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Journal of Materials Chemistry A · 2015 ·Vol. 3 ·期 21 ·11587-11595 · IF 7.443

A designable magnetic MOF composite and facile coordination-based post-synthetic strategy for the enhanced removal of Hg2+ from water

Lijin Huang,Man He,Beibei Chen,Bin Hu

A magnetic MOF composite was successfully prepared by a novel and green strategy through reasonable design. The nano Fe3O4@SiO2 core was first coated by a shell of Cu(OH)2 as the self-template, followed by a conversion of Cu(OH)2 into HKUST-1 at room temperature in a water–ethanol mixture solvent, and Fe3O4@SiO2@HKUST-1 core–shell nanostructures were obtained successfully. Based on this, a Bi-I-functionalized-magnetic HKUST-1 composite was prepared through a flexible coordination-based post-synthetic strategy. Powder X-ray diffraction spectrometry, N2 sorption–desorption isotherms and Fourier transform infrared spectroscopy were used for the characterization of the magnetic MOF composites. The core–shell morphology was confirmed by transmission electron microscope images and the result of thermogravimetric analysis showed that the magnetic composites had excellent thermal stability. Besides, the adsorption of Hg2+ on Fe3O4@SiO2, Fe3O4@SiO2@HKUST-1 and Bi-I-functionalized magnetic MOF composites was investigated, and a good adsorption selectivity of Bi-I-functionalized magnetic MOF composites towards Hg2+ was demonstrated, with high adsorption capacity (264 mg g−1) and fast adsorption dynamics. The Bi-I-functionalized magnetic HKUST-1 composite was then successfully employed for the selective removal of Hg2+ from water, demonstrating great potential application of the prepared magnetic MOF composite as a fascinating adsorbent in environmental monitoring.

CAS / MDL: 7787-64-6 554-95-0
研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2021 · IF 8.067

Novel sulfhydryl functionalized covalent organic frameworks for ultra-trace Hg2+ removal from aqueous solution

Fei Pan,Chunyi Tong,Zhaoyang Wang,Fenghua Xu,Xiaofei Wang,Baicheng Weng,Dawei Pan,Rilong Zhu

Two kinds of novel sulfhydryl functionalized covalent organic frameworks were fabricated as adsorbents for the removal of ultra-trace concentrations of Hg 2+ from water. The two kinds of sulfhydryl functionalized covalent organic frameworks were obtained via a thiol-ene click reaction between the thiol groups of trithiocyanuric acid (TTC) or bismuththiol (BMT) and vinyl groups on the surface of covalent organic frameworks. The material structure was characterized by XRD, SEM, EDS, FT-IR, BET, and TG analysis. Due to their rich sulfur content, both adsorbents (COF-SH-1 and COF-SH-2) exhibited a high level of selective Hg 2+ removal from aqueous solution with maximum adsorption capacities of 763.4 mg g −1 and 526.3 mg g −1 , respectively. Furthermore, in the presence of ultra-low concentrations of Hg 2+ both materials exhibited excellent performance, achieving rapid Hg 2+ removal at concentrations from 10 μg L −1 to less than 0.02 ng L −1 . Analysis of the adsorption mechanism indicates that the sulfur containing chelating groups exhibit a strong binding capacity for Hg 2+ . Results show that the structure determines the performance, with the amount of adsorption sites being related to the adsorption capacity. Therefore, as sulfhydryl functionalized covalent organic frameworks contain an abundance of adsorption sites, these materials can effectively achieve the removal of ultra-low trace Hg 2+ concentrations and have promising future application potential for the environmental detection of heavy metals.

研究领域: 环境科学 · 材料科学
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EUROPEAN POLYMER JOURNAL · 2024 · IF 5.8

Thiophene network polyamides (TPPA) with tri(4-aminophenyl)benzene: Synthesis and removal of Hg2+ from aqueous solution

Chaoji Xiong,Kejie Li,Chunzhi Peng,Xingmao Zhang,Kun Liang,Wei Wu,Qian Chen

In this study, the thiophenyl polyamide ( TPPA ) derived from tri(4-aminophenyl) benzene was synthesized for the removal of Hg 2+ from the aqueous solution. The adsorbent was characterized by the Fourier transform infrared spectroscopy, x-ray photoelectron spectroscopy, scanning electron microscopy, nitrogen adsorption–desorption, thermogravimetric analysis and differential scanning calorimetry. The adsorption capacity of Hg 2+ is 518.7 mg g −1 at a dose of 1.1 g/L of adsorbent. TPPA was shown to have the following advantages: (i) the high selectivity for the excess metal ions Hg 2+ , (ii) the stability in the pH values ranging between 2 and 6, and (iii) the proper recyclability (87 % of Hg 2+ can be removed in 5 adsorption–desorption cycles). Our analysis suggests the models of the pseudo-second-order kinetics and the Langmuir isotherm are suitable for the description of the adsorption of Hg 2+ on the thiophene network polyamide. Our experimental and theoretical results reveal the relationship between the structures and the adsorption capacities of TPPA , identifying the oxygen atom (amide) and the sulphur atom (thiophene) as the most important chemical-reaction sites.

