改性石墨烯电吸附去除水中砷离子

doi:10.19741/j.issn.1673-4831.2019.0863

生态与农村环境学报 ›› 2020, Vol. 36 ›› Issue (4): 531-541.doi: 10.19741/j.issn.1673-4831.2019.0863

改性石墨烯电吸附去除水中砷离子

徐斌¹, 吴文倩², 皋海岭^1,3, 张毅敏¹, 张书陵⁴

1. 生态环境部南京环境科学研究所, 江苏南京 210042;
2. 南京市水利规划设计院股份有限公司, 江苏南京 210008;
3. 河海大学环境学院, 江苏南京 210098;
4. 常州大学环境与安全工程学院, 江苏常州 213164

收稿日期:2019-10-29 出版日期:2020-04-25 发布日期:2020-04-27
通讯作者: 徐斌,E-mail:xubinnies@163.com E-mail:xubinnies@163.com
作者简介:徐斌(1988-),男,江苏南京人,助理研究员,博士,主要从事水处理技术和水体生态修复研究。E-mail:xubinnies@163.com
基金资助:
江苏省科协青年科技人才托举工程；江苏省自然科学基金青年科学基金（BK20170111）；国家自然科学基金青年科学基金（51808251）；国家水体污染控制与治理科技重大专项（2017ZX07203-004）

Study on Electrosorption of As Ions in Aqueous Solution by Modified Graphene

XU Bin¹, WU Wen-qian², GAO Hai-ling^1,3, ZHANG Yi-min¹, ZHANG Shu-ling⁴

1. Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment, Nanjing 210042, China;
2. Nanjing Water Planning and Designing Institute Co. Ltd., Nanjing 210008, China;
3. College of Environment, Hohai University, Nanjing 210098, China;
4. School of Environmental and Safety Engineering, Changzhou University, Changzhou 213164, China

Received:2019-10-29 Online:2020-04-25 Published:2020-04-27

摘要/Abstract

摘要： 采用水热法制备得到改性石墨烯材料：石墨烯/TiO₂（GA/TiO₂）复合材料。通过扫描电镜（SEM）、透射电镜（TEM）、氮气吸附-脱附、拉曼光谱、电化学等手段对石墨烯（GA）和GA/TiO₂材料的外观形貌、孔隙结构、电化学性能等进行了表征；将GA和GA/TiO₂材料组装成电极，应用于电容去离子（CDI）去除砷离子，分析电压、循环流速、温度和初始浓度对砷离子去除效果的影响。结果表明：GA/TiO₂材料具有三维孔状结构，比表面积为416.99 m²·g^-1，比电容为320.75 F·g^-1，优于GA材料。GA/TiO₂电极CDI除砷性能优于GA电极。随着电压的升高，砷离子去除率和吸附量均增大；随着温度的升高，砷离子去除率和吸附量均减少；随着初始离子质量浓度的增大，砷离子吸附量增加，去除率减小；而循环流速对砷离子去除率没有明显影响。GA /TiO₂电极对砷离子吸附过程符合准一级动力学模型和Freundlich等温模型。

关键词: 电容去离子技术, 石墨烯, 二氧化钛, 砷离子

Abstract: In this paper, the modified graphene material, graphene/titanium dioxide (GA/TiO₂) composite, was prepared by hydrothermal method. The morphology, pore structure and electrochemical properties of graphene (GA) and GA/TiO₂ were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen adsorption-desorption, Raman spectroscopy and electrochemistry. Then GA and GA/TiO₂ were assembled into electrodes to remove As ions by capacitive deionization (CDI) method. The removal efficiency of As ions was analyzed through different experimental conditions including voltage, circulating flow rate, temperature and initial As ion concentration. The results show that GA/TiO₂ had a three-dimensional porous structure with specific surface area of 416.99 m²·g^-1 and specific capacitance of 320.75 F·g^-1, which were better than that of GA. In addition, the removal performance of As ions by CDI on GA/TiO₂ electrode was better than that of GA electrode. The removal efficiency and adsorption capacity of As ions increased with the increase in voltage, but decreased with the increase in temperature. However, the removal efficiency decreased and adsorption capacity increased with the increase in initial ion concentration. The circulating flow rate had no significant effect on the removal efficiency. Moreover, the adsorption process of As ions on GA/TiO₂ electrode can be well fitted by the pseudo-first order kinetic model and Freundlich model.

Key words: capacitance deionization technology, graphene, titanium dioxide, As ions

中图分类号:

X703.1

徐斌, 吴文倩, 皋海岭, 张毅敏, 张书陵. 改性石墨烯电吸附去除水中砷离子[J]. 生态与农村环境学报, 2020, 36(4): 531-541.

