Investigation on the catalysis performance of metal-doped zeolites on ring-opening acidolysis reaction

Huo, Fanglin; Liu, Zhendong; Liu, Zhendong; Lu, Yangcheng

doi:10.1016/j.cej.2023.143029

Cited by 6 publications

(4 citation statements)

References 52 publications

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“…The small figures in Figure a reveal that the LUMO on the silicate (011) surface were localized primarily around the O atom within a narrow spatial range, whereas the LUMO on the Zr-MFI (011) surface predominantly localized within a substantial range surrounding the Zr atom. The XPS characterization results supports the notion that the incorporation of Zr enhances the Lewis acidity of the zeolite …”

Section: Resultssupporting

confidence: 76%

“…The simulation calculations of the proton affinity of BAS and LAS on zeolite revealed that BAS exhibits a higher proton affinity, thereby playing a more positive role during the reaction process. Due to the facile adjustment of the acidic strength and acid distribution through doping other elements into zeolite, − the incorporation of metal dopants at framework sites in zeolites holds significant implications for designing novel catalysts with tailored activity. − Zhou et al prepared zeolite catalysts loaded with different metals (Zr, Ga, Mo, Co) using impregnation method for propane dehydrogenation reaction. It was found that the total acid content and B/L ratio of the catalyst exhibited varying degrees of decrease after metal loading.…”

Section: Introductionmentioning

confidence: 99%

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One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂

Gao,

Lv,

Qian

et al. 2024

Ind. Eng. Chem. Res.

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Solid acid will be an ecofriendly and efficient catalyst for the hydrolysis of polyethylene terephthalate (PET). Very highly Zr-doped MFIstructured zeolites as catalysts for PET hydrolysis were successfully synthesized for the first time. Comprehensive characterizations confirmed the successful incorporation of Zr into the framework. To comprehend the role of Zr within the framework, density functional calculations were employed to investigate its impact on the surface properties and hydrolysis processes. The results demonstrated that Zr d-orbitals enhance Lewis acidity of the catalyst by contributing to the formation of zeolite's lowest unoccupied molecular orbitals. The interaction between the model molecule and the catalyst surface was enhanced by doping Zr, leading to electron redistribution toward the surface direction on the carbonyl oxygen of model molecule. Consequently, the carbonyl carbon developed a partial positive charge, and the hydrolysis reaction was promoted. The experimental results validated that the Zr-doped catalyst exhibited a 64% enhancement in the reaction rate.

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Section: Resultssupporting

confidence: 76%

Section: Introductionmentioning

confidence: 99%

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂

Gao,

Lv,

Qian

et al. 2024

Ind. Eng. Chem. Res.

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“…We postulate the slow heating rate and extended treatment at 823 K are needed to ensure sufficient time for (CH 3 ) 2 SnCl 2 to diffuse throughout the pores of Si-BEA and to react to yield Sn atoms within tetrahedral positions of the *BEA framework. Notably, Sn atoms can form oxide clusters during this process, which can be alleviated by introducing a prepyrolysis treatment in an inert environment (i.e., Ar, N 2 ). , Ti- and Zr-BEA were prepared by liquid-phase metal incorporation based on previously reported procedures. , Si-BEA was heated in a round-bottom flask under vacuum (<5 Pa, 473 K) for 2 h to create a moisture-free environment. Dichloromethane (CH 2 Cl 2 , Fisher Chemicals, 20 cm 3 g zeolite –1 ) solvent was then added to the flask for Ti-BEA, and isopropanol (C 2 H 7 OH, Fisher Chemicals, 20 cm 3 g zeolite –1 ) was added for Zr-BEA.…”

Section: Methods and Materialsmentioning

confidence: 99%

“…Notably, Sn atoms can form oxide clusters during this process, which can be alleviated by introducing a prepyrolysis treatment in an inert environment (i.e., Ar, N 2 ). 67,68 Ti-and Zr-BEA were prepared by liquid-phase metal incorporation based on previously reported procedures. 35,42 Si-BEA was heated in a round-bottom flask under vacuum (<5 Pa, 473 K) for 2 h to create a moisture-free environment.…”

Section: Methodsmentioning

confidence: 99%

Understanding Rates and Regioselectivities for Epoxide Methanolysis within Zeolites: Mechanism and Roles of Covalent and Non-covalent Interactions

Potts,

Komar,

Locht

et al. 2023

ACS Catal.

