Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Zhang, Yanfei; Qi, Liang; Li, Yuting; Yang, Tingshu; Meira, Debora M.; Dun, Chaochao; Hu, Haocheng; Chen, Huihui; Xu, Shutao; Urban, Jeffrey J.; Sadow, Aaron D.; Kobayashi, Takeshi; Qi, Long; Tian, Peng; Bell, Alexis T.

doi:10.1021/acscatal.4c03935

Title: Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Journal Article · 02 October 2024 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.4c03935 · OSTI ID:2475776

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^[3]; Yang, Tingshu ^[4]; Meira, Debora M. ^[5];

^[6]; Hu, Haocheng ^[7]; Chen, Huihui ^[7]; Xu, Shutao ^[7];

^[6];

^[3]; Kobayashi, Takeshi ^[3];

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Dalian Maritime University (China); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Chinese Academy of Sciences (CAS), Dalian (China). Dalian Institute of Chemical Physics; Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Chinese Academy of Sciences (CAS), Dalian (China). Dalian Institute of Chemical Physics; Univ. of California, Berkeley, CA (United States)
Ames Lab., and Iowa State Univ., Ames, IA (United States)
Dalian Maritime University (China)
Univ. of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
Chinese Academy of Sciences (CAS), Dalian (China). Dalian Institute of Chemical Physics
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Biomass-derived ethanol (EtOH) and acetaldehyde (AcH) conversion to 1,3-butadiene (1,3-BD) is an alternative process for 1,3-BD production. The present investigation reports the preparation and characterization of isolated La sites introduced into the silanol nests in DeAlBEA as well as detailed studies of the mechanism and kinetics for the conversion of an EtOH-AcH mixture to 1,3-BD. La sites supported on DeAlBEA are found to be present as (≡SiO)₂La-OH groups that are H-bonded with adjacent Si-OH groups, possessing high C-C coupling activity and stability, superior to state-of-the-art Y-DeAlBEA. La sites supported on silica (La-SiO₂) with a similar chemical structure but no H-bonding interaction with Si-OH groups were prepared for comparison. Lewis acid La sites promote AcH aldol condensation, and the activity of such sites is nearly identical for both La-DeAlBEA and La-SiO₂. Further, the rate of C₄ product formation increases by a factor of 4.8 upon addition of EtOH to the feed of AcH over La-DeAlBEA, whereas that over La/SiO₂ remains unchanged. Investigation of the mechanism and kinetics of AcH aldol condensation and EtOH-AcH conversion to 1,3-BD revealed two C-C bond forming pathways-AcH aldol condensation by Lewis acid La sites and direct coupling of EtOH-AcH over H-bonded (≡SiO)₂La-OH···HO-Si≡ sites. This study provides important information about the role of the local environment of isolated Lewis acid sites and their effects on the direct coupling of EtOH and AcH to form 1,3-BD.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC02-05CH11231; AC02-07CH11358; AC02-06CH11357

OSTI ID:: 2475776

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 20 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

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