XU Bin, WU Wen-qian, GAO Hai-ling, ZHANG Yi-min, ZHANG Shu-ling. Study on Electrosorption of As Ions in Aqueous Solution by Modified Graphene[J]. Journal of Ecology and Rural Environment, 2020, 36(4): 531-541.

参考文献 28

[1]	AMIRI A,AHMADI G,SHANBEDI M,et al.Microwave-Assisted Synthesis of Highly-Crumpled,Few-Layered Graphene and Nitrogen-Doped Graphene for Use as High-Performance Electrodes in Capacitive Deionization[J].Scientific Reports,2015,5:17503.
[2]	QU Y T,CAMPBELL P G,HEMMATIFAR A,et al.Charging and Transport Dynamics of a Flow-Through Electrode Capacitive Deionization System[J].The Journal of Physical Chemistry B,2018,122(1):240-249.
[3]	梁宏旭,赵新坤,宋彬,等.改性活性碳毡电吸附污水中的Zn2+[J].中国环境科学,2018,38(4):1336-1345.[LIANG Hong-xu,ZHAO Xin-kun,SONG Bin,et al.Electro-Chemical Adsorption of Zn2+ in Wastewater by Modified Activated Carbon Felt［J].China Environmental Science,2018,38(4):1336-1345.］
[4]	LIU P Y,YAN T T,SHI L Y,et al.Graphene-Based Materials for Capacitive Deionization[J].Journal of Materials Chemistry A,2017,5(27):13907-13943.
[5]	LEONARD K C,SUYAMA W E,ANDERSON M A.Evaluating the Electrochemical Capacitance of Surface-Charged Nanoparticle Oxide Coatings[J].Langmuir,2012,28(15):6476-6484.
[6]	EL-DEEN A G,BARAKAT N A M,KIM H Y.Graphene Wrapped MnO2-Nanostructures as Effective and Stable Electrode Materials for Capacitive Deionization Desalination Technology[J].Desalination,2014,344:289-298.
[7]	LI H B,LEONG Z Y,SHI W H,et al.Hydrothermally Synthesized Graphene and Fe3O4 Nanocomposites for High Performance Capacitive Deionization[J].RSC Advances,2016,6(15):11967-11972.
[8]	YIN H J,ZHAO S L,WAN J W,et al.Three-Dimensional Graphene/Metal Oxide Nanoparticle Hybrids for High-Performance Capacitive Deionization of Saline Water[J].Advanced Materials,2013,25(43):6270-6276.
[9]	HU X B,YU Y,HOU W M,et al.Effects of Particle Size and pH Value on the Hydrophilicity of Graphene Oxide[J].Applied Surface Science,2013,273:118-121.
[10]	孟玉兰.多孔炭和流动电极的制备及其脱盐性能的研究[D].大连:大连理工大学,2015.[MENG Yu-lan.The Preparation of Porous Carbon and Flow Electrode and Its Application in Capacitive Deionization［D].Dalian:Dalian University of Technology,2015.］
[11]	蒋绍阶,马丹丹,盛贵尚,等.KOH改性活性炭涂层电极的电容去离子性能研究[J].工业水处理,2015,35(9):53-56.[JIANG Shao-jie,MA Dan-dan,SHENG Gui-shang,et al.Research on the Capacitive Deionization Performance of Activated Carbon-Coated Electrodes Modified With KOH［J].Industrial Water Treatment,2015,35(9):53-56.］
[12]	FAN C S,TSENG S C,LI K C,et al.Electro-Removal of Arsenic(Ⅲ) and Arsenic(Ⅴ) From Aqueous Solutions by Capacitive Deionization[J].Journal of Hazardous Materials,2016,312:208-215.
[13]	张亚坤.磁性石墨烯纳米材料对水中第一类重金属的吸附研究[D].济南:济南大学,2014.[ZHANG Ya-kun.Study on Adsorption of the First Category Metal Pollutants From Aqueous Solution by Magnetic Graphene Nano Material［D].Jinan:University of Jinan,2014.］
[14]	王志,赵研,姜秋俚,等.强化电容去离子脱盐的吸附机理研究[J].环境工程,2018,36(2):78-82.[WANG Zhi,ZHAO Yan,JIANG Qiu-li,et al.Study on Adsorption Mechanism of Improving Deionization Desalination Efficiency［J].Environmental Engineering,2018,36(2):78-82.］
[15]	SHAWABKEH R.Equilibrium Study and Kinetics of Cu2+ Removal from Water by Zeolite Prepared From Oil Shale Ash[J].Process Safety and Environmental Protection,2009,87(4):261-266.
