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Temperature-dependent synthesis of dimethyl ether (DME) from methanol over beta zeolite: a novel approach to a sustainable fuel.

ABSTRACT: Crystalline beta zeolite molecular sieve with SiO₂/Al₂O₃ molar ratio of 28.5 was synthesized by the hydrothermal crystallization method and examined for methanol dehydration reaction. The micro-mesoporous beta zeolite was active between 280 and 450°C. Dimethyl ether (DME) was observed as the predominant product at all reaction temperatures, with a maximum selectivity of 47.9% at 300°C and a methanol turnover frequency (TOF_MeOH) of 741.9 h^-1. At increased reaction temperatures, beta zeolite showed enhanced strong acid site fraction, promoting higher hydrocarbon formation following the olefin-based cycle. It was revealed that the crystallinity, porosity and acidity of beta zeolite change in the reaction environment. Amorphous carbon deposition occurred on beta zeolite, which involved a loss in crystallinity to some extent. The temperature increase showed a pore-broadening phenomenon at elevated temperature regions. Regeneration cycle testing demonstrated beta zeolite activity maintained stable throughout a 280 h time-on-stream period.

SUBMITTER: Chaudhary PK

PROVIDER: S-EPMC10445025 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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Temperature-dependent synthesis of dimethyl ether (DME) from methanol over beta zeolite: a novel approach to a sustainable fuel.

Chaudhary Puneet Kumar PK Arundhathi Racha R Kasture Mahesh W MW Samanta Chanchal C Vankayala Rakesh R Thota Chiranjeevi C

Royal Society open science 20230823 8

Crystalline beta zeolite molecular sieve with SiO2/Al2O3 molar ratio of 28.5 was synthesized by the hydrothermal crystallization method and examined for methanol dehydration reaction. The micro-mesoporous beta zeolite was active between 280 and 450°C. Dimethyl ether (DME) was observed as the predominant product at all reaction temperatures, with a maximum selectivity of 47.9% at 300°C and a methanol turnover frequency (TOFMeOH) of 741.9 h-1. ...[more]

PMID: 37621656

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Project description:Control of the spatial proximity of Brønsted acid sites within the zeolite framework can result in materials with properties that are distinct from materials synthesized through conventional crystallization methods or available from commercial sources. Recent experimental evidence has shown that turnover rates of different acid-catalyzed reactions increase with the fraction of proximal sites in chabazite (CHA) zeolites. The catalytic conversion of oxygenates is an important research area, and the dehydration of methanol to dimethyl ether (DME) is a well-studied reaction as part of methanol-to-olefin chemistry catalyzed by solid acids. Published experimental data have shown that DME formation rates (per acid site) increase systematically with the fraction of proximal acid sites in the six-membered ring of CHA. Here, we probe the effect of acid site proximity in CHA on methanol dehydration rates using electronic structure calculations and microkinetic modeling to identify the primary causes of this chemistry and their relationship to the local structure of the catalyst at the nanoscale. We report a density functional theory-parametrized microkinetic model of methanol dehydration to DME, catalyzed by acidic CHA zeolite with direct comparison to experimental data. Effects of proximal acid sites on reaction rates were captured quantitatively for a range of operating conditions and catalyst compositions, with a focus on total paired acid site concentration and reactant clustering to form higher nuclearity complexes. Next-nearest neighbor paired acid sites were identified as promoting the formation of methanol trimer clusters rather than the inhibiting tetramer or pentamer clusters, resulting in large increases in the rate for DME production due to the lower energy barriers present in the concerted methanol trimer reaction pathway. The model framework developed in this study can be extended to other zeolite materials and reaction chemistries toward the goal of rational design and development of next-generation catalytic materials and chemical processes.

Dataset Information

Temperature-dependent synthesis of dimethyl ether (DME) from methanol over beta zeolite: a novel approach to a sustainable fuel.

Publications

Temperature-dependent synthesis of dimethyl ether (DME) from methanol over beta zeolite: a novel approach to a sustainable fuel.

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