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磺化共价三嗪基框架作为将纤维二糖水解为葡萄糖的催化剂。

Sulfonated covalent triazine-based frameworks as catalysts for the hydrolysis of cellobiose to glucose.

作者信息

Artz Jens, Delidovich Irina, Pilaski Moritz, Niemeier Johannes, Kübber Britta Maria, Rahimi Khosrow, Palkovits Regina

机构信息

Chair of Heterogeneous Catalysis & Chemical Technology Institut für Technische und Makromolekulare Chemie, RWTH Aachen University Worringerweg 2 52074 Aachen Germany

DWI Leibniz-Institut für Interaktive Materialien Forckenbeckstr. 50 52074 Aachen Germany.

出版信息

RSC Adv. 2018 Jun 19;8(40):22392-22401. doi: 10.1039/c8ra04254c.

Abstract

Covalent triazine-based frameworks (CTFs) were synthesized in large scale from various monomers. The materials were post-synthetically modified with acid functionalities gas-phase sulfonation. Acid capacities of up to 0.83 mmol g at sulfonation degrees of up to 10.7 mol% were achieved. Sulfonated CTFs exhibit high specific surface area and porosity as well as excellent thermal stability under aerobic conditions (>300 °C). Successful functionalization was verified investigating catalytic activity in the acid-catalyzed hydrolysis of cellobiose to glucose at 150 °C in HO. Catalytic activity is mostly affected by porosity, indicating that mesoporosity is beneficial for hydrolysis of cellobiose. Like other sulfonated materials, S-CTFs show low stability under hydrothermal reaction conditions. Recycling of the catalyst is challenging and significant amounts of sulfur leached out of the materials. Nevertheless, gas-phase sulfonation opens a path to tailored solid acids for application in various reactions. S-CTFs form the basis for multi-functional catalysts, containing basic coordination sites for metal catalysts, tunable structural parameters and surface acidity within one sole system.

摘要

基于共价三嗪的框架材料(CTFs)由各种单体大规模合成。这些材料通过酸官能团进行后合成修饰——气相磺化。在磺化度高达10.7 mol%时,酸容量达到0.83 mmol/g。磺化的CTFs具有高比表面积和孔隙率,以及在有氧条件下(>300°C)优异的热稳定性。通过在150°C的水中研究其在酸催化纤维二糖水解为葡萄糖反应中的催化活性,验证了功能化的成功。催化活性主要受孔隙率影响,表明中孔结构有利于纤维二糖的水解。与其他磺化材料一样,S-CTFs在水热反应条件下稳定性较低。催化剂的循环利用具有挑战性,并且有大量硫从材料中浸出。尽管如此,气相磺化为定制用于各种反应的固体酸开辟了一条途径。S-CTFs构成了多功能催化剂的基础,在单一体系中包含金属催化剂的碱性配位位点、可调节的结构参数和表面酸度。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3c57/9081118/3826bed56c24/c8ra04254c-s1.jpg

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