Zeolite-Tailored Active Site Proximity for the Efficient Production of Pentanoic Biofuels
He, Jiang; Wu, Zhijie; Gu, Qingqing; Liu, Yuanshuai; Chu, Shenqi; Chen, Shaohua; Zhang, Yafeng; Yang, Bing; Chen, Tiehong; Wang, Aiqin; Weckhuysen, Bert M; Zhang, Tao; Luo, Wenhao
(2021) Angewandte Chemie-International Edition, volume 60, issue 44, pp. 23713 - 23721
(Article)
Abstract
Biofuel production can alleviate reliance on fossil resources and thus carbon dioxide emission. Hydrodeoxygenation (HDO) refers collectively to a series of important biorefinery processes to produce biofuels. Here, well-dispersed and ultra-small Ru metal nanoclusters (ca. 1 nm), confined within the micropores of zeolite Y, provide the required active site intimacy,
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which significantly boosts the chemoselectivity towards the production of pentanoic biofuels in the direct, one-pot HDO of neat ethyl levulinate. Crucial for improving catalyst stability is the addition of La, which upholds the confined proximity by preventing zeolite lattice deconstruction during catalysis. We have established and extended an understanding of the “intimacy criterion” in catalytic biomass valorization. These findings bring new understanding of HDO reactions over confined proximity sites, leading to potential application for pentanoic biofuels in biomass conversion.
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Keywords: bifunctional catalysis, biomass conversion, hydrodeoxygenation, proximity, zeolites, Taverne, Catalysis, General Chemistry
ISSN: 1433-7851
Publisher: John Wiley and Sons Ltd
Note: Funding Information: The National Key R&D Program of China (2018YFB1501602), National Natural Science Foundation of China (21721004, 21703238 and 22078316) are acknowledged for financial support. Z.Wu and S.Chu acknowledges the support of Science Foundation of China University of Petroleum, Beijing (ZX20200125) and National Key Research and Development Project (2017YFA0403401) respectively. B.Yang acknowledges the support of the National Natural Science Foundation of China (21872145) and the Foundation of Dalian Institute of Chemical Physics (DICP I201943). Dr. Rui Chen, Dr. Xiaoli Pan, Yang Su are acknowledged for the XPS and STEM measurements, respectively. We thank Xiaoge Bai from Tianjin Xianquan Instrument Co. for the assistance with FTIR experiments. Dr. Lu Lin and Prof. Feng Wang are also acknowledged for the editing of the figures and fruitful discussion. Publisher Copyright: © 2021 Wiley-VCH GmbH
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