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巯基功能化共价三嗪框架用于选择性汞去除。

Thio-groups decorated covalent triazine frameworks for selective mercury removal.

机构信息

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092, PR China.

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092, PR China; School of Energy and Environment, City University of Hong Kong, Tat Chee Avenue, Kowloon, 999077, Hong Kong, China.

出版信息

J Hazard Mater. 2021 Feb 5;403:123702. doi: 10.1016/j.jhazmat.2020.123702. Epub 2020 Aug 15.

Abstract

Covalent triazine frameworks (CTFs) as a kind of covalent organic framework (COF) materials show great potential for practical application by virtue of their high stability and facile large-scale synthesis. In this work, we developed three CTFs (MSCTF-1, MSCTF-2, and xSCTF-2) of different pore size decorated with S-groups using different functionalization methods for achieving selective Hg removal from aqueous solutions. The material structures were comprehensively studied by gas adsorption, IR and XPS, etc. Among them, the MSCTF-2 with 24.45% S content showed the highest Hg adsorption capacity of 840.5 mg g, while MSCTF-1 exhibiting much larger distribution coefficient of 1.67 × 10 mL g renders an exceptionally high efficiency for reducing the concentration of Hg contaminated water to less than 0.03 μg L. Moreover, the MSCTFs show distinct features of: (i) high selectivity toward Hg over various transition metal ions; (ii) high stability over a wide pH range from pH 1 to 12; and (iii) good recyclability with 94% of Hg removal over five consecutive cycles. The Hg adsorption on functionalized CTFs followed pseudo-second-order kinetics and Langmuir isotherm. Our results revealed the material structure-performance relationship that the adsorption capacities depend on the binding site density whereas the distribution coefficient is essential to the removal efficiency.

摘要

共价三嗪框架(CTFs)作为一种共价有机框架(COF)材料,由于其高稳定性和易于大规模合成,在实际应用中具有很大的潜力。在这项工作中,我们使用不同的功能化方法开发了三种不同孔径的 CTFs(MSCTF-1、MSCTF-2 和 xSCTF-2),并用 S 基团进行了修饰,以实现从水溶液中选择性去除 Hg。通过气体吸附、IR 和 XPS 等方法对材料结构进行了全面研究。其中,S 含量为 24.45%的 MSCTF-2 具有最高的 Hg 吸附容量 840.5 mg g,而 MSCTF-1 的分配系数高达 1.67×10 mL g,对 Hg 污染水的浓度降低到 0.03μg L 以下具有极高的效率。此外,MSCTFs 还具有以下特点:(i)对各种过渡金属离子具有高选择性;(ii)在 pH 值为 1 至 12 的宽范围内具有高稳定性;(iii)在五个连续循环中具有 94%的 Hg 去除率,具有良好的可回收性。Hg 在功能化 CTFs 上的吸附遵循准二级动力学和 Langmuir 等温线。我们的结果揭示了材料结构-性能关系,即吸附容量取决于结合位点密度,而分配系数对去除效率至关重要。

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