Synthesis of γ-Valerolactone through coupling of methyl levulinate hydrogenation with aqueous phase reforming of methanol over Pt/CoxAl catalyst

Q3 Energy 燃料化学学报 Pub Date : 2024-09-01 DOI:10.1016/S1872-5813(24)60453-6
LÜ Zexiang , ZHU Shanhui , DONG Mei , QIN Zhangfeng , FAN Weibin , WANG Jianguo
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Abstract

The synthesis of high-value γ-valerolactone (GVL) from biomass-derived methyl levulinate (ML) conventionally requires a high-pressure hydrogen, which incurs significant costs and safety concerns. This study proposes an innovative approach to produce GVL by integrating ML hydrogenation with aqueous phase reforming of methanol (APRM) using Pt/CoxAl catalysts, thereby eliminating the need for an external hydrogen source. The influence of catalyst composition, methanol concentration, and reaction temperature on catalytic performance has been carefully examined. The results suggest that Pt/Co1Al demonstrated exceptional activity, yielding up to 98.2% GVL, and maintaining stable performance over multiple cycles. Characterization results revealed that Pt0 facilitates both APRM and ML hydrogenation, while Brønsted acid sites catalyze the hydrolysis of ML and lactonization of intermediates. The synergy between Pt0 and Brønsted acid sites is essential for GVL formation. The appropriate amount of Co not only enhances Pt dispersion but also increases Brønsted acid sites, thereby boosting catalytic efficiency. This work offers a sustainable and economically feasible strategy for transforming biomass derivatives into valuable fuels and chemicals.

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在 Pt/CoxAl 催化剂上通过乙酰丙酸甲酯加氢与甲醇水相重整耦合合成 γ-戊内酯
从生物质衍生的乙酰丙酸甲酯(ML)合成高价值的γ-戊内酯(GVL)传统上需要高压氢气,这产生了巨大的成本和安全问题。本研究提出了一种生产 GVL 的创新方法,即使用 Pt/CoxAl 催化剂将 ML 加氢与甲醇水相重整(APRM)结合起来,从而无需外部氢源。我们仔细研究了催化剂组成、甲醇浓度和反应温度对催化性能的影响。结果表明,Pt/Co1Al 表现出卓越的活性,GVL 收率高达 98.2%,并在多次循环中保持稳定的性能。表征结果表明,Pt0 可促进 APRM 和 ML 的氢化,而布氏酸位点则可催化 ML 的水解和中间产物的内酯化。Pt0 和布氏酸位点之间的协同作用对 GVL 的形成至关重要。适量的 Co 不仅能增强铂的分散性,还能增加布氏硬度酸位点,从而提高催化效率。这项研究为将生物质衍生物转化为有价值的燃料和化学品提供了一种可持续且经济可行的策略。
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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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