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具有 N 掺杂骨架和封装铁基催化剂的分级多孔纤维素基碳气凝胶,用于高效四环素催化降解。

Hierarchically porous cellulose-based carbon aerogels with N-doped skeletons and encapsulated iron-based catalysts for efficient tetracycline catalytic degradation.

机构信息

College of Polymer Science and Engineering and State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, PR China.

College of Polymer Science and Engineering and State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, PR China.

出版信息

Int J Biol Macromol. 2024 Mar;261(Pt 2):129829. doi: 10.1016/j.ijbiomac.2024.129829. Epub 2024 Jan 29.

DOI:10.1016/j.ijbiomac.2024.129829
PMID:38296134
Abstract

Three-dimensional interpenetrating and hierarchically porous carbon material is an efficient catalyst support in water remediation and it is still a daunting challenge to establish the relationship between hierarchically porous structure and catalytic degradation performance. Herein, a highly porous silica (SiO)/cellulose-based carbon aerogel with iron-based catalyst (FeO) was fabricated by in-situ synthesis, freeze-drying and pyrolysis, where the addition of SiO induced the hierarchically porous morphology and three-dimensional interpenetrating sheet-like network with nitrogen doping. The destruction of cellulose crystalline structure by SiO and the iron-catalyzed breakdown of glycosidic bonds synergistically facilitated the formation of electron-rich graphite-like carbon skeleton. The unique microstructure is confirmed to be favorable for the diffusion of reactants and electron transport during catalytic process, thus boosting the catalytic degradation performance of carbon aerogels. As a result, the catalytic degradation efficiency of tetracycline under light irradiation by adding only 5 mg of FeO/SiO cellulose carbon aerogels was as high as 90 % within 60 min, demonstrating the synergistic effect of photocatalysis and Fenton reaction. This ingenious structure design provides new insight into the relationship between hierarchically porous structure of carbon aerogels and their catalytic degradation performance, and opens a new avenue to develop cellulose-based carbon aerogel catalysts with efficient catalytic performance.

摘要

三维互穿和分级多孔碳材料是水修复中的一种高效催化剂载体,但建立分级多孔结构与催化降解性能之间的关系仍然是一个艰巨的挑战。本文通过原位合成、冷冻干燥和热解制备了一种具有铁基催化剂(FeO)的高多孔硅(SiO)/纤维素基碳气凝胶,其中 SiO 的添加诱导了具有氮掺杂的分级多孔形态和三维互穿片状网络。SiO 破坏纤维素的结晶结构,以及铁催化的糖苷键断裂协同促进了富电子石墨状碳骨架的形成。独特的微观结构有利于在催化过程中促进反应物的扩散和电子传输,从而提高碳气凝胶的催化降解性能。结果表明,在光照射下,只需添加 5mg 的 FeO/SiO 纤维素碳气凝胶,四环素的催化降解效率在 60min 内高达 90%,这证明了光催化和芬顿反应的协同效应。这种巧妙的结构设计为碳气凝胶的分级多孔结构与其催化降解性能之间的关系提供了新的见解,并为开发具有高效催化性能的纤维素基碳气凝胶催化剂开辟了新途径。

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