Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon

Brack, Enzo; Plodinec, Milivoj; Willinger, Marc-Georg; Copéret, Christophe

doi:10.1039/d3sc04711c

Cited by 3 publications

(3 citation statements)

References 28 publications

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“…Considering that carbon is a more neutral support and less prompt to interfere with the dynamic at the PtGa−GaO x interface than silica, we thus prepared carbon-supported PtGa nanoparticles (PtGa@ C) via SOMC. 35 For this, a mesoporous carbon was first treated in refluxing nitric acid to introduce oxygen functional groups (R−OH), 36 followed by sequential grafting of two siloxide-free precursors Ga(Mesityl) 3 and Pt(η 3 -allyl)(DIA) to avoid the introduction of an additional oxide interface (Figure S18). Finally, treatment under H 2 resulted in the formation of narrowly distributed PtGa nanoparticles supported on carbon with an average size of 1.4 nm (Figure S23) and a Pt/Ga 0 ratio of ca.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…We next examined the influence of the support on the catalytic performance of the PtGa system. Considering that carbon is a more neutral support and less prompt to interfere with the dynamic at the PtGa–GaO x interface than silica, we thus prepared carbon-supported PtGa nanoparticles (PtGa@C) via SOMC . For this, a mesoporous carbon was first treated in refluxing nitric acid to introduce oxygen functional groups (R–OH), followed by sequential grafting of two siloxide-free precursors Ga(Mesityl) 3 and Pt(η 3 -allyl)(DIA) to avoid the introduction of an additional oxide interface (Figure S18).…”

Section: Resultsmentioning

confidence: 99%

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Reactivity Switch of Platinum with Gallium: From Reverse Water Gas Shift to Methanol Synthesis

Zhou,

Brack,

Ehinger

et al. 2024

J. Am. Chem. Soc.

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The development of efficient catalysts for the hydrogenation of CO 2 to methanol using "green" H 2 is foreseen to be a key step to close the carbon cycle. In this study, we show that small and narrowly distributed alloyed PtGa nanoparticles supported on silica, prepared via a surface organometallic chemistry (SOMC) approach, display notable activity for the hydrogenation of CO 2 to methanol, reaching a 7.2 mol CH3OH h −1 mol Pt −1 methanol formation rate with a 54% intrinsic CH 3 OH selectivity. This reactivity sharply contrasts with what is expected for Pt, which favors the reverse water gas shift reaction, albeit with poor activity (2.6 mol CO2 h −1 mol Pt −1 ). In situ XAS studies indicate that ca. 50% of Ga is reduced to Ga 0 yielding alloyed PtGa nanoparticles, while the remaining 50% persist as isolated Ga III sites. The PtGa catalyst slightly dealloys under CO 2 hydrogenation conditions and displays redox dynamics with PtGa−GaO x interfaces responsible for promoting both the CO 2 hydrogenation activity and methanol selectivity. Further tailoring the catalyst interface by using a carbon support in place of silica enables to improve the methanol formation rate by a factor of ∼5.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Reactivity Switch of Platinum with Gallium: From Reverse Water Gas Shift to Methanol Synthesis

Zhou,

Brack,

Ehinger

et al. 2024

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

show abstract

“…Considering that carbon is a more neutral support and less prompt to interfere with the dynamic at the PtGa-GaOx interface than silica, we thus prepared carbon-supported PtGa nanoparticles (PtGa@C) via SOMC. 32 For this, a mesoporous carbon was first treated in refluxing nitric acid to introduce oxygen functional groups (R-OH), 33 followed by sequential grafting of two siloxide-free precursors Ga(Mesityl)3 and Pt ( 3 -allyl)(DIA) to avoid the introduction of an additional oxide interface (Figure S17). Finally, treatment under H2 resulted in the formation of narrowly distributed Pt nanoparticles supported on carbon with an average size of 1.4 nm (Figure S22) and a Pt/Ga 0 ratio of ca.…”

Section: Introductionmentioning

confidence: 99%

Reactivity Switch of Platinum with Gallium: from Reverse Water Gas Shift to Methanol Synthesis

Zhou,

Brack,

Ehinger

et al. 2024

Preprint

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The development of efficient catalysts for the hydrogenation of CO2 to methanol using “green” H2 is foreseen to be a key step to close the carbon cycle. In this study, we show that small and narrowly distributed alloyed PtGa nanoparticles supported on silica, prepared via a surface organometallic chemistry (SOMC) approach, display notable activity for the hydrogenation of CO2 to methanol, reaching 7.2 mol h-1 molPt-1 methanol formation rate with a 54% intrinsic CH3OH selectivity. This reactivity sharply contrasts with what is expected for Pt, which favors the reverse water gas shift reaction, albeit with a poor activity (2.6 mol h-1 molPt-1). In situ XAS studies indicate that ca. 50% of Ga is reduced to Ga0 yielding alloyed PtGa nanoparticles, while the remaining 50% persist as isolated GaIII sites. The PtGa catalyst slightly dealloys under CO2 hydrogenation conditions and displays redox dynamics with PtGa-GaOx interfaces, responsible for promoting both CO2 hydrogenation activity and methanol selectivity. Further tailoring the catalyst interface by using a carbon support in place of silica enables to improve the methanol formation rate by a factor of ~5.

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Pt-based catalysts for direct propane dehydrogenation: Mechanisms revelation, advanced design, and challenges

Sun,

Zhai,

Weng

et al. 2024

Molecular Catalysis

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Implications of Ga promotion and metal–oxide interface from tailored PtGa propane dehydrogenation catalysts supported on carbon

Abstract: Propane Dehydrogenation is a key technology, where Pt-based catalysts have widely been investigated in industry and academia, with development exploring the use of promoters (Sn, Zn, Ga, etc.) and additives...

Cited by 3 publications

References 28 publications

Reactivity Switch of Platinum with Gallium: From Reverse Water Gas Shift to Methanol Synthesis

Reactivity Switch of Platinum with Gallium: From Reverse Water Gas Shift to Methanol Synthesis

Reactivity Switch of Platinum with Gallium: from Reverse Water Gas Shift to Methanol Synthesis

Pt-based catalysts for direct propane dehydrogenation: Mechanisms revelation, advanced design, and challenges

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