利用三氟乙酸 (TFA) 通过效率结构缺陷定制 PET 衍生 Sn-MOFs 性能的水基简便绿色合成路线

IF 5.5 3区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of the Taiwan Institute of Chemical Engineers Pub Date : 2024-09-10 DOI:10.1016/j.jtice.2024.105754
Thi-Hong Nguyen, Kung-Yuh Chiang
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引用次数: 0

摘要

背景金属有机框架(MOFs)的合成越来越注重实现绿色、低成本的方法,同时生产出具有丰富活性位点的高质量产品。这种方法正引起研究人员的极大关注。其中一种很有前景的方法--调制合成法,因其能够诱导 MOFs 结构缺陷并增强其活性位点而脱颖而出。然而,在确定关键因素的最佳条件,特别是调制剂与影响 MOFs 性能的关键独立变量之间的定量相关性方面存在挑战,这凸显了该领域研究工作的重要性。采用水热法,利用类水溶剂和三氟乙酸(TFA)作为调节剂,有效地诱导结构缺陷。研究发现,温度、反应时间和 TFA 浓度对 Sn-MOFs 的性能有显著影响,凸显了 TFA 在通过缺陷工程创造活性位点、提高 Sn-MOFs 表面积和孔体积方面的巨大潜力。Sn-MOFs 的最佳合成条件包括温度为 148℃,反应时间为 24 小时,H2BDC/TFA 的摩尔比为 1.7,产率为 98.51 ± 1.47%,CI 为 80.21 ± 1.32%,且检测不到残留的 H2BDC。所制备的 Sn-MOF-150 具有高热稳定性和化学稳定性、丰富的功能基团以及由球形纳米颗粒组成的独特分层纳米结构等特点。这些发现进一步强调了通过关键参数优化和缺陷工程技术合成 Sn-MOF 的有效性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Tailoring properties of PET-derived Sn-MOFs through efficiency structure defects using trifluoroacetic acid (TFA) with water-based facile and green synthesis route

Background

The synthesis of Metal-Organic Frameworks (MOFs) is increasingly focused on achieving green and cost-efficient methods while producing high-quality products with abundant active sites. This approach is attracting significant attention from researchers. One promising method, modulated synthesis, stands out for its ability to induce structural defects in MOFs and enhance their active sites. However, the challenges in identifying the optimal conditions for critical factors, particularly the quantitative correlation between the modulator and crucial independent variables influencing MOFs performance, underscore the importance of research work in this field.

Methods

This study synthesized tin-based MOFs (Sn-MOFs) utilizing a linker derived from recycled polyethylene terephthalate (PET) waste. A hydrothermal approach was employed, utilizing water-like solvents and trifluoroacetic acid (TFA) as a modulator to effectively induce structural defects. Response Surface Methodology (RSM) was applied to evaluate the effects and interactions of temperature, reaction time, and TFA concentration on optimizing yield and crystalline index (CI) while simultaneously reducing the residual percentage of 1,4-benzene dicarboxylate (H2BDC) in the Sn-MOFs (DI).

Significant findings

The research revealed that temperature, reaction time, and TFA concentration significantly influenced the performance of Sn-MOFs, highlighting the considerable potential of TFA in creating active sites and enhancing the surface area and pore volume of Sn-MOFs through defect engineering. Optimal synthesis conditions for Sn-MOFs included a temperature of 148℃, a reaction time of 24 h, and a molar ratio of H2BDC/TFA of 1.7, yielding 98.51 ± 1.47 % for yield and 80.21 ± 1.32 % for CI, with no detectable residual H2BDC. The resulting Sn-MOF-150 exhibited characteristics such as high thermal and chemical stability, abundant function groups, and a unique hierarchical nanostructure composed of spherical nanoparticles. These findings further emphasize the efficacy of the synthesis approach for Sn-MOF through critical parameter optimization and defect engineering techniques.

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来源期刊
CiteScore
9.10
自引率
14.00%
发文量
362
审稿时长
35 days
期刊介绍: Journal of the Taiwan Institute of Chemical Engineers (formerly known as Journal of the Chinese Institute of Chemical Engineers) publishes original works, from fundamental principles to practical applications, in the broad field of chemical engineering with special focus on three aspects: Chemical and Biomolecular Science and Technology, Energy and Environmental Science and Technology, and Materials Science and Technology. Authors should choose for their manuscript an appropriate aspect section and a few related classifications when submitting to the journal online.
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