负载型零价铁对水体中2,4,6-三氯苯酚的去除
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摘要
以壳聚糖接枝杨梅单宁(CS-T)为载体,硼氢化钠为还原剂,制备负载型零价铁催化剂(Fe0/CS-T);通过傅里叶红外光谱(FTIR)、X射线衍射(XRD)、透射电镜(TEM)、热重分析仪(TGA)对负载型零价铁催化剂的物理性质与结构进行了表征,零价铁分散于壳聚糖接枝杨梅单宁载体上,直径200~500nm.研究其对水环境中2,4,6-三氯苯酚(2,4,6-TCP)的去除,结果表明:2,4,6-TCP在Fe0/CS-T的作用下发生了脱氯反应,脱氯率为60%左右,反应动力学符合Langmuir-Hinshelwood动力学模型,为表面反应;当材料投加量为0.2g、初始pH值为7、反应温度为25℃、反应时间为2h、2,4,6-TCP的初始质量浓度为20mg·L-1时,去除率为88.94%;在重复使用6次材料后,去除率从88.94%降到57.19%.
The supported zero valent iron catalyst(Fe0/CS-T)was prepared by using biomass resource chitosan grafting bayberry tannin as carrier and using NaBH4 as reducing agent.The structure and physical properties of supported zero valent iron catalysts were characterized by fourier transform infrared spectrometer(FTIR),X-ray diffractometer(XRD),transmission electron microscope(TEM),and thermo gravimetric analyzer(TGA).The result showed that zero valent iron was dispersed on the carrier,and the size of the zero valent iron particle was 200-500 nm.The experiments were carried out for the removal of 2,4,6-trichlorophenol by this material.The results indicated that the dechlorination reaction happened with Fe0/CST,and the rate of dechlorination was about 60%.The kinetics of the reaction was in accordance with Langmuir-Hinshelwood kinetic model and it was a surface reaction.The optimum reaction conditions were that the dosage of Fe0/CS-T was 0.2 g,initial pH was 7,temperature was 25℃,reaction time was 2 h,the initial concentration of 2,4,6-TCP was 20 mg·L-1,and the removal rate was 88.94%.The removal rate decreased from 88.94%to 57.19% when the material was reused for 6 times.
The supported zero valent iron catalyst(Fe0/CS-T)was prepared by using biomass resource chitosan grafting bayberry tannin as carrier and using NaBH4 as reducing agent.The structure and physical properties of supported zero valent iron catalysts were characterized by fourier transform infrared spectrometer(FTIR),X-ray diffractometer(XRD),transmission electron microscope(TEM),and thermo gravimetric analyzer(TGA).The result showed that zero valent iron was dispersed on the carrier,and the size of the zero valent iron particle was 200-500 nm.The experiments were carried out for the removal of 2,4,6-trichlorophenol by this material.The results indicated that the dechlorination reaction happened with Fe0/CST,and the rate of dechlorination was about 60%.The kinetics of the reaction was in accordance with Langmuir-Hinshelwood kinetic model and it was a surface reaction.The optimum reaction conditions were that the dosage of Fe0/CS-T was 0.2 g,initial pH was 7,temperature was 25℃,reaction time was 2 h,the initial concentration of 2,4,6-TCP was 20 mg·L-1,and the removal rate was 88.94%.The removal rate decreased from 88.94%to 57.19% when the material was reused for 6 times.
引文
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[26]甘润,李玲,赵丽,等.壳聚糖吸附水中铜离子的影响因素及红外光谱分析[J].环境与健康杂志,2013,30(10):915-918.
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[28]张健,孟昭虹,刘惠玲.零价铁用于水中氯代有机物还原脱氯的现状与发展[J].环境保护科学,2010,36(1):7-10.
[29]任轶舟,王亦飞,朱龙雏,等.高温煤焦气化反应的Langmuir-Hinshelwood动力学模型[J].化工学报,2014,65(10):3906-3915.
[30]王超.生物质快速热解制油工艺分析及油品改质实验研究[D].天津:天津大学,2014.
[31]陈诵英.催化反应动力学[M].北京:化学工业出版社,2007.
[2]卢杰,李梦红,潘嘉芬.有机氯代烃污染地下水环境的治理与修复[J].山东理工大学学报(自然科学版),2008,22(4):27-30.
[3]高霏,刘菲,陈鸿汉.三氯乙烯污染土壤和地下水污染源区的修复研究进展[J].地球科学进展,2008,23(8):821-829.
[4]BADANTHADKA M,MEHENDALE H M.Encyclopedia of Toxicology[M].3rd ed.American:Academic Press Inc,2014.
[5]王晓玭.活性炭的表面改性及对水中三氯苯酚的去除研究[D].南昌:南昌大学,2008.