研究领域: 材料科学 · 环境科学
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 14 ·5159-5166 · IF 8.262

A mercapto functionalized magnetic Zr-MOF by solvent-assisted ligand exchange for Hg2+ removal from water

Lijin Huang,Man He,Beibei Chen,Bin Hu

A facile preparation of magnetic MOF composites with flexible mercapto group pendants in their pores is realized through solvent-assisted ligand exchange (SALE) under mild conditions in water, and terephthalate in UIO-66 is replaced with mercaptoacetic acid (MAA). After the SALE processing, the crystallinity, porosity, and superparamagnetism of the mercapto functionalized magnetic Zr-MOF (MFC-S) are well maintained, and the obtained MFC-S exhibits a higher adsorption capacity (282 mg g−1) for Hg2+ than that of the magnetic Zr-MOF (MFC-O). Furthermore, the prepared MFC-S can be regenerated easily by liquid desorption after adsorption of metal ions and be reused more than 5 times without obvious decrease in removal performance. The proposed SALE method for the preparation of mercapto functionalized magnetic MOF composites (MFCs) is easy-to-operate and low cost, providing not only a reliable porous MFC platform for the removal of metal ions, but also a simple and efficient synthesis route for the preparation of functionalized MFCs which cannot be achieved through conventional approaches.

研究领域: 材料科学 · 环境科学 · 化学工程
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Highly Efficient Magnetic Nitrogen-Doped Porous Carbon Prepared by One-Step Carbonization Strategy for Hg2+ Removal from Water

Lijin Huang,Man He,Bei-bei Chen,Qian Cheng,Bin Hu

Hydrophilic magnetic N-doped porous carbon composites (MNPCs) with high special surface areas and rich nitrogen content was prepared via simple one-step carbonization of zinc oxide nanoparticles (ZnO NPs), 2-methylimidazole (HmIm), and Fe3O4@SiO2 magnetic nanoparticles (MNPs) mixture directly. During the carbonization process, ZnO NPs directly reacts with HmIm to yield porous ZIF-8 while the MNPs are incorporated into the frameworks to generate magnetic metal–organic frameworks (MFCs), and the MFCs acts as a self-sacrificing template to prepare MNPC. The obtained MNPCs via simple one-step carbonization strategy display higher adsorption capacity (429 mg g–1) for Hg2+ ions than MNPC-T700-M3-T (382 mg g–1) which was obtained by two-step synthesis strategy for comparison. It also exhibits very fast adsorption dynamics (adsorption rate constant (K2) = 2.45 g mg–1 min–1) for Hg2+ and could efficiently remove 95% Hg2+ in 2 min for 20 mg L–1 Hg2+ solution. Furthermore, the prepared MNPC exhibits good chemical stability and the adsorption capacity is still more than 95% even after 10 adsorption–elution cycles. The proposed method is easy-processing and economic, which not only provides highly efficient MNPCs for metal ions capture but also paves the ways toward various MFCs with different ligands through solvent/additive-free synthesis approaches.

CAS / MDL: 1314-13-2
研究领域: 材料科学 · 环境科学 · 化学工程
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Materials Today Chemistry · 2023 · IF 7.3

Hg2+ removal from wastewater by anchoring nitrogen/sulfur active center onto metal-organic framework via Schiff-base reaction: Synthesis, characterization, and experiment

W. Ruan,H. Wu,H. Yang

Remediation of Hg 2+ pollution in wastewater is imminent. Herein, a Metal-Organic Framework hybrid Uio-DBD-x was designed and synthesized via rational introducing the 5-Diamino-1,4-benzenedithiol Dihydrochloride (DBD) molecule onto parent Uio-66-NH 2 . By optimizing the synthesis conditions, the material exhibited better adsorption performance when x = 1. The characteristics including crystallinity, morphology, and pore size were analyzed. 12.64 nm for pore diameter and 493.73 m 2 /g for surface areas of Uio-DBD-1 were obtained. Subsequently, the adsorption performance of Uio-DBD-1 towards Hg 2+ was studied under different pH, dosage, concentration, and time. The corresponding maximum adsorption capacity of 423.10 mg/g and equilibrium time of 10 min was achieved. Remarkably, Hg 2+ concentration could be reduced below the emission limit (0.05 mg/L). Furthermore, the selectivity and reusability of the adsorbent were investigated, and the results manifested that Uio-DBD-1 maintains high removal efficiency (82.10%) after 6 times recycles. The possible adsorption mechanism could be ascribed to the strong interaction (chelation, proton exchange, and coordination) between Hg 2+ and –NH 2 /-SH groups. This work breaks new ground in functional material design and paves the way for wastewater treatment.

CAS / MDL: 68-12-2 10026-11-6
研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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