Zr/Ti柱撑蒙脱石的制备及对硝基苯的吸附
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摘要
为了解决硝基苯的水体污染问题,将锆/钛聚合羟基阳离子插入到钠基蒙脱石(Na-MMT)层间,制备锆/钛柱撑蒙脱石(Zr/Ti-MMT)材料,并用于吸附废水中硝基苯。用X射线衍射、Fourier红外光谱仪及比表面积测量对Zr/Ti-MMT材料进行表征,并考察了Zr/Ti-MMT材料对废水中硝基苯的吸附效果。结果表明:Zr/Ti-MMT主要以窄缝型介孔和微孔为主,晶面间距d_((001))为3.29 nm,比表面积为115.4 m~2/g,平均孔径为4.35 nm。当Zr/Ti-MMT用量为0.1 g、硝基苯初始浓度为40 mg/L、温度为45℃,硝基苯去除率最高,吸附量(q_e)和去除率分别为17.59 mg/g和87.94%。Zr/Ti-MMT对硝基苯的吸附过程以物理吸附方式为主,符合Langmuir等温线模型。Zr/Ti-MMT材料吸附硝基苯属于自发的吸热熵增的过程,符合一级动力学。
Zirconium/titanium-pillared montmorillonite(Zr/Ti-MMT) was prepared via inserting zirconium/titanium polyhydroxy cations into the interlayer spaces of Na-montmorillonite(Na-MMT) as an adsorbent for adsorption of nitrobenzene in wastewater.Zr/Ti-MMT was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, and specific surface area measurement.The adsorption performance of Zr/Ti-MMT on nitrobenzene in wastewater was investigated.The results show that Zr/Ti-MMT mainly consists of narrow mesopores and micropores, the interplanar spacing(d_((001))) is 3.29 nm, the specific surface area is 115.4 m~2/g and the average pore size is 4.35 nm.The removal rate of nitrobenzene reaches the maximum value, the adsorption quantity(q_e) and removal rate are 17.59 mg/g and 87.94%, respectively, when Zr/Ti-MMT is 0.1 g, the initial concentration of nitrobenzene is 40 mg/L and the adsorption temperature is 45 ℃.It is indicated that the adsorption by Zr/Ti-MMT belongs to a physical adsorption, and follows the Langmuir isothermal model.The adsorption of Zr/Ti-MMT on nitrobenzene is a spontaneous process of heat absorption and entropy increase, and the adsorption process fits the first-order kinetic model.
Zirconium/titanium-pillared montmorillonite(Zr/Ti-MMT) was prepared via inserting zirconium/titanium polyhydroxy cations into the interlayer spaces of Na-montmorillonite(Na-MMT) as an adsorbent for adsorption of nitrobenzene in wastewater.Zr/Ti-MMT was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, and specific surface area measurement.The adsorption performance of Zr/Ti-MMT on nitrobenzene in wastewater was investigated.The results show that Zr/Ti-MMT mainly consists of narrow mesopores and micropores, the interplanar spacing(d_((001))) is 3.29 nm, the specific surface area is 115.4 m~2/g and the average pore size is 4.35 nm.The removal rate of nitrobenzene reaches the maximum value, the adsorption quantity(q_e) and removal rate are 17.59 mg/g and 87.94%, respectively, when Zr/Ti-MMT is 0.1 g, the initial concentration of nitrobenzene is 40 mg/L and the adsorption temperature is 45 ℃.It is indicated that the adsorption by Zr/Ti-MMT belongs to a physical adsorption, and follows the Langmuir isothermal model.The adsorption of Zr/Ti-MMT on nitrobenzene is a spontaneous process of heat absorption and entropy increase, and the adsorption process fits the first-order kinetic model.
引文
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[25]GUO Z,LIU X,HUANG H,et al.Adsorption thermodynamics and kinetics of yohimbine onto strong acid cation exchange fiber[J].JTaiwan Inst Chem E,2017,71:1-12.
[2]LI T,ZHOU Z F,LI H.A novel approach for enhancing bacterial strains’Nitrobenzene degradation rate[J].Int Biodeter Biodegr,2017,123:63-69.
[3]马冬梅.多相Fenton氧化法处理染料中间体结晶废液的研究[D].上海:东华大学,2014.MA Dongmei.Study on spent liquor of dye intermediate crystallization by heterogeneous Fenton oxidation technology(in Chinese,dissertation).Shanghai:Donghua University,2014.
[4]BAI J F,LIU Y,YIN X H,et al.Efficient removal of nitrobenzene by Fenton-like process with Co-Fe layered double hydroxide[J].Appl Surf Sci,2017,416:45-50.
[5]ZHANG Q,LIU Y M,CHEN S,et al.Nitrogen-doped diamond electrode shows high performance for electrochemical reduction of nitrobenzene[J].J Hazard Mater,2014,265:185-190.
[6]ZHAO C,SI B,MIRZA Z A,et al.Activated carbon fiber(ACF)enhances the UV/EF system to remove nitrobenzene in water[J].Sep Purif Technol,2017,187:397-406.
