功能化共价有机框架材料对水体中汞离子的吸附性能研究

doi:10.19741/j.issn.1673-4831.2022.0736

Abstract

Abstract: In this study, amino and mercapto functional groups were introduced to design the surface of covalent organic framework materials (COFs), and COFs were prepared and applied to adsorb mercury ions in water. It was characterized by X-ray diffraction, Fourier transform infrared spectroscopy and scanning electron microscope, respectively. The concentration of mercury ions in aqueous solution after adsorption with COFs was measured by atomic fluorescence spectrometer, the experimental data were fitted by adsorption isotherm and kinetic model to explore the adsorption performance of the material under different conditions. According to the data, when the mercury ion concentration was 600 mg·L^-1, the adsorption amount reached the maximum of 587.6 mg·g^-1. The adsorption rate remains above 95% in the range of pH 1-10. The reaction can reach the adsorption equilibrium state within 1 min. In the solution with multiple ions coexisting, the adsorption rate of mercury ions can still reach to 66%. The study of adsorption process proved that the adsorption fit the pseudo-second-order kinetic model and Langmuir adsorption isotherm. It is a kind of easy reaction chemical adsorption. Therefore, COFs materials have good development potential in the field of adsorption and separation of heavy metal ions from water environment.

Key words: covalent organic framework materials, mercury ions, water environment, adsorption properties

CLC Number:

X703

LU Su-fen, ZHANG Gao-rong, WU Li-juan, YANG Mei-feng, LU Jun-yu. Adsorption Properties of Functional Covalent Organic Framework Materials for Mercury Ions in Water[J]. Journal of Ecology and Rural Environment, 2023, 39(8): 1059-1066.

