Elemental zoning enhances mass transport in zeolite catalysts for methanol to hydrocarbons

Le, Thuy T.; Qin, Wei; Agarwal, Ankur; Nikolopoulos, Nikolaos; Fu, Donglong; Patton, Matthew D.; Weiland, Conan; Bare, Simon R.; Palmer, Jeremy C.; Weckhuysen, Bert M.; Rimer, Jeffrey D.

doi:10.1038/s41929-023-00927-2

Title: Elemental zoning enhances mass transport in zeolite catalysts for methanol to hydrocarbons

Journal Article · 15 March 2023 · Nature Catalysis

DOI: https://doi.org/10.1038/s41929-023-00927-2 · OSTI ID:2004904

Le, Thuy T. ^[1]; Qin, Wei ^[2]; Agarwal, Ankur ^[2];

^[3]; Fu, Donglong ^[3]; Patton, Matthew D. ^[2];

^[4];

^[5]; Palmer, Jeremy C. ^[2];

^[3];

^[2]

Univ. of Houston, TX (United States); SLAC
Univ. of Houston, TX (United States)
Utrecht University (Netherlands)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Mass transport limitations in zeolite catalysts pose major hurdles for their optimal performance in diverse chemical reactions. Most approaches to reduce these restrictions focus on the synthesis of either hierarchical or nanosized zeolites. Here we demonstrate that the existence of a siliceous, catalytically inactive exterior rim on ZSM-5 particles dramatically reduces the diffusion limitations, which leads to an enhanced catalyst lifetime for the methanol-to-hydrocarbon reaction. In this study, our findings reveal that binary inorganic and organic structure-directing agents enable a one-pot synthesis of Si-zoned ZSM-5 catalysts with diffusion properties that are characteristic of particles with a much smaller size. Operando ultraviolet–visible light diffuse reflectance spectroscopy reveals a marked reduction in external coking among Si-zoned samples. Molecular dynamics simulations to assess the diffusion of methanol and benzene in siliceous pores and in those with Brønsted acids reveal substantially reduced transport limitations in zoned regions, consistent with the improved catalyst activity of Si-zoned zeolites relative to that of ZSM-5 with a homogeneous acid-site distribution.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-76SF00515; SC0014468; SC0012704

OSTI ID:: 2004904

Alternate ID(s):: OSTI ID: 2339459

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 3 Vol. 6; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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