Synthesis of a novel amorphous metal-organic framework containing rich N and S groups for efficient adsorption of Ag(I) in aqueous solutions

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Journal of Solid State Chemistry Pub Date : 2025-04-01 Epub Date: 2025-01-10 DOI:10.1016/j.jssc.2025.125193
Yingxia Ma , Miaoshi Li , Tianze Li , Haijun Yang , Ruilin Zhang , Xiaofei Ye , Wenli Meng , Xiaojun Chai , Cuixia Li
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Abstract

Industrial wastewater containing heavy metal Ag(I) causes irreversible harm to human health through food chain, necessitating effective removal methods. According to hard-soft acids-bases (HSAB) theory, nitrogen (N) and sulfur (S) functional groups form stable chelates with Ag(I). In this study, 2-amino-5-sulfanyl-1,3,4-thiadiazole (AST) with three N and two S groups served as organic ligand, and zinc nitrate hexahydrate provided metal center, novel amorphous metal-organic framework (Zn-AST) rich in N and S groups was synthesized via a one-pot solvothermal method. Batch experiments assessed the Zn-AST adsorption properties for Ag(I) in aqueous solutions. In addition, density-functional theory, frontier orbital theory, and molecular electrostatic surface potential analyses were used to elucidate the synthesis and adsorption mechanisms. The maximum adsorption capacity of Zn-AST for Ag(I) was 2932.91 mg/g. The Zn-AST exhibited good selectivity in the presence of Cu(II), Co(II), Ni(II), and Pb(II) ions, the removal rate for Ag(I) was 98.28 %, which was far higher than the values of other ions (all less than 10 %). The main adsorption mechanisms of Ag(I) by the Zn-AST involved electrostatic interactions, the formation of Ag–S bonds, and chelation between Ag and nitrogen functional groups. This study offers a viable strategy for developing unique adsorbents for Ag(I) removal from wastewater.

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一种新型富N、S基非晶态金属有机骨架的合成及其在水溶液中对银(I)的高效吸附
含重金属Ag(I)的工业废水通过食物链对人体健康造成不可逆转的危害,需要有效的去除方法。根据硬-软酸碱(HSAB)理论,氮(N)和硫(S)官能团与Ag(I)形成稳定的螯合物。本研究以具有3个N和2个S基团的2-氨基-5-磺胺基-1,3,4-噻二唑(AST)为有机配体,以六水硝酸锌为金属中心,通过一锅溶剂热法合成了富含N和S基团的新型非晶态金属-有机骨架(Zn-AST)。批量实验评估了Zn-AST在水溶液中对Ag(I)的吸附性能。此外,利用密度泛函理论、前沿轨道理论和分子静电表面势分析对其合成和吸附机理进行了分析。Zn-AST对Ag(I)的最大吸附量为2932.91 mg/g。Zn-AST在Cu(II)、Co(II)、Ni(II)和Pb(II)离子存在下表现出良好的选择性,对Ag(I)的去除率高达98.28%,远高于其他离子(均小于10%)。Zn-AST吸附Ag(I)的主要机理包括静电相互作用、Ag - s键的形成以及Ag与氮官能团的螯合作用。该研究为开发去除废水中Ag(I)的独特吸附剂提供了可行的策略。
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来源期刊
Journal of Solid State Chemistry
Journal of Solid State Chemistry 化学-无机化学与核化学
CiteScore
6.00
自引率
9.10%
发文量
848
审稿时长
25 days
期刊介绍: Covering major developments in the field of solid state chemistry and related areas such as ceramics and amorphous materials, the Journal of Solid State Chemistry features studies of chemical, structural, thermodynamic, electronic, magnetic, and optical properties and processes in solids.
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