References

[1] ABDELDAYEM R.A Preliminary Study of Heavy Metals Pollution Risk in Water[J].Applied Water Science,2019,10(6):2682-2687.
[2] BAIMENOV A Z,BERILLO D A,MOUSTAKAS K,et al.Efficient Removal of Mercury (Ⅱ) from Water by Use of Cryogels and Comparison to Commercial Adsorbents under Environmentally Relevant Conditions[J].Journal of Hazardous Materials,2020,399:123056.
[3] 刘亚平,葛文超,毕文杰,等.聊城市城区水体汞砷含量分布特征及其健康风险评价研究[J].环境科学与管理,2019,44(5):52-56.[LIU Ya-ping,GE Wen-chao,BI Wen-jie,et al.Distribution Characteristics and Health Risk Assessment of Mercury and Arsenic Concentrations in Lake and Rivers of Liaocheng Urban Area[J].Environmental Science and Management,2019,44 (5):52-56.]
[4] UDHAYAKUMARI D.Review on Fluorescent Sensors-based Environmentally Related Toxic Mercury Ion Detection[J].Journal of Inclusion Phenomena and Macrocyclic Chemistry,2022,102(5/6):451-476.
[5] ZHANG R Q,WU F C,GIESY J P.Tissue-Based Assessment of Hazard Posed by Mercury and Selenium to Wild Fishes in Two Shallow Chinese Lakes[J].Environmental Science and Pollution Research,2019,26(16):159 89-15999.
[6] 鲁秀国,肖凡昊,郑宇佳,等.两种改性核桃壳材料对水中Hg²⁺的吸附研究[J].离子交换与吸附,2021,37(3):220-233.[LU Xiu-guo,XIAO Fan-hao,ZHENG Yu-jia,et al.Adsorption of Hg²⁺ by Two Kinds of Modified Walnut Shells in Aqueous Solution[J].Ion Exchange and Adsorption,2021,37(3):220-233.]
[7] SAITO H.Congenital Minamata Disease:A Description of Two Cases in Niigata[J].Neuro Toxicology,2020,81:360-363.
[8] 李远征.华东地区印染企业废水中汞污染现状评估及原因分析[J].染料与染色,2020,57(3):58-61.[LI Yuan-zheng.Current Assessment and Root Cause Analysis of Mercury in the Effluent of Dyeing and Printing Factories in Eastern China[J].Dyestuffs and Coloration,2020,57(3):58-61.]
[9] 陈若思,刘定富,武晓阳.红枫湖沉积物中汞污染评价[J].贵州化工,2012,37(4):40-42.[CHEN Ruo-si,LIU Ding-fu,WU Xiao-yang.An Assessment of Mercuury Pollution in Sediments of Hongfeng Lake[J].Guizhou Chemical Industry,2012,37(4):40-42.]
[10] 唐帮成,王仲如,龙小青,等.贵州万山汞矿区农用水体汞污染情况调查[J].环境工程,2015,33(S1):673-675.[TANG Bang-cheng,WANG Zhong-ru,LONG Xiao-qing,et al.Investigation of Mercury as Pollutant in Agricultural Water in the Zooms of Wanshan Mecury Mine,Guizhou Province[J].Environmental Engineering,2015,33(S1):673-675.]
[11] 孙悦,周晓馨,楼子墨,等.铁基纳米材料功能化及对水中汞离子的去除[J].化学进展,2016,28(8):1156-1169.[SUN Yue,ZHOU Xiao-xin,LOU Zi-mo,et al.Functionalized Iron-based Nano-materials for Removal of Mercury from Aqueous Solution[J].Progress in Chemistry,2016,28(8):1156-1169.]
[12] WANG Y J,BAO S Y,LIU Y Q,et al.CoS₂/GO Nanocomposites for Highly Efficient and Ppb Level Adsorption of Hg(Ⅱ) from Wastewater[J].Journal of Molecular Liquids,2021,322:114899
[13] QIAN H L,WANG Y,YAN X P.Covalent Organic Frameworks for Environmental Analysis[J].TrAC Trends in Analytical Chemistry,2022,147:116516.
[14] 刘桂梅,曾玉彬,彭梦娇,等.强化混凝-吸附耦合法对气田水中汞的去除研究[J].水处理技术,2020,46(7):16-19.[LIU Gui-mei,ZENG Yu-bin,PENG Meng-jiao,et al.Removal of Mercury in Gas Field Water by Enhanced Coagulation-adsorption Coupled Method[J].Technology of Water Treatment,2020,46(7):16-19.]
[15] HUA K,XU X L,LUO Z P,et al.Effective Removal of Mercury Ions in Aqueous Solutions:A Review[J].Current Nanoscience,2020,16 (3):363-375.
[16] HU X L,CHEN C H,ZHANG D W,et al.Kinetics,Isotherm and Chemical Speciation Analysis of Hg(Ⅱ) Adsorption over Oxygen-Containing MXene Adsorbent[J].Chemosphere,2021,278:130206.