[16]	PIMENTEL P M,MELO M A F,MELO D M A,et al.Kinetics and Thermodynamics of Cu(Ⅱ) Adsorption on Oil Shale Wastes[J].Fuel Processing Technology,2008,89(1):62-67.
[17]	蒲生彦,王可心,马慧,等.磁性壳聚糖凝胶微球对水中Pb(Ⅱ)的吸附性能[J].中国环境科学,2018,38(4):1364-1370.[PU Sheng-yan,WANG Ke-xin,MA Hui,et al.Adsorption Properties Ofmagnetic Chitosan Hydrogelmicrospheres to Pb(Ⅱ) From Aqueous Solutions［J].China Environmental Science,2018,38(4):1364-1370.］
[18]	WANG H,ZHANG D S,YAN T T,et al.Three-Dimensional Macroporous Graphene Architectures as High Performance Electrodes for Capacitive Deionization[J].Journal of Materials Chemistry A,2013,1(38):11778.
[19]	BRUN N,PRABAHARAN S R S,SURCIN C,et al.Design of Hierarchical Porous Carbonaceous Foams From a Dual-Template Approach and Their Use as Electrochemical Capacitor and Li Ion Battery Negative Electrodes[J].The Journal of Physical Chemistry C,2012,116(1):1408-1421.
[20]	EL-DEEN A G,CHOI J H,KIM C S,et al.TiO2 Nanorod-Intercalated Reduced Graphene Oxide as High Performance Electrode Material for Membrane Capacitive Deionization[J].Desalination,2015,361:53-64.
[21]	YAN J,WEI T,SHAO B,et al.Electrochemical Properties of Graphene Nanosheet/Carbon Black Composites as Electrodes for Supercapacitors[J].Carbon,2010,48(6):1731-1737.
[22]	施周,杨文浩,杨灵芳,等.等离子改性CNT/TiO2电极吸附去除水中苯酚的研究[J].中国环境科学,2015,35(9):2664-2669.[SHI Zhou,YANG Wen-hao,YANG Ling-fang,et al.Electrosorption of Phenol in Aqueous Solution Using a Plasma-activated CNT/TiO2 Electrode［J].China Environmental Science,2015,35(9):2664-2669.］
[23]	LEI Z B,CHRISTOV N,ZHAO X S.Intercalation of Mesoporous Carbon Spheres Between Reduced Graphene Oxide Sheets for Preparing High-Rate Supercapacitor Electrodes[J].Energy & Environmental Science,2011,4(5):1866.
[24]	杨慧云.电容去离子技术中活性炭纤维电极体系的研究[D].北京:北京工商大学,2006.[YANG Hui-yun.Study on the Activated Carbon Fiber Electrodes of Capacitive Deionization Technology［D].Beijing:Beijing Technology and Business University,2006.］
[25]	FAN C S,LIOU S Y H,HOU C H.Capacitive Deionization of Arsenic-Contaminated Groundwater in a Single-Pass Mode[J].Chemosphere,2017,184:924-931.
[26]	施周,靳兆祺,邓林,等.CNT/PANI电极吸附去除水中Cu2+的研究[J].中国环境科学,2016,36(12):3650-3656.[SHI Zhou,JIN Zhao-qi,DENG Lin,et al.Electrosorption of Cu2+ in Aqueous Solution Using CNT/PANI Electrodes［J].China Environmental Science,2016,36(12):3650-3656.］
[27]	杨灵芳.等离子强化碳纳米管及其复合物电极电容去除铅离子研究[D].长沙:湖南大学,2015.[YANG Ling-fang.Plasma Enhanced Carbon Nanotube and Its Composite Electrodes for Capacitive Deionization of Lead Ions From Aqueous Solution［D].Changsha:Hunan University,2015.］
[28]	JEON S I,PARK H R,YEO J G,et al.Desalination Via a New Membrane Capacitive Deionization Process Utilizing Flow-Electrodes[J].Energy & Environmental Science,2013,6(5):1471.

改性石墨烯电吸附去除水中砷离子

Study on Electrosorption of As Ions in Aqueous Solution by Modified Graphene

RichHTML

PDF

可视化

摘要/Abstract

引用本文

使用本文

参考文献 28

相关文章 3

编辑推荐

Metrics

本文评价

[1]	张书陵, 封金财, 徐斌, 张毅敏, 杨飞, 张志伟. SA/GO@Fe₃O₄磁性粒子电极降解甲基橙废水的研究[J]. 生态与农村环境学报, 2020, 36(6): 803-810.
[2]	张志伟, 徐斌, 张毅敏, 巴翠翠, 汤志凯, 顾诗云. 氧化石墨烯复合膜在水处理中的应用研究进展与展望[J]. 生态与农村环境学报, 2019, 35(10): 1225-1231.
[3]	邓天天, 胡烨, 刘帅霞, 李晗晟, 侯宇梦. Fe₂O₃@GO聚合物对水中As³⁺的吸附特性表征[J]. 生态与农村环境学报, 2018, 34(10): 930-938.