[6]中华人民共国建设部.城市供水水质标准:CJ/T 206—2005[S/OL].(2005-02-05)[2018-03-16].https://wenku.baidu.com/view/e382f82f0912a216147929f2.html.
[7]饶欣,王菊先,戴树桂.水环境中2,4,6-三氯酚的光化学降解研究[J].中国环境科学,1995,15(2):107-112.
[8]皮运正,王建龙.臭氧氧化水中2,4,6-三氯酚的反应机理研究[J].环境科学学报,2005,25(12):1619-1623.
[9]HAMEED B H,TAN I A W,AHMAD A L.Adsorption isotherm,kinetic modeling and mechanism of 2,4,6-trichlorophenol on coconut husk-based activated carbon[J].Chemical Engineering J,2008,144(2):235-244.
[10]GILLHAM R W,O’HANNESIN S F.Enhanced degradation of halogenated aliphatics by zero-valent iron[J].Groundwater,1994,32(6):958-967.
[11]揣小明,单爱琴,刘敬武,等.利用零价铁去除四氯化碳的批实验研究[J].农业环境科学学报,2008,27(2):762-766.
[12]郭耀广,关杰,顾卫星.氯酚类化合物的污染现状及去除方法研究进展[J].上海第二工业大学学报,2016,33(3):198-207.
[13]李健.环境背景值数据手册[M].北京:中国环境科学出版社,1988.
[14]HE H P,FROST R L,BOSTROM T,et al.Changes in the morphology of organoclays with HDTMA+surfactant loading[J].Applied Clay Science,2006,31(3/4):262-271.
[15]NI S Q,YANG N.Cation exchange resin immobilized bimetallic nickel-iron nanoparticles to facilitate their application in pollutants degradation[J].J Colloid&Interface Science,2014,420(8):158.
[16]颜爱,卞琼,刘明华.改性纤维素负载零价铁去除三氯甲烷的研究[J].中国环境科学,2014,34(1):105-110.
[17]刘佩佩,罗汉金,方伟.石墨烯/二氧化硅负载纳米零价铁对As(Ⅲ)的去除[J].环境工程学报,2016,10(7):3607-3615.
[18]晏江波,杨秀英,何勇,等.活性炭负载纳米零价铁去除水中溴酸盐研究[J].应用化工,2017,46(2):249-253,269.
[19]袁飞,冯雅丽,王维大,等.碳纤维负载零价铁的制备及其去除水溶液中的六价铬[J].北京科技大学学报,2015(5):626-632.
[20]PALMA G,FREER J,BAEZA J.Removal of metal ions by modified Pinus radiata bark and tannins from water solutions[J].Water Research,2003,37(20):4974.
[21]ZHAN X M,ZHAO X.Mechanism of lead adsorption from aqueous solutions using an adsorbent synthesized from natural condensed tannin[J].Water Research,2003,37(16):3905-3912.
[22]MA H W,LIAO X P,LIU X,et al.Recovery of platinum(IV)and palladium(II)by bayberry tannin immobilized collagen fiber membrane from water solution[J].J Membrane Science,2006,278:373-380.
[23]MAO H,YU H,CHEN J,et al.Biphasic catalysis using amphiphilic polyphenols-chelated noble metals as highly active and selective catalysts[J].Scientific Reports,2013,3(7):2226.
[24]MAO H,MA J,LIAO Y,et al.Using plant tannin as natural amphiphilic stabilizer to construct an aqueous-organic biphasic system for highly active and selective hydrogenation of quinoline[J].Catalysis Science&Technology,2013,3(6):1612-1617.
[25]沈跃跃,刘祎玮,李颖,等.固化杨梅单宁对水体环境中铁离子的吸附特性研究[J].四川师范大学学报(自然科学版),2016,39(5):705-710.
[26]甘润,李玲,赵丽,等.壳聚糖吸附水中铜离子的影响因素及红外光谱分析[J].环境与健康杂志,2013,30(10):915-918.
[27]董婷婷,罗汉金,吴锦华.纳米零价铁的制备及其去除水中对氯硝基苯的研究[J].环境工程学报,2010,4(6):1257-1261.
[28]张健,孟昭虹,刘惠玲.零价铁用于水中氯代有机物还原脱氯的现状与发展[J].环境保护科学,2010,36(1):7-10.
[29]任轶舟,王亦飞,朱龙雏,等.高温煤焦气化反应的Langmuir-Hinshelwood动力学模型[J].化工学报,2014,65(10):3906-3915.
[30]王超.生物质快速热解制油工艺分析及油品改质实验研究[D].天津:天津大学,2014.
[31]陈诵英.催化反应动力学[M].北京:化学工业出版社,2007.