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采用混合表面活性剂合成富含硅醇的 MCM-48 及其在丙酮吸附中的应用:平衡、动力学和热力学研究。

Synthesis of Silanol-Rich MCM-48 with Mixed Surfactants and Their Application in Acetone Adsorption: Equilibrium, Kinetic, and Thermodynamic Studies.

机构信息

Tianjin Key Lab of Indoor Air Environmental Quality Control, School of Environmental Science and Technology, Tianjin University, Tianjin, 300350, China.

State Key Laboratory of Engines, Tianjin University, Tianjin, 300350, China.

出版信息

Langmuir. 2020 Oct 6;36(39):11528-11537. doi: 10.1021/acs.langmuir.0c01933. Epub 2020 Sep 17.

DOI:10.1021/acs.langmuir.0c01933
PMID:32883083
Abstract

Mesoporous silica MCM-48 with rich silanol was prepared using polyvinylpyrrolidone (PVP) and cetyltrimethylammonium bromide (CTAB) as mixed templates, and the dynamic adsorption performance of acetone was evaluated by testing breakthrough curves. The mixed micelle formed by CTAB and PVP, as well as the hydrogen bond between the carbonyl group of PVP and silanol group affected the condensation process of Si-OH group during the formation of mesoporous structure, resulting in the increase of Si-OH group number on the surface of MCM-48. Compared with MCM-48 synthesized by single template (CTAB), the acetone adsorption capacity of MCM-48 (1:3) synthesized by mixed templates (PVP:CTAB = 1:3) improved by 23.86%, which was attributed to the increase of silanol group amount and the decrease of pore size. In addition, Bangham model had the highest goodness of fit to describe the adsorption process among four kinetic models for the adsorbents, conforming to the mechanism of pore diffusion. The Langmuir and Freundlich models were used to fit the adsorption isotherm data, and the Freundlich model could better describe the adsorption of acetone. Freundlich model fitting results showed that MCM-48 with rich silanol had a strong affinity for acetone, and the adsorption of acetone on MCM-48 belonged to multilayer adsorption. The thermodynamic results showed that the adsorption of MCM-48 for acetone was physical adsorption, and the adsorption behavior was exothermic. This work provided insight into how the inherent properties of an adsorbent and environmental factors (including initial concentration and adsorption temperature) affected the adsorption performance of ketones, thus more ideas could be provided for the accurate design of adsorbents. Furthermore, silanol-rich MCM-48 synthesized by mixed templates is expected to be a promising adsorbent for acetone removal.

摘要

采用十六烷基三甲基溴化铵(CTAB)和聚乙烯吡咯烷酮(PVP)为混合模板剂制备了富含硅醇的介孔硅 MCM-48,并通过测试穿透曲线评估了其对丙酮的动态吸附性能。CTAB 和 PVP 形成的混合胶束以及 PVP 中的羰基与硅醇基团之间的氢键影响了介孔结构形成过程中 Si-OH 基团的缩合过程,导致 MCM-48 表面的 Si-OH 基团数量增加。与单模板剂(CTAB)合成的 MCM-48 相比,混合模板剂(PVP:CTAB=1:3)合成的 MCM-48(1:3)的丙酮吸附量提高了 23.86%,这归因于硅醇基团数量的增加和孔径的减小。此外,在四种动力学模型中,Bangham 模型对吸附剂吸附过程的拟合度最高,符合孔扩散机制。Langmuir 和 Freundlich 模型用于拟合吸附等温线数据, Freundlich 模型可以更好地描述丙酮的吸附。Freundlich 模型拟合结果表明,富含硅醇的 MCM-48 对丙酮具有很强的亲和力,丙酮在 MCM-48 上的吸附属于多层吸附。热力学结果表明,MCM-48 对丙酮的吸附为物理吸附,吸附行为为放热。这项工作深入了解了吸附剂的固有性质和环境因素(包括初始浓度和吸附温度)如何影响酮类的吸附性能,从而为准确设计吸附剂提供了更多思路。此外,预计富含硅醇的混合模板合成的 MCM-48 有望成为一种有前途的丙酮去除吸附剂。

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