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通过硫醇功能化的缺陷型锆基金属有机框架增强重金属离子去除的多配体策略。

Multi-ligand strategy for enhanced removal of heavy metal ions by thiol-functionalized defective Zr-MOFs.

作者信息

Zhou Yu, Xiong Jiaxing, Wang Li, Li Feng, Bai Huiping, Wang Shixiong, Yang Xiangjun

机构信息

Research Center of Lake Restoration Technology Engineering for Universities of Yunnan Province, School of Chemical Science and Technology, Yunnan University, No. 2, Cuihu North Road, Kunming 650091, China.

The Unconventional Oil and Gas Institute, China University of Petroleum-Beijing, Beijing 102200, China.

出版信息

J Hazard Mater. 2024 Nov 5;479:135723. doi: 10.1016/j.jhazmat.2024.135723. Epub 2024 Sep 3.

DOI:10.1016/j.jhazmat.2024.135723
PMID:39243545
Abstract

Given the significant global concern about heavy metal pollution, the development of effective adsorbents to capture pollutants has become an urgent issue. In this work, thiol-functionalized defective Zr-MSA-DMSA was designed by mixing 2,3-dimercaptosuccinic acid and mercaptosuccinic acid, which was applied for the rapid and efficient removal of M(II) (i.e., Pb(II), Hg(II), Cd(II)) from wastewater. Zr-MSA-DMSA exhibited excellent adsorption performance, and the maximum adsorption capacities for Pb(II), Hg(II), and Cd(II) were 715.2 mg g, 862.7 mg g, and 450.5 mg g. In actual wastewater, Zr-DMSA-MSA exhibited up to 97 % M(II) removal efficiency and excellent anti-interference ability. It also maintained good structural stability after five adsorption/regeneration cycles. Thus, the abundant oxygen vacancies and unsaturated adsorption sites on Zr-MSA-DMSA significantly improved the adsorption performance of M(II). Spectral analysis and DFT calculations confirmed that Zr-MSA-DMSA mainly relied on the coordination of sulfur and oxygen atoms, electrostatic attraction and a large number of defective sites to achieve the adsorption of M(II). Fixed bed experiments showed that Zr-MSA-DMSA exhibited a depletion time of 10500 min and a volume of 7.0 L. In summary, Zr-MSA-DMSA holds significant potential for treating heavy metal wastewater and provides potential applications for defect engineering.

摘要

鉴于全球对重金属污染的高度关注,开发有效的吸附剂来捕获污染物已成为一个紧迫的问题。在这项工作中,通过混合2,3-二巯基琥珀酸和巯基琥珀酸设计了硫醇功能化的缺陷Zr-MSA-DMSA,用于从废水中快速高效地去除M(II)(即Pb(II)、Hg(II)、Cd(II))。Zr-MSA-DMSA表现出优异的吸附性能,对Pb(II)、Hg(II)和Cd(II)的最大吸附容量分别为715.2 mg/g、862.7 mg/g和450.5 mg/g。在实际废水中,Zr-DMSA-MSA表现出高达97%的M(II)去除效率和优异的抗干扰能力。在五个吸附/再生循环后,它还保持了良好的结构稳定性。因此,Zr-MSA-DMSA上丰富的氧空位和不饱和吸附位点显著提高了对M(II)的吸附性能。光谱分析和DFT计算证实,Zr-MSA-DMSA主要依靠硫和氧原子的配位、静电吸引以及大量缺陷位点来实现对M(II)的吸附。固定床实验表明,Zr-MSA-DMSA的耗尽时间为10500分钟,体积为7.0 L。总之,Zr-MSA-DMSA在处理重金属废水方面具有巨大潜力,并为缺陷工程提供了潜在应用。

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