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Please use this identifier to cite or link to this item: http://hdl.handle.net/10119/19045

Title: Genesis of Bi-functional Acid-Base Site on Cr-supported Layered Double Hydroxide Catalyst Surface for One-pot Synthesis of Furfurals from Xylose with Solid Acid Catalyst
Authors: Shirotori, Mahiro
Nishimura, Shun
Ebitani, Kohki
Issue Date: 2016-10-03
Publisher: Royal Society of Chemistry
Magazine name: Catalysis Science & Technology
Volume: 6
Number: 23
Start page: 8200
End page: 8211
DOI: 10.1039/C6CY01426G
Abstract: Cr-supported Mg-Al layered double hydroxide (Cr/Mg-Al LDH) composed bi-functional Lewis acid – Brønsted base activesites on the catalyst surface at close boundaries between Cr3+ oxide and Mg-Al LDH. These proceeded to efficient aldose–ketose isomerization. The combined use of solid Brønsted acid Amberlyst-15 and bi-functional acid–base Cr/Mg-Al LDH exhibits higher activity for one-pot transformation of xylose into furfural via aldose–ketose isomerization and successive dehydration under mild conditions than the activity shown by basic bare Mg-Al LDH, substituted Mg-Cr LDH, and Lewis acidic Cr3+ supported catalysts with Amberlyst-15. Correlation between the activity and the Cr loading amount for Mg-Al LDH was evaluated using several characterizations and MPV reduction as a model reaction for Lewis acidity investigation. Results show the following: (1) The monomer of Lewis acidic Cr3+ oxide is supported on the Mg-Al LDH surface below 1 wt%. (2) Thereafter, Cr3+ species form Lewis acidic small Cr3+ oxide dimer and/or trimer up to 5 wt%. Then they cover the Mg-Al LDH surface to generate highly active bi-functional Lewis acid – Brønsted base sites. (3) Above 5 wt%, the excess Cr3+ species generate inert Mg-Cr and/or Mg-Al-Cr LDH like composites. These deposit on some active sites, leading to decreased activity. Results show that the furfural yields vary significantly in accordance with Cr loadings, and the 5wt%Cr/Mg-Al LDH achieves the highest value (59% yield, 18 h) because the most effective interaction between the Lewis acidic Cr3+ oxide and Mg-Al LDH basic site is produced at 5 wt% Cr loading.
Rights: Copyright (C) 2016 Royal Society of Chemistry. Mahiro Shirotori, Shun Nishimura and Kohki Ebitani, Catalysis Science & Technology, 2016, 6(23), 8200-8211. https://doi.org/10.1039/C6CY01426G - Reproduced by permission of the Royal Society of Chemistry
URI: http://hdl.handle.net/10119/19045
Material Type: author
Appears in Collections:d10-1. 雑誌掲載論文 (Journal Articles)

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