[17] PANDA A,YANG Y Q,VENKATESWARLU S,et al.Highly Durable Covalent Organic Framework for the Simultaneous Ultrasensitive Detection and Removal of Noxious Hg²⁺[J].Microporous and Mesoporous Materials,2020,306:110399.
[18] 郭冀峰,孙亚晶,马煜萱.新型磁性共价有机框架材料的合成及其应用研究进展[J].安全与环境学报,2023,23(3):911-918.[GUO Ji-feng,SUN Ya-jing,MA Yu-xuan.Reviews on Application in Environment and Synthesis of New Magnetic Covalent Organic Framework Materials[J].Journal of Safety and Environment,2023,23(3):911-918.]
[19] 商林杰,刘江,兰亚乾.共价有机框架材料用于光/电催化CO₂还原的研究进展[J].应用化学,2022,39(4):559-584.[SHANG Lin-jie,LIU Jiang,LAN Ya-qian.Covalent Organic Framework Materials for Photo/Electrocatalytic Carbon Dioxide Reduction[J].Chinese Journal of Applied Chemistry,2022,39(4):559-584.]
[20] 张关印,关清卿,庙荣荣,等.共价有机骨架材料的合成及应用[J].材料导报,2021,35(13):13215-13226.[ZHANG Guan-yin,GUAN Qing-qing,MIAO Rong-rong,et al.Synthesis and Application of Covalent Organic Frameworks[J].Materials Reports,2021,35(13):13215-13226.]
[21] 李诗宇,阴永光,史建波,等.共价有机框架在水中二价汞吸附去除中的应用[J].化学进展,2022,34(5):1017-1025.[LI Shi-yu,YIN Yong-guang,SHI Jian-bo,et al.Application of Covalent Organic Frameworks in Adsorptive Removal of Divalent Mercury from Water[J].Progress in Chemistry,2022,34(5):1017-1025.]
[22] 马蕴杰,丁思文,张成格,等.共价有机骨架材料(COFs)对Cr(Ⅵ)的吸附行为分析[J].功能材料,2021,52(6):6195-6199.[MA Yun-jie,DING Si-wen,ZHANG Cheng-ge,et al.Adsorption Behavior of Cr (Ⅵ) on Covalent Organic Frameworks (COFs)[J].Journal of Functional Materials,2021,52(6):6195-6199.]
[23] TAO Y,XIONG X H,XIONG J B,et al.High-performance Removal of Mercury Ions (Ⅱ) and Mercury Vapor by SO_3--Anchored Covalent Organic Framework[J].Journal of Solid State Chemistry,2020,282:121126.
[24] MERÍBOFÍ L,ROYUELA S,ZAMORA F,et al.Thiol Grafted Imine-Based Covalent Organic Frameworks for Water Remediation through Selective Removal of Hg(Ⅱ)[J].Journal of Materials Chemistry A,2017,5(34):17973-17981.
[25] LU X F,JI W H,YUAN L,et al.Preparation of Carboxy-Functionalized Covalent Organic Framework for Efficient Removal of Hg²⁺ and Pb²⁺ from Water[J].Industrial & Engineering Chemistry Research,2019,58(38):17660-17667.
[26] SUN Q.AGUILA B,PERMAN J,et al.Postsynthetically Modified Covalent Organic Frameworks for Efficient and Effective Mercury Removal[J].Journal of the American Chemical Society,2017,139(7):2786-2793.
[27] SEYFI H Z,RAHIMI R,SHAYEGAN H,et al.Removal of Hg²⁺ Heavy Metal Ion Using a Highly Stable Mesoporous Porphyrinic Zirconium Metal-organic Framework[J].Inorganica Chimica Acta,2020,501:119264.
[28] 彭灿伟,汪莉,陈受惠.二维片层卟啉基共价有机框架材料修饰电极用于污水中汞离子的高灵敏检测[J].分析化学,2022,50(3):356-364.[PENG Can-wei,WANG Li,CHEN Shou-hui.Two-Dimensional Lamellar Porphyrin-based Covalent-organic Framework Modified Electrode for Highly Sensitive Detection of Mercury Ions in Sewage[J].Chinese Journal of Analytical Chemistry,2022,50(3):356-364.]
[29] XIONG Y Y,LI J Q,GONG L L,et al.Using MOF-74 for Hg²⁺ Removal from Ultra-low Concentration Aqueous Solution[J].Journal of Solid State Chemistry,2017,246:16-22.
[30] HUANG L J,SHEN R J,LIU R Q,et al.Thiol-Functionalized Magnetic Covalent Organic Frameworks by a Cutting Strategy for Efficient Removal of Hg²⁺ from Water[J].Journal of Hazardous Materials,2020,392:122320.
[31] PAN F,TONG C,WANG Z,et al.Novel Sulfhydryl Functionalized Covalent Organic Frameworks for Ultra-trace Hg²⁺ Removal from Aqueous Solution[J].Journal of Materials Science & Technology,2021.