[7]任广军,翟玉春.宋恩军,等.水中硝基苯在柱撑膨润土上的吸附行为[J].化工学报,2004,11:1833-1836.REN Guangjun,ZHAI Yuchun,SONG Enjun,et al.J Chen Ind Eng(in Chinese),2004,11:1833-1836.
[8]张敏.钛交联蒙脱石的制备与表征的研究[D].武汉:武汉科技大学,2015.ZHANG Min.Study on preparation and characterization of Ti-pillared montmorillonite(in Chinese,dissertation).Wuhan:Wuhan University of Science and Technology,2015.
[9]龙森,庹必阳,韩朗,等.锆柱撑蒙脱石对十二烷基苯磺酸钠的吸附研究[J].非金属矿,2017(2):4-7.LONG Sen,TUO Biyang,HAN Lang,et al.Non-Met Min(in Chinese),2017(2):4-7.
[10]牛露,赵彬侠,叶维,等.Fe-Zn-Al-柱撑蒙脱石催化剂的制备及其降解酸性橙II性能[J].硅酸盐学报,2016,44(10):1501-1508.NIU Lu,ZHAO Binxia,YE Wei,et al.J Chin Ceram Soc,2016,44(10):1501-1508.
[11]MICHALIK-ZYM A,DULA R,DURACZYNSKA D,et al.Active,selective and robust Pd and/or Cr catalysts supported on Ti/Zr-or[Ti/Zr]-pillared montmorillonites for destruction of chlorinated volatile organic compounds[J].Appl Catal B:Environ,2015,174-175:293-307.
[12]孙东亚.羟基锆柱撑二硫化钼的制备及其催化加氢性能[D].厦门:华侨大学,2007.SUN Dongya.Preparation of hydroxyl zirconium pillared molybdenum disulfide and its catalytic hydrogenation properties(in Chinese,dissertation).Xiamen:Huaqiao University,2007.
[13]崔静洁,何文,廖世军,等.多孔材料的孔结构表征及其分析[J].材料导报,2009,23(13):82-86.CUI Jingjie,HE Wen,LIAO Shijun,et al.Mater Rev(in Chinese),2009,23(13):82-86.
[14]邹雪刚,吕文英,王雅兰,等.介孔铁锰双金属氧化物对Pb2+的吸附及其机理研究[J].环境科学学报,2017,38(3):982-991.ZHOU Xuegang,LU Wenying,WANG Yalan,et al.Acta Sci Circumstantiae(in Chinese),2017,38(3):982-991.
[15]闻辂.矿物红外光谱学[M].重庆大学出版社,1988.
[16]管俊芳,狄敬茹,于吉顺,等.Zr/Al基柱撑蒙脱石矿物材料的红外光谱研究[J].硅酸盐学报,2005,33(2):220-224.GUAN Junfang,DI Jingru,YU Jishun,et al.J Chin Ceram Soc,2005,33(2):220-224.
[17]郑跃国,谢继铃,李燕峰,等.脱硫渣吸附剂对Cu2+的吸附动力学和热力学[J].硅酸盐学报,2013,41(3):396-401.ZHENG Yueguo,XIE Jiling,LI Yanfeng,et al.J Chin Ceram Soc,2013,41(3):396-401.
[18]韩朗,庹必阳,杨慧,等.锆柱撑蒙脱石对黄药的吸附机理[J].硅酸盐学报,2017,45(5):729-736.HAN Lang,TUO Biyang,YANG Hui,et al.J Chin Ceram Soc,2017,45(5):729-736.
[19]WANG N,JIN R N,OMER A M,et al.Adsorption of Pb(Ⅱ)from fish sauce using carboxylated cellulose nanocrystal:Isotherm,kinetics and thermodynamic studies[J].Int J Biol Macromol,2017,102:232-240.
[20]WIBOWO E,ROKHMAT M,SUTISNA,et al.Reduction of seawater salinity by natural zeolite(Clinoptilolite):Adsorption isotherms,thermodynamics and kinetics[J].Desalination,2017,409:146-156.
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[23]保佳媛,李峻峰,张钱丽,等.活性炭纤维对亚甲基蓝的吸附动力学和热力学研究[J].苏州科技学院学报,2015(3):30-35.BAO Jiayuan,LI Junfeng,ZHANG Qianli,et al.J Suzhou Univ Sci Technol(in Chinese),2015(3):30-35.
[24]EBITANI K,KATO M,MOTOKURA K,et al.Highly efficient heterogeneous acylations of aromatic compounds with acid anhydrides and carboxylic acids by montmorillonite-enwrapped titanium as a solid acid catalyst[J].Res Chem Intermed,2006,32(3/4):305-315.
[25]GUO Z,LIU X,HUANG H,et al.Adsorption thermodynamics and kinetics of yohimbine onto strong acid cation exchange fiber[J].JTaiwan Inst Chem E,2017,71:1-12.