopores of SBA-15 showed a high steady-state activity (43% conversion) and selectivity (96% to isobutylene) in the dehydrogenation of isobutane at 550 °C for several hours. Temperature-programmed reduction profiles determined not only the substantially higher reducibility of FeOx species with doping amounts of platinum in the as-prepared (calcined) catalysts but also the detrimental structural changes undergone after consecutive reaction–regeneration cycles. Finally, reactivation under controlled conditions allows to minimize irreversible catalyst deactivation after successive cycles.",

author = "{Rodriguez Gomez}, Alberto and Samy Ould-Chikh and Wilson Henao and Giovanni Agostini and Gonzalo Prieto and Jorge Gascon",

note = "KAUST Repository Item: Exported on 2023-10-05 Acknowledgements: Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). A.R.G. acknowledge support by his postdoctoral grant IJC2020-044050-I funded by MCIN/AEI/10.13039/501100011033 and by European Union NextGenerationEU/PRTR. XAS experiments were performed at NOTOS beamline (ALBA Synchrotron) with the collaboration of ALBA staff. We also thank Jullian Vittenet, Diego Mateo, and Alla Dikhtiarenko for technical support and Sandra Ramirez Cherbuy (InkScience) for artwork.",

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doi = "10.1021/acsanm.3c03572",

language = "English (US)",

journal = "ACS Applied Nano Materials",

issn = "2574-0970",

publisher = "American Chemical Society",

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T1 - Pt–Fe Nanoparticles Dispersed on Mesoporous Silica as Selective Catalysts for Dehydrogenation of Isobutane

AU - Rodriguez Gomez, Alberto

AU - Ould-Chikh, Samy

AU - Henao, Wilson

AU - Agostini, Giovanni

AU - Prieto, Gonzalo

AU - Gascon, Jorge

N1 - KAUST Repository Item: Exported on 2023-10-05 Acknowledgements: Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). A.R.G. acknowledge support by his postdoctoral grant IJC2020-044050-I funded by MCIN/AEI/10.13039/501100011033 and by European Union NextGenerationEU/PRTR. XAS experiments were performed at NOTOS beamline (ALBA Synchrotron) with the collaboration of ALBA staff. We also thank Jullian Vittenet, Diego Mateo, and Alla Dikhtiarenko for technical support and Sandra Ramirez Cherbuy (InkScience) for artwork.

PY - 2023/10/2

Y1 - 2023/10/2

N2 - A series of catalysts composed of Pt–Fe nanoparticles supported on mesoporous silica SBA-15 (ca. 7 nm pore diameter) have been prepared by ultrasound-assisted coimpregnation of the metal precursors and evaluated in the nonoxidative dehydrogenation of isobutane. Prereduced catalytic systems were characterized by STEM-HAADF + EDS mapping and XAS to determine the chemical environment of the highly dispersed platinum active sites on the iron host matrix. While the monometallic platinum (nanoparticles) supported on SBA-15 material presented a rapid catalyst deactivation under reaction conditions, coordinatively unsaturated Pt–Fe (Pt ≪ Fe) sites located in the mesopores of SBA-15 showed a high steady-state activity (43% conversion) and selectivity (96% to isobutylene) in the dehydrogenation of isobutane at 550 °C for several hours. Temperature-programmed reduction profiles determined not only the substantially higher reducibility of FeOx species with doping amounts of platinum in the as-prepared (calcined) catalysts but also the detrimental structural changes undergone after consecutive reaction–regeneration cycles. Finally, reactivation under controlled conditions allows to minimize irreversible catalyst deactivation after successive cycles.

AB - A series of catalysts composed of Pt–Fe nanoparticles supported on mesoporous silica SBA-15 (ca. 7 nm pore diameter) have been prepared by ultrasound-assisted coimpregnation of the metal precursors and evaluated in the nonoxidative dehydrogenation of isobutane. Prereduced catalytic systems were characterized by STEM-HAADF + EDS mapping and XAS to determine the chemical environment of the highly dispersed platinum active sites on the iron host matrix. While the monometallic platinum (nanoparticles) supported on SBA-15 material presented a rapid catalyst deactivation under reaction conditions, coordinatively unsaturated Pt–Fe (Pt ≪ Fe) sites located in the mesopores of SBA-15 showed a high steady-state activity (43% conversion) and selectivity (96% to isobutylene) in the dehydrogenation of isobutane at 550 °C for several hours. Temperature-programmed reduction profiles determined not only the substantially higher reducibility of FeOx species with doping amounts of platinum in the as-prepared (calcined) catalysts but also the detrimental structural changes undergone after consecutive reaction–regeneration cycles. Finally, reactivation under controlled conditions allows to minimize irreversible catalyst deactivation after successive cycles.

UR - http://hdl.handle.net/10754/694853

UR - https://pubs.acs.org/doi/10.1021/acsanm.3c03572

U2 - 10.1021/acsanm.3c03572

DO - 10.1021/acsanm.3c03572

M3 - Article

SN - 2574-0970

JO - ACS Applied Nano Materials

JF - ACS Applied Nano Materials

ER -

Pt–Fe Nanoparticles Dispersed on Mesoporous Silica as Selective Catalysts for Dehydrogenation of Isobutane

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