{"title":"介孔氨基功能化HKUST-1(Fe)快速吸附水中痕量汞并具有再生能力","authors":"Shuaibo Song , Zheng Chen , Dingfan Yan, Jiahao Lu, Simin Wang, Jinbo Zhang, Fang Yuan","doi":"10.1016/j.micromeso.2025.113677","DOIUrl":null,"url":null,"abstract":"<div><div>Trace Hg<sup>2+</sup> posed a serious threat to water safety. However, adsorption materials that can remove low concentration of mercury from water are still needed to be developed. In this work, amino-functionalized HKUST-1(Fe) with mesopores structure was synthesized by a one-pot method for the adsorption of trace mercury in the aqueous environment. Favorable pore conditions were beneficial for the diffusion of Hg<sup>2+</sup>. The doping of Fe<sup>3+</sup> improved the stability of the material, effectively inhibited the original metal ion leaching by 85.54 % decrease. In addition, NH<sub>2</sub>-BDC, and EDTA introduced nitrogen-containing groups to provide numerous active sites which captured Hg<sup>2+</sup> specifically. Under optimal conditions, based on the changes in the binding energies of -NH-and O-C=O, HKUST(Fe)-NH<sub>2</sub>@EDTA removed 95.45 % of Hg<sup>2+</sup> (the initial concentration as low as 10 μg L<sup>−1</sup>) within 10 min, with a maximum adsorption capacity of 1206.62 mg/g. After four adsorption-desorption cycles, it was still capable of removing 85.94 % of Hg<sup>2+</sup> with regeneration performance. Combined with the excellent selectivity and anti-interference, the composited realized the removal of Hg<sup>2+</sup> in real water samples, which meet the drinking water standards. This study provided a theoretical basis for the rapid and efficient adsorption of trace mercury in water by novel nanomaterials.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"394 ","pages":"Article 113677"},"PeriodicalIF":4.8000,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mesoporous amino-functionalized HKUST-1(Fe) for rapid adsorption of aqueous trace mercury with regeneration ability\",\"authors\":\"Shuaibo Song , Zheng Chen , Dingfan Yan, Jiahao Lu, Simin Wang, Jinbo Zhang, Fang Yuan\",\"doi\":\"10.1016/j.micromeso.2025.113677\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Trace Hg<sup>2+</sup> posed a serious threat to water safety. However, adsorption materials that can remove low concentration of mercury from water are still needed to be developed. In this work, amino-functionalized HKUST-1(Fe) with mesopores structure was synthesized by a one-pot method for the adsorption of trace mercury in the aqueous environment. Favorable pore conditions were beneficial for the diffusion of Hg<sup>2+</sup>. The doping of Fe<sup>3+</sup> improved the stability of the material, effectively inhibited the original metal ion leaching by 85.54 % decrease. In addition, NH<sub>2</sub>-BDC, and EDTA introduced nitrogen-containing groups to provide numerous active sites which captured Hg<sup>2+</sup> specifically. Under optimal conditions, based on the changes in the binding energies of -NH-and O-C=O, HKUST(Fe)-NH<sub>2</sub>@EDTA removed 95.45 % of Hg<sup>2+</sup> (the initial concentration as low as 10 μg L<sup>−1</sup>) within 10 min, with a maximum adsorption capacity of 1206.62 mg/g. After four adsorption-desorption cycles, it was still capable of removing 85.94 % of Hg<sup>2+</sup> with regeneration performance. Combined with the excellent selectivity and anti-interference, the composited realized the removal of Hg<sup>2+</sup> in real water samples, which meet the drinking water standards. This study provided a theoretical basis for the rapid and efficient adsorption of trace mercury in water by novel nanomaterials.</div></div>\",\"PeriodicalId\":392,\"journal\":{\"name\":\"Microporous and Mesoporous Materials\",\"volume\":\"394 \",\"pages\":\"Article 113677\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-05-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microporous and Mesoporous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S138718112500191X\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S138718112500191X","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
微量Hg2+对水体安全构成严重威胁。然而,能够去除水中低浓度汞的吸附材料仍有待开发。本文采用一锅法制备了具有介孔结构的氨基功能化HKUST-1(Fe),用于吸附水中痕量汞。有利的孔隙条件有利于Hg2+的扩散。Fe3+的掺杂提高了材料的稳定性,有效抑制了原始金属离子的浸出,浸出率降低了85.54%。此外,NH2-BDC和EDTA引入了含氮基团,提供了大量的活性位点,可以特异性捕获Hg2+。在最佳条件下,基于- nhh和O- c =O结合能的变化,HKUST(Fe)-NH2@EDTA在10 min内脱除了95.45%的Hg2+(初始浓度低至10 μg L−1),最大吸附量为1206.62 mg/g。经过4次吸附-解吸循环后,仍能脱除85.94%的Hg2+,并具有再生性能。结合优异的选择性和抗干扰性,该复合材料实现了对实际水样中Hg2+的去除,达到了饮用水标准。该研究为新型纳米材料对水中痕量汞的快速高效吸附提供了理论基础。
Mesoporous amino-functionalized HKUST-1(Fe) for rapid adsorption of aqueous trace mercury with regeneration ability
Trace Hg2+ posed a serious threat to water safety. However, adsorption materials that can remove low concentration of mercury from water are still needed to be developed. In this work, amino-functionalized HKUST-1(Fe) with mesopores structure was synthesized by a one-pot method for the adsorption of trace mercury in the aqueous environment. Favorable pore conditions were beneficial for the diffusion of Hg2+. The doping of Fe3+ improved the stability of the material, effectively inhibited the original metal ion leaching by 85.54 % decrease. In addition, NH2-BDC, and EDTA introduced nitrogen-containing groups to provide numerous active sites which captured Hg2+ specifically. Under optimal conditions, based on the changes in the binding energies of -NH-and O-C=O, HKUST(Fe)-NH2@EDTA removed 95.45 % of Hg2+ (the initial concentration as low as 10 μg L−1) within 10 min, with a maximum adsorption capacity of 1206.62 mg/g. After four adsorption-desorption cycles, it was still capable of removing 85.94 % of Hg2+ with regeneration performance. Combined with the excellent selectivity and anti-interference, the composited realized the removal of Hg2+ in real water samples, which meet the drinking water standards. This study provided a theoretical basis for the rapid and efficient adsorption of trace mercury in water by novel nanomaterials.
期刊介绍:
Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal.
Topics which are particularly of interest include:
All aspects of natural microporous and mesoporous solids
The synthesis of crystalline or amorphous porous materials
The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic
The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions
All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials
Adsorption (and other separation techniques) using microporous or mesoporous adsorbents
Catalysis by microporous and mesoporous materials
Host/guest interactions
Theoretical chemistry and modelling of host/guest interactions
All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.