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Rates and selectivities for liquid-phase reactions depend on the structure and acidity of active sites within zeolite catalysts and the solvent environment surrounding the active sites. Here, we demonstrate and explain the effects of these interactions on the ring-opening of 1,2-epoxybutane (C 4 H 8 O) with methanol (CH 3 OH) in acetonitrile (CH 3 CN) solvent over *BEA zeolites by varying the identity of the catalytically active element within the framework (Al, Sn, Ti, Zr) and composition of the fluid. Molecular interpretations of kinetics show that the nucleophilic attack to C 4 H 8 O determines product formation rates at sites saturated by C 4 H 8 O-or CH 3 OH-derived intermediates and favors the production of terminal ethers. Among Lewis acid catalysts, turnover rates increase with exponential dependence upon C 4 H 8 O adsorption enthalpies, measured by liquid-phase isothermal titration calorimetry, which reflects covalent and non-covalent interactions. The activation enthalpies for ring-opening and C 4 H 8 O adsorption enthalpies are least endothermic in CH 3 CN and become more endothermic with the addition of CH 3 OH. Greater concentrations of CH 3 OH increase regioselectivities toward the terminal alcohol due to the enrichment of CH 3 OH near active sites and preferential stabilization of transition states by non-covalent interactions (e.g., hydrogen bonding). These findings demonstrate opportunities to leverage cooperative inner-and outer-sphere interactions to control rates and regioselectivities of zeolite-catalyzed ring opening reactions and guide strategies to create desired products.

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Porous Materials for the Heterogeneously Catalyzed Synthesis of High Value‐Added Products: Latest Trends and Future Prospects

Sanoja‐López,

Luque

2024

Chemistry An Asian Journal

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Heterogeneous catalysis currently stands as a foundational area in materials synthesis and applied chemistry. In this context, emphasizing the significance of heterogeneous catalysis in expediting chemical reactions and controlling the formation of desired products using porous materials represents an intriguing approach in the current technological landscape. This work delves into the synthesis and design of a variety of porous materials, encompassing microporous, mesoporous and macroporous materials (e.g. carbonaceous materials, metal oxides, MOFs, zeolites and functionalized analogues), alongside their properties and characteristics pivotal in heterogeneous catalysis. among others, and their subsequent modification, underscoring the significance of tailoring porous materials for specific catalytic applications.

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Investigation on the catalysis performance of metal-doped zeolites on ring-opening acidolysis reaction

Cited by 6 publications

References 52 publications

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂

Understanding Rates and Regioselectivities for Epoxide Methanolysis within Zeolites: Mechanism and Roles of Covalent and Non-covalent Interactions

Porous Materials for the Heterogeneously Catalyzed Synthesis of High Value‐Added Products: Latest Trends and Future Prospects

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Investigation on the catalysis performance of metal-doped zeolites on ring-opening acidolysis reaction

Cited by 6 publications

References 52 publications

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO2

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO2

Understanding Rates and Regioselectivities for Epoxide Methanolysis within Zeolites: Mechanism and Roles of Covalent and Non-covalent Interactions

Porous Materials for the Heterogeneously Catalyzed Synthesis of High Value‐Added Products: Latest Trends and Future Prospects

Contact Info

Product

Resources

About

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂

One-Step Synthesized Solid Acid Catalyst with High Zr Content for Efficient and Green PET Degradation in Supercritical CO₂