Journal
JOURNAL OF ENERGY CHEMISTRY
Volume 71, Issue -, Pages 411-417Publisher
ELSEVIER
DOI: 10.1016/j.jechem.2022.02.047
Keywords
Hydrogenation; Biomass; Metal organic framework; Biorefinery
Funding
- National Key R&D Program of China [2020YFA0710000]
- National Natural Science Foundation of China [22122901, 21902047]
- Provincial Natural Science Foundation of Hunan [2020JJ5045, 2021JJ20024, 2021RC3054]
- Shenzhen Science and Technology Program [JCYJ20210324140610028]
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In this study, a catalytic material with strong Lewis acidic-basic and Brønsted acidic-basic sites was successfully prepared by introducing sulfonic groups onto UIO-66. The material exhibited excellent catalytic performance in the selective catalytic transfer hydrogenation of furfural to furfuryl alcohol.
The highly selective catalytic transfer hydrogenation (CTH) of furfural (FF) to furfuryl alcohol (FOL) is a significant route of biomass valorization. Herein, a series microporous Zr-metal organic framework (ZrMOF) functionalized by sulfonic groups are prepared. Based on the comprehensive structural characterizations by means of X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N-2 physisorption, Thermogravimetric (TG) and Fourier transformed infrared spectroscopy (FTIR), we find that sulfonic acid (-SO3H) functional groups are tethered on the UIO-66 without affecting the structure of the framework. Systematic characterizations (NH3-TPD, CO2-TPD, and in-situ FTIR) demonstrate that modifying of sulfonic groups on UIO-66 results in the formation of stronger Lewis acidic-basic and Bronsted acidis sites. The cooperative role of the versatile Lewis acidic-basic and Bronsted acidic sites in 60% mol fraction of sulfonic acid-containing UIO-66 (UIO-S0.6) retain high surface area and exhibit excellent catalytic performance of 94.7% FOL yield and 16.9 h(-1) turnover number (TOF) under mild conditions. Kinetic experiments reveal that the activation energy of the CTH of furfural (FF) over UIO-S0.6 catalyst is as low as 50.8 kJ mol-1. Besides, the hydrogen transfer mechanism is investigated through isotope labeling experiments, exhibiting that the b-H in isopropanol is transferred to the a-C of FF by forming six-membered intermediates on the Lewis acidic-basic and Bronsted acidic sites of the UIO-S0.6, which is the rate-determining step in the formation of FOL. (C) 2022 The Author(s). Published by Elsevier B.V. on behalf of King Saud University. All rights reserved.
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