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在功能化的Pt/deAl-β沸石催化剂上由蔗糖催化生产1,2-丙二醇。

Catalytic production of 1,2-propanediol from sucrose over a functionalized Pt/deAl-beta zeolite catalyst.

作者信息

Wang Shizhuo, Jiang Jikang, Gu Minyan, Gao Feng, Shen Zheng

机构信息

National Facility Agriculture Engineering Technology Research Center, Institute of New Rural Development, Tongji University Shanghai 201804 China

State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University Shanghai 200092 China

出版信息

RSC Adv. 2023 Jan 3;13(1):734-741. doi: 10.1039/d2ra07097a. eCollection 2022 Dec 19.

Abstract

To eliminate the dependence on fossil fuels and expand the applications of biomass conversion, an efficient Pt/deAl-beta@Mg(OH) catalyst was designed, with dealuminated beta zeolite loaded with Pt as the core and Mg(OH) as the shell. The catalyst was used to produce 1,2-propanediol (1,2-PDO) from sucrose. The preparation and reaction conditions of the catalyst were optimized. The optimal yield of 1,2-PDO was 33.5% when the conditions were 20 h of dealumination, 3.0 wt% Pt loading, 5.0 wt% Mg(OH), 200 mg of catalyst, 10 mL (11.25 mg mL) of sucrose solution, an initial H pressure of 6 MPa, 200 °C, and 3 h. The core-shell structure of the modified beta zeolite shows good stability, yielding more than 30.0% after three cycles of reuse. Firstly, the molecular zeolite can host more acid sites after dealumination by concentrated nitric acid and this can prolong the catalyst's service life. Secondly, the loading of Pt increases the distribution of acid sites and improves the shape selectivity of the catalyst. The introduction of alkali produces many alkaline sites, inhibits the occurrence of side reactions, and increases the product yield. The above modification methods increase the production of 1,2-PDO by promoting isomerization between glucose and fructose from sucrose hydrolysis and the reverse aldol condensation (RAC) reaction. This paper provides a theoretical basis and reference route for applying biomass conversion technology in practical production, which is of great significance for developing biomass resources into high-value-added chemical products.

摘要

为消除对化石燃料的依赖并扩大生物质转化的应用,设计了一种高效的Pt/deAl-beta@Mg(OH)催化剂,以负载Pt的脱铝β沸石为核,Mg(OH)为壳。该催化剂用于由蔗糖生产1,2-丙二醇(1,2-PDO)。对催化剂的制备和反应条件进行了优化。当脱铝20小时、Pt负载量为3.0 wt%、Mg(OH)为5.0 wt%、催化剂200 mg、蔗糖溶液10 mL(11.25 mg/mL)、初始氢气压力6 MPa、200℃和反应3小时的条件下,1,2-PDO的最佳产率为33.5%。改性β沸石的核壳结构显示出良好的稳定性,在三次重复使用循环后产率超过30.0%。首先,分子沸石经浓硝酸脱铝后可容纳更多酸性位点,这可延长催化剂的使用寿命。其次,Pt的负载增加了酸性位点的分布并提高了催化剂的择形性。碱的引入产生了许多碱性位点,抑制了副反应的发生并提高了产物产率。上述改性方法通过促进蔗糖水解产生的葡萄糖和果糖之间的异构化以及逆羟醛缩合(RAC)反应来提高1,2-PDO的产量。本文为生物质转化技术在实际生产中的应用提供了理论依据和参考路线,这对于将生物质资源开发成高附加值化学产品具有重要意义。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6658/9808589/d39037181393/d2ra07097a-f1.jpg

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