TiO_2插层氧化石墨烯降解亚甲基蓝性能研究
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摘要
采用改进的Hummers法制备氧化石墨烯,再利用钛酸丁酯原位水解制得TiO_2插层氧化石墨烯。通过扫描电镜(SEM)、透射电镜(TEM)和X射线衍射(XRD)等表征手法对TiO_2插层氧化石墨烯的形貌、结构进行表征分析;并通过降解亚甲基蓝试验评估了样品的光催化性能。XRD与TEM表征结果表明,氧化石墨烯氧化均匀,在超声状态下,酞酸丁酯可在氧化石墨烯片层间原位生成锐钛矿相的纳米级TiO_2。降解试验结果表明:TiO_2插层氧化石墨烯对亚甲基蓝有优异的光催化降解性能,所制备的TiO_2插层氧化石墨烯重复降解亚甲基蓝4次,降解率依然可维持在99.97%,具有较高的重复使用性能。
Graphene oxide is prepared by the modified Hummers method and the TiO_2-intercalated graphene oxide( TiO_2-GO) isprepared by in-situ formation. The morphology of TiO_2-GO are characterized by scanning electron microscopy(SEM), transmission electronmicroscopy(TEM) and X-ray diffraction(XRD) respectively. The photocatalytic degradation activity of TiO_2-GO is studied. The results ofXRD and TEM show that GO is uniformly oxidized and anatase phase of nano-TiO_2 could be generated among the GO sheets in situ byhydrolysis of butyl titanate under ultrasonic state. The results of photocatalytic activity show that TiO_2-GO has an excellent photocatalyticdegradation property toward methylene blue, the degradation of methylene blue is repeated four times by TiO_2-GO and the degradation ratecould still be maintained at 99.97%, which proved that TiO_2-GO has a high reuse performance.
Graphene oxide is prepared by the modified Hummers method and the TiO_2-intercalated graphene oxide( TiO_2-GO) isprepared by in-situ formation. The morphology of TiO_2-GO are characterized by scanning electron microscopy(SEM), transmission electronmicroscopy(TEM) and X-ray diffraction(XRD) respectively. The photocatalytic degradation activity of TiO_2-GO is studied. The results ofXRD and TEM show that GO is uniformly oxidized and anatase phase of nano-TiO_2 could be generated among the GO sheets in situ byhydrolysis of butyl titanate under ultrasonic state. The results of photocatalytic activity show that TiO_2-GO has an excellent photocatalyticdegradation property toward methylene blue, the degradation of methylene blue is repeated four times by TiO_2-GO and the degradation ratecould still be maintained at 99.97%, which proved that TiO_2-GO has a high reuse performance.
引文
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[2]LU S Y,WU D,WANG Q L,et al.Photocatalytic decomposition on nano-TiO2:Destruction of chloroaromatic compounds[J].Chemosphere,2011,82(9):1215-1224.
[3]CHEN X B,MAO S S.Titanium dioxide nanomaterials:Synthesis,properties,modifications and applications[J].Chemical Reviews,2007,38(41):2891.
[4]ZHANG J,WU W C,YAN S,et al.Enhanced photocatalytic activity for the degradation of rhodamine B by TiO2modified with Gd2O3calcined at high temperature[J].Applied Surface Science,2015(344):249-256.
[5]熊轶超.纳米二氧化钛改性及其可见光光催化性能研究[D].大连:大连工业大学,2012.
[6]KUMAR S G,DEVI L G.Review on modified TiO2Photocatalysis under UV/Visible light:selected results and related mechanisms on interfacial charge carrier transfer dynamics[J].Journal of Physical Chemistry A,2011,115(46):13211-13241.
[7]MELE G,ANNESE C,ACCOLTI L D,et al.Photoreduction of carbon dioxide to formic acid in aqueous suspension:a comparsion between phthalocyanine/TiO2and porphyrin/TiO2catalysed processes[J].Molecules,2015,20(1):396-415.
[8]谷留安.共轭分子/二氧化钛复合材料的制备及光催化性能研究[D].哈尔滨:哈尔滨工业大学,2013.
[9]GERISCHER H,HEUER A.The role of oxygen Zn photooxidation of organic molecules on semiconductor particles[J].Journal of Physical Chemistry,1991(95):5261-5267.
[10]VINODGOPAL K,STAFFORD U.Electrochemitally assisted photocatalysis.2.The role of oxygen and reaction intermediates in the degradation of 4-chlