The stability of Pd/TS-1 and Pd/silicalite-1 for catalytic oxidation of methane – understanding the role of titanium

Hosseiniamoli, Hadi; Setiawan, Adi; Adesina, Adesoji A.; Kennedy, Eric M.; Stockenhuber, Michael

doi:10.1039/c9cy01579e

Cited by 35 publications

(37 citation statements)

References 52 publications

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“…This partial agglomeration and oxidation of gold clusters results in a slight decrease in catalytic activity [40] as the time‐on‐stream increases (Figure 3 i–k) [41] . Furthermore, the comparison of Ti 2p spectra of untreated and post reaction Au/TS‐1 samples (Figure S10) reveals no shift in the binding energy, indicating the high stability of Ti in such oxidizing environment [42] . Titania plays a crucial role in the overall stability of Au/TS‐1 catalyst, since there is strong interaction between Au and Ti via adsorption of Au nanoparticles on Ti defect sites of the TS‐1 lattice [42, 43] .…”

Section: Resultsmentioning

confidence: 99%

“…[41] Furthermore,t he comparison of Ti 2p spectra of untreated and post reaction Au/TS-1 samples (Figure S10) reveals no shift in the binding energy,indicating the high stability of Ti in such oxidizing environment. [42] Titania plays ac rucial role in the overall stability of Au/TS-1 catalyst, since there is strong interaction between Au and Ti via adsorption of Au nanoparticles on Ti defect sites of the TS-1 lattice. [42,43] These Ti sites act as nucleating sites for Au nanoparticles (in the range of 1-10 nm) resulting in ah ighly stable Au/TS-1 catalyst.…”

Section: Methodsmentioning

confidence: 99%

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Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

et al. 2021

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Designing a stable and selective catalyst with high H2 utilisation is of pivotal importance for the direct gas‐phase epoxidation of propylene. This work describes a facile one‐pot methodology to synthesise ligand‐stabilised sub‐nanometre gold clusters immobilised onto a zeolitic support (TS‐1) to engineer a stable Au/TS‐1 catalyst. A non‐thermal O2 plasma technique is used for the quick removal of ligands with limited increase in particle size. Compared to untreated Au/TS‐1 catalysts prepared using the deposition precipitation method, the synthesised catalyst exhibits improved catalytic performance, including 10 times longer lifetime (>20 days), increased PO selectivity and hydrogen efficiency in direct gas phase epoxidation. The structure‐stability relationship of the catalyst is illustrated using multiple characterisation techniques, such as XPS, 31P MAS NMR, DR‐UV/VIS, HRTEM and TGA. It is hypothesised that the ligands play a guardian role in stabilising the Au particle size, which is vital in this reaction. This strategy is a promising approach towards designing a more stable heterogeneous catalyst.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

et al. 2021

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“… [41] Furthermore, the comparison of Ti 2p spectra of untreated and post reaction Au/TS‐1 samples (Figure S10) reveals no shift in the binding energy, indicating the high stability of Ti in such oxidizing environment. [42] Titania plays a crucial role in the overall stability of Au/TS‐1 catalyst, since there is strong interaction between Au and Ti via adsorption of Au nanoparticles on Ti defect sites of the TS‐1 lattice. [ 42 , 43 ] These Ti sites act as nucleating sites for Au nanoparticles (in the range of 1–10 nm) resulting in a highly stable Au/TS‐1 catalyst.…”

Section: Resultsmentioning

confidence: 99%

“… [42] Titania plays a crucial role in the overall stability of Au/TS‐1 catalyst, since there is strong interaction between Au and Ti via adsorption of Au nanoparticles on Ti defect sites of the TS‐1 lattice. [ 42 , 43 ] These Ti sites act as nucleating sites for Au nanoparticles (in the range of 1–10 nm) resulting in a highly stable Au/TS‐1 catalyst. [44] …”

Section: Resultsmentioning

confidence: 99%

“…Apart from these phosphine ligands, an additional factor contributing to the enhanced stability of Au nanoparticles during the epoxidation reaction is the presence of Ti defect sites, which act as nucleating sites for Au nanoparticles, preventing their oxidation and improving the stability of Au/TS‐1. [ 42 , 43 , 44 ] Although this work focused on propylene epoxidation, the insights provided herein can be used to rationally design stable catalysts with a longer lifetime for other reactions, which is an important aspect in the design of catalysts for industrial applications.…”

Section: Discussionmentioning

confidence: 99%

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Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

et al. 2021

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Designing astable and selective catalyst with high H 2 utilisation is of pivotal importance for the direct gas-phase epoxidation of propylene.This work describes afacile one-pot methodology to synthesise ligand-stabilised sub-nanometre gold clusters immobilised onto az eolitic support (TS-1) to engineer as table Au/TS-1 catalyst. An on-thermal O 2 plasma technique is used for the quickremoval of ligands with limited increase in particle size. Compared to untreated Au/TS-1catalysts prepared using the deposition precipitation method, the synthesised catalyst exhibits improved catalytic performance,i ncluding 10 times longer lifetime (> 20 days), increased PO selectivity and hydrogen efficiency in direct gas phase epoxidation. The structure-stability relationship of the catalyst is illustrated using multiple characterisation techniques,s uch as XPS, 31 PM AS NMR, DR-UV/VIS,H RTEM and TGA. It is hypothesised that the ligands play ag uardian role in stabilising the Au particle size, whichi sv ital in this reaction. This strategy is ap romising approach towards designing amore stable heterogeneous catalyst.

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Zeolites for Sustainable Chemical Transformations

Harvey

Drewery

Kennedy

et al. 2022

Heterogeneous Catalysis for Sustainable Energy

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The stability of Pd/TS-1 and Pd/silicalite-1 for catalytic oxidation of methane – understanding the role of titanium

Abstract: The stability of Pd/TS-1 and Pd/silicalite-1 catalysts was assessed at 400 °C and an approximate relative humidity (RH) of 80% for catalytic combustion of fugitive methane emissions, aiming to understand the role of titanium in the stability of the catalysts.

Cited by 35 publications

References 52 publications

Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

Precisely Engineered Supported Gold Clusters as a Stable Catalyst for Propylene Epoxidation

Zeolites for Sustainable Chemical Transformations

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