[32] HUANG N,ZHAI L P,XU H,et al.Stable Covalent Organic Frameworks for Exceptional Mercury Removal from Aqueous Solutions[J].Journal of the American Chemical Society,2017,139(6):2428-2434.
[33] CUI W R,JIANG W,ZHANG C R,et al.Regenerable Carbohydrazide-Linked Fluorescent Covalent Organic Frameworks for Ultrasensitive Detection and Removal of Mercury[J].ACS Sustainable Chemistry & Engineering,2020,8(1):445-451.
[34] CHANDRA S,KUNDU T,DEY K,et al.Interplaying Intrinsic and Extrinsic Proton Conductivities in Covalent Organic Frameworks[J].Chemistry of Materials,2016,28(5):1489-1494.
[35] BISWAL B P,CHANDRA S,KANDAMBETH S,et al.Mechanochemical Synthesis of Chemically Stable Isoreticular Covalent Organic Frameworks[J].Journal of the American Chemical Society,2013,135(14):5328-5331.
[36] LI Y,WANG C,MA S J,et al.Fabrication of Hydrazone-linked Covalent Organic Frameworks Using Alkyl Amine as Building Block for High Adsorption Capacity of Metal Ions[J].ACS Applied Materials & Interfaces,2019,11(12):11706-11714.
[37] WU X H,WANG D Z,ZHANG S Y,et al.Investigation of Adsorption Behaviors of Cu(Ⅱ),Pb(Ⅱ),and Cd(Ⅱ) from Water Onto the High Molecular Weight Poly(Arylene Ether Sulfone) with Pendant Carboxyl Groups[J].Journal of Applied Polymer Science,2015,132(20):41984.
[38] LI G L,WANG S X,WU Q R,et al.Mechanism Identification of Temperature Influence on Mercury Adsorption Capacity of Different Halides Modified Bio-chars[J].Chemical Engineering Journal,2017,315:251-261.
[39] LI C Y,YAN Y Y,ZHANG Q Z,et al.Adsorption of Cd²⁺ and Ni²⁺ from Aqueous Single-metal Solutions on Graphene Oxide-chitosan-Poly(Vinyl Alcohol) Hydrogels[J].Langmuir:the ACS Journal of Surfaces and Colloids,2019,35(13):4481-4490.
[40] 谢婧如,陈本寿,张进忠,等.巯基改性海泡石吸附水中的Hg(Ⅱ)[J].环境科学,2016,37(6):2187-2194.[XIE Jing-ru,CHEN Ben-shou,ZHANG Jin-zhong,et al.Adsorption of Hg(Ⅱ) in Water by Sulfydryl-modified Sepiolite[J].Environmental Science,2016,37(6):2187-2194.]
[41] 邵爱云,程德义,代静玉,等.巯基改性稻壳炭对水中Cd²⁺的吸附特性[J].生态与农村环境学报,2019,35(8):1071-1079.[SHAO Ai-yun,CHENG De-yi,DAI Jing-yu,et al.Characteristics of Cd²⁺ Adsorption from Water by Sulfhydryl Group Modified Rice Hull Biochar[J].Journal of Ecology and Rural Environment,2019,35(8):1071-1079.]
[42] 李正龙,周咏春,李海波,等.巯基改性生物炭对镉污染土壤的稳定化效果[J].环境工程,2022,40(9):143-149,157.[LI Zheng-long,ZHOU Yong-chun,LI Hai-bo,et al.Stabilization of cadmium-contaminated Soil by Sulfhydryl Modified Biochar[J].Environmental Engineering,2022,40(9):143-149,157.]
[43] 狄冠丞,周强,陶信,等.掺硫介孔炭的制备及其汞脱除特性[J].化工进展,2022,41(5):2761-2769.[DI Guan-cheng,ZHOU Qiang,TAO Xin,et al.Preparation of Sulfur-doped Mesoporous Carbon and Its Mercury Removal[J].Chemical Industry and Engineering Progress,2022,41(5):2761-2769.]
[44] 贾里,李泽鹏,郭晋荣,等.多元金属定向修饰的改性生物焦微观特性及单质汞脱除性能研究[J].环境科学学报,2021,41(8):3100-3111.[JIA Li,LI Ze-peng,GUO Jin-rong,et al.Study on the Micro-characteristics and Elemental Mercury Removal Performance of Biochar Doped by Multi-Metal Directional Modification[J].Acta Scientiae Circumstantiae,2021,41 (8):3100-3111.]
[45] 张永强,贾里,乔晓磊,等.腐殖酸定向修饰Ce-Co铁基生物焦汞吸附机理[J].中国环境科学,2021,41 (12):5522-5530.[ZHANG Yong-qiang,JIA Li,QIAO Xiao-lei,et al.The Adsorption Mechanism of Humic Acid Directional Modification Ce-Co Modified Iron-based Biochar Mercury[J].China Environmental Science,2021,41 (12):5522-5530.]

