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| 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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| S-NISHIMURA-T-0526-5.pdf | | 1074Kb | Adobe PDF | View/Open |
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