C60改性疏水催化剂上玉米秸秆生物质合成气制备储氢液体燃料的研究

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-20 DOI:10.1021/acssuschemeng.4c09852
Gaofeng Chen, Zhiwei Wang, Na Guo, Lei Liu, Huina Zhu, Qun Wang, Tingzhou Lei
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引用次数: 0

摘要

醇类燃料是一类重要的储氢液体燃料,具有广阔的发展潜力。醇基储氢液体燃料可以有效地从生物质衍生合成气(CO和H2)中生产。在通过高精醇合成(HAS)反应将合成气转化为醇方面已经做了相当大的努力。然而,不可避免地会产生大量的H2O和C1副产物(CO2和CH4)。本研究设计了富勒烯(C60,一种全碳笼分子)修饰的疏水CoCuSNT@C60催化剂,以阻止H2O和C1副产物的形成。疏水C60缩短了活性位点界面上H2O的滞留,抑制了水气移位反应。这导致二氧化碳的产生显著减少,同时CO的转化率和对醇的选择性增加。通过x射线衍射、傅里叶变换红外光谱、N2吸附-脱附等温线、x射线光电子能谱、扫描电镜和透射电镜对该疏水CoCuSNT@C60催化剂进行了表征。与未改性的CoCuSNT相比,c60改性的疏水CoCuSNT@C60催化剂具有更高的CO加氢活性和高醇选择性,以及长达350 h的稳定性,可满足工业应用。
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Preparation of Hydrogen Storage Liquid Fuel by Biomass-Based Syngas from Corn Straw over a C60 Modified Hydrophobic Catalyst
Alcohols, being a substantial category of hydrogen storage liquid fuels, exhibit promising development potential. Alcohol-based hydrogen storage liquid fuels can be efficiently produced from biomass-derived syngas (CO and H2). Considerable efforts have been made in the conversion of syngas to alcohols through a higher alcohol synthesis (HAS) reaction. However, inevitably, there will be significant generation of H2O and C1 byproducts (CO2 and CH4). In this study, a hydrophobic CoCuSNT@C60 catalyst modified with fullerene (C60, an all-carbon cage molecule) was designed to hinder the formation of H2O and C1 byproducts. The hydrophobic C60 shortened the retention of H2O on the active site interface, restraining the water–gas shift reaction. This leads to a significant decrease in CO2 generation, accompanied by an increase in the CO conversion and selectivity toward alcohols. The hydrophobic CoCuSNT@C60 catalyst was characterized by X-ray diffraction, Fourier transform infrared spectra, N2 adsorption–desorption isotherms, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy. Compared to the unmodified CoCuSNT, the C60-modified hydrophobic CoCuSNT@C60 catalyst possesses higher CO hydrogenation activity and high alcohol selectivity, along with an impressive stability of up to 350 h to meet industrial applications.
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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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