Reversible transformation of sub-nanometer Ga-based clusters to isolated <sup>[4]</sup>Ga<sub>(4Si)</sub> sites creates active centers for propane dehydrogenation

Chen, Zixuan; Serykh, Alexander I.; Kierzkowska, Agnieszka; Gajan, David; Docherty, Scott R.; Yakimov, Alexander V.; Abdala, Paula M.; Copéret, Christophe; Florian, Pierre; Fedorov, Alexey; Müller, Christoph R.

doi:10.1039/d3cy01446k

Catal. Sci. Technol.

2024

DOI: 10.1039/d3cy01446k

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Reversible transformation of sub-nanometer Ga-based clusters to isolated ^[4]Ga_(4Si) sites creates active centers for propane dehydrogenation

Zixuan Chen,

Alexander I. Serykh,

Agnieszka Kierzkowska

et al.

Abstract: This work describes how a propane dehydrogenation catalyst with isolated [4]Ga(4Si) sites can be prepared from silica-supported sub-nm gallia clusters containing [4]Ga(Ga) and [6]Ga(Ga) sites.

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The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts

Castro‐Fernández,

Serykh,

Yarar

et al. 2024

Helvetica Chimica Acta

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Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga:Al (x : y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1 : 0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalysts reveals that the dispersion on silica increases the Ga‐normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2‐treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mostly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2‐treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga–H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga:Al ratios, give Ga–H bands at ca. 2040 and 2060 cm−1.

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The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts

Castro‐Fernández,

Serykh,

Yarar

et al. 2024

Helvetica Chimica Acta

View full text Add to dashboard Cite

show abstract

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Reversible transformation of sub-nanometer Ga-based clusters to isolated ^[4]Ga_(4Si) sites creates active centers for propane dehydrogenation

Abstract: This work describes how a propane dehydrogenation catalyst with isolated [4]Ga(4Si) sites can be prepared from silica-supported sub-nm gallia clusters containing [4]Ga(Ga) and [6]Ga(Ga) sites.

Cited by 1 publication

References 64 publications

The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts

The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts

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Reversible transformation of sub-nanometer Ga-based clusters to isolated [4]Ga(4Si) sites creates active centers for propane dehydrogenation

Abstract: This work describes how a propane dehydrogenation catalyst with isolated [4]Ga(4Si) sites can be prepared from silica-supported sub-nm gallia clusters containing [4]Ga(Ga) and [6]Ga(Ga) sites.

Cited by 1 publication

References 64 publications

The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts

The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts

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Product

Resources

About

Reversible transformation of sub-nanometer Ga-based clusters to isolated ^[4]Ga_(4Si) sites creates active centers for propane dehydrogenation

The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts

The Relation between Nature and Stability of H₂‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)₂O₃ Mixed Oxide Propane Dehydrogenation Catalysts