Co-aromatization of methane with olefins: The role of inner pore and external surface catalytic sites

He, Peng; Jarvis, Jack; Meng, Shijun; Wang, Aiguo; Kou, Shiyu; Gatip, Richard; Yung, Matthew M.; Liu, Lijia; Song, Hua

doi:10.1016/j.apcatb.2018.04.034

Cited by 36 publications

(17 citation statements)

References 57 publications

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“…4-8 and Supplementary Table 9). Characterisation of fresh and 1-decene spent Ag-Ga/ZSM-5 agrees with our previous studies on this catalyst 11,17 . The reader is directed to Supplementary Discussion for in-depth discussion and results.…”

Section: Resultssupporting

confidence: 90%

“…Inner pore accessibility. To confirm the importance of inner pore accessibility in the upgrading of 1-decene, we performed a coking procedure known to selectively coke the inner pores of ZSM-5 17,41 . When this coked Ag-Ga/ZSM-5 catalyst is employed for 1-decene upgrading at 330°C, the catalyst activity is substantially diminished (Fig.…”

Section: Resultsmentioning

confidence: 99%

“…Catalyst preparation. Ammonium type ZSM-5 (NH 4 -ZSM-5) obtained from Zeolyst, USA (CBV 8014) was converted to hydrogen type ZSM-5 (HZSM-5) by calcination in static air at 600°C for 3 h. A silver-and gallium metal-modified HZSM-5 reported in our previous studies 11,17 was prepared by wetness impregnation technique. In a typical synthesis, a certain amount of AgNO 3 (Sigma-Aldrich, 99.9+%) and Ga(NO 3 ) 3 •xH 2 O (Sigma-Aldrich, 99.9%+) were dissolved in 10 g deionised (DI) water to form an aqueous solution of metal precursors and HZSM-5 support was then impregnated with the metal precursor to give the desired metal weight loading.…”

Section: Methodsmentioning

confidence: 99%

“…Coked Ag-Ga/ZSM-5 was prepared using the method described in the literature 17,41 . In a typical synthesis, NH 4 -ZSM-5 was ion exchanged three times by stirring an aqueous 0.1 M Ca(NO 3 ) 2 •4H 2 O (Alfa Aesar, 99%) (100 cm 3 g −1 zeolite ) at 80°C and then calcined in static air at 550°C for 2 h. The obtained powder was placed into a lab-fabricated flow reactor and treated at 600°C under N 2 flow for 2 h followed by an ethylene/N 2 mixture for an additional hour.…”

Section: Methodsmentioning

confidence: 99%

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Understanding zeolite deactivation by sulfur poisoning during direct olefin upgrading

et al. 2019

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The presence of sulfur contaminants in bitumen derived crude oils can lead to rapid catalyst deactivation and is a major problem faced by downstream refiners. Whilst expensive hydrotreating steps may remove much of the sulfur content, it is important to understand how catalyst deactivation by sulfur poisoning occurs and how it may be mitigated. Here we report a mechanistic study of sulfur poisoning over a zeolite catalyst promoted with silver and gallium Lewis acids. Olefin upgrading, an essential process in the refinement of heavy oils, is used as a model reaction. Access to the zeolite inner pores is blocked by bulky, weakly adsorbed sulfur species. Pore access and thus catalyst activity is restored by increasing the reaction temperature. We also show that a simple alkaline treatment greatly improves both the sulfur tolerance and performance of the catalyst. These findings may enhance the rational design of heterogenous catalysts for olefin upgrading.

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Section: Resultssupporting

confidence: 90%

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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Understanding zeolite deactivation by sulfur poisoning during direct olefin upgrading

et al. 2019

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“…The positive correlation between aromatic selectivity and the amount of acid sites suggests that higher acidity is favorable for aromatic formation, which is widely accepted as the main function of zeolite catalysts. [10,[12][13][14][15] However, with limited acidity, the aromatic content can be greatly lowered and ole n products with high purity of methylcyclopentene predominates, indicating that aromatization and isomerization are two competing reactions in catalytic cyclohexene conversion process, which can be effectively controlled by tuning the amount of acid sites.…”

Section: Relationship Between Surface Acidity and Catalytic Performanmentioning

confidence: 99%

Highly Selective Skeletal Isomerization of Cyclohexene Over Zeolite-Based Catalysts for High-Purity Methylcyclopentene Production

Song

Xu²,

Li³

et al. 2020

Preprint

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Cyclohexene skeletal isomerization was achieved under mild conditions over rationally designed zeolite-based catalysts with high selectivity towards methylcyclopentene and satisfactory stability for multiple runs. The favorable performance was investigated, which can be attributed to unique acidic, structural and morphologic features of optimized Co/NaUZSM-5 catalyst. Further experimental data suggested that carboncationic mechanism might be followed and the reaction mainly occurs within the internal pores of zeolite structures, which was also validated by DFT study.

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Application of co‐feeds in the catalytic conversion of light alkanes to aromatics: A comprehensive review

Lim,

Ryu,

Hwang

et al. 2024

ChemCatChem

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Catalytic conversion of light alkanes (C1‐C3) to aromatics offers an attractive valorization route for abundant gas resources and has been a prevalent topic of research over the past few decades. Despite considerable advancements in the understanding of these reactions, several fundamental and practical hurdles have prevented their industrial application. Among the numerous attempts to resolve these issues, co‐feeding certain additives yields promising results, including the activation of alkanes under milder conditions, an increase in catalytic stability, and a shift in product distribution towards more desirable compounds. Systematic studies have elucidated the precise working mechanism of the co‐feeds in aromatization systems, explaining the experimentally observed results. This review provides an extensive compilation of information on the application of co‐feeds in light alkane aromatization, which has accumulated in the literature since the pioneering reports in the 1990s. Detailed summaries are provided for each additive, ranging from hydrocarbons to oxidants. Viable strategies for future work in this field, aiming to bridge the gap between academic studies and industrial applications, are also discussed.

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Co-aromatization of methane with olefins: The role of inner pore and external surface catalytic sites

Cited by 36 publications

References 57 publications

Understanding zeolite deactivation by sulfur poisoning during direct olefin upgrading

Understanding zeolite deactivation by sulfur poisoning during direct olefin upgrading

Highly Selective Skeletal Isomerization of Cyclohexene Over Zeolite-Based Catalysts for High-Purity Methylcyclopentene Production

Application of co‐feeds in the catalytic conversion of light alkanes to aromatics: A comprehensive review

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