Adsorption Properties of Functional Covalent Organic Framework Materials for Mercury Ions in Water

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	ZHEN Ling, XIE Rong-rong, SHI Cheng-chun, LIU Ji-hui, JIANG Hua, LI Jia-bing, CHEN Jin, TIAN Kai-di. Study on Water Quality Variation and the Influencing Factors of Near-dam Section of Shuikou Reservoir in Summer [J]. Journal of Ecology and Rural Environment, 2023, 39(7): 943-953.
[2]	LIU Zhuang, LIU Ai-ping, ZHUANG Wei, ZHANG Li, HE Fei, XIE Yu-feng, HANG Xiao-shuai, GAO Ji-xi. Use of TMDL for Reference and Flow-Chat of Management of Water Pollution Volume Control in China [J]. Journal of Ecology and Rural Environment, 2016, 32(1): 47-52.
[3]	JIANG Xin, XU Shi-Guo, LIAN Jian-Jun, MENG Qing-Guo. Analysis and Calculation of Dynamic Water Environmental Capacity of Rivers in North China [J]. Journal of Ecology and Rural Environment, 2013, 29(4): 409-414.
[4]	WU Xue-Fei, LIU Lu-Jia, MA Han, LIU Yang, ZHOU Ming-Yao, QIAN Xiao-Qing. Species of Duckweeds in Summer in Jiangsu Province and Water Environments They Grow in [J]. Journal of Ecology and Rural Environment, 2012, 28(5): 554-558.
[5]	CAO Xiao, LIU Hong-Yu, LI Yu-Feng, ZHENG Nan. Relationship Between Wetland Plant Communities and Water Environment Quality in Xixi Wetland Park [J]. Journal of Ecology and Rural Environment, 2011, 27(3): 69-75.
[6]	ZHAO Yong-hong;DENG Xiang-zheng;LU Qi. Nitrogen Budget in Farming-Feeding System and Its Impacts on Local Environment in Wuliangsuhai Lake Watershed [J]. Journal of Ecology and Rural Environment, 2010, 26(5): 442-447.
[7]	LI Yu-Feng, LIU Hong-Yu, HAO Jing-Feng, CAO Xiao, HU Jun-Na. Relationship Between Landscape Stucture and Water Environment in Small Rural Watersheds [J]. Journal of Ecology and Rural Environment, 2010, 26(1): 15-19.
[8]	HUANG Shen-Fa, WANG Min, CHE Yue, YANG Kai. Effect of Land Use on Water Quality in Waterhead Region in River Network Plain——A Case Study of the Upper Huangpu River [J]. Journal of Ecology and Rural Environment, 2006, 22(4): 14-19.
[9]	ZENG Yue, HONG Hua-Sheng, CHEN Wei-Qi, ZHENG Yu. Impact of phosphorus loss on water environment in intensive livestock rearing areas and the countermeasures [J]. Journal of Ecology and Rural Environment, 2004, 20(3): 77-80.
[10]	JIAO Feng, XU Peng-Zhu, LI Xin. Annual variation of major water quality indices of Yixing and Liyang′s rivers and their causes [J]. Journal of Ecology and Rural Environment, 2004, 20(1): 52-55.
[11]	GAO Chao, ZHANG Tao-Lin. Agricultural Soil Phosphorus Dynamics in Taihu Lake Watershed and Its Environmental Impact [J]. Journal of Ecology and Rural Environment, 2000, 16(4): 24-27.
[12]	ZHU Wei-Bin, WANG Wan-Jie, ZHU Huai-Ning. Discussion on Harmfulness and Causes of Water Pollution in Jiangsu Province [J]. Journal of Ecology and Rural Environment, 1997, 13(1): 50-52.
[13]	ZHAO Yin-Wei, ZHENG Shi-Zhang, YE Yu-Wu. Study on controlling system for environniental pollution of a-griculture and animal husbandry in Songjiang,a source regiou of drinking water for Shangbai [J]. Journal of Ecology and Rural Environment, 1994, 10(3): 9-13.
[14]	SHEN Jian, ZHAO Yin-Wei. One Dimension Dynamic Mathematical Model for Water Quantity and Quality in Tongbotang River and Water Envi- ronmental Capacity [J]. Journal of Ecology and Rural Environment, 1993, 9(4): 5-7,62.
[15]	HE Jian-Min, ZHAO Yin-Wei. Model for the Management of Drinking Water Environ- ment at songjiang Town [J]. Journal of Ecology and Rural Environment, 1993, 9(3): 1-3,62.