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由二硫化钴催化纤维素制备甲基戊酸酯:晶面(111)的重要性。

Production of methyl levulinate from cellulose over cobalt disulfide: The importance of the crystal facet (111).

机构信息

Joint International Research Laboratory of Biomass Energy and Materials, Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing, Jiangsu 210037, China.

Department of Chemistry, Shantou University Medical College, Shantou, Guangdong 515041, China.

出版信息

Bioresour Technol. 2022 Mar;347:126436. doi: 10.1016/j.biortech.2021.126436. Epub 2021 Nov 27.

DOI:10.1016/j.biortech.2021.126436
PMID:34848331
Abstract

The conversion of cellulose to platform chemicals has attracted much attention because of its renewability. This work proposed an earth-abundant cobalt disulfide as a heterogeneous catalyst for methyl levulinate production from cellulose. The highest yield of methyl levulinate reached 61 mol% under the tested conditions of 200 °C, 2 MPa initial pressure, 0.45 catalyst/cellulose mass ratio, and 3 h reaction time. The XRD and TEM analyses demonstrated the crystal facet (111) of cobalt disulfide as a robust active site, which was in good agreement with the highest acidity of the crystal facet (111) calculated by the work functions. The XPS characterization showed that the main chemical valence of cobalt disulfide responsible for the methyl levulinate production was the surface Co species. This study is valuable for the development of a recoverable catalyst for the cellulose to methyl levulinate process.

摘要

纤维素转化为平台化学品因其可再生性而备受关注。本工作提出了一种丰富的地球元素——二硫化钴作为纤维素制备甲基戊酸酯的非均相催化剂。在 200°C、2 MPa 初始压力、0.45 催化剂/纤维素质量比和 3 h 反应时间的测试条件下,甲基戊酸酯的最高收率达到 61 mol%。XRD 和 TEM 分析表明,二硫化钴的晶面(111)是一个稳定的活性位,这与晶面(111)的功函数计算出的最高酸度非常吻合。XPS 表征表明,二硫化钴中负责生成甲基戊酸酯的主要化学价态是表面 Co 物种。这项研究对于开发可回收的纤维素制备甲基戊酸酯的催化剂具有重要意义。

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引用本文的文献

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Alkyl Levulinates and 2-Methyltetrahydrofuran: Possible Biomass-Based Solvents in Palladium-Catalyzed Aminocarbonylation.烷基戊内酯和 2-甲基四氢呋喃:钯催化氨甲酰化反应中可能的基于生物质的溶剂。
Molecules. 2023 Jan 3;28(1):442. doi: 10.3390/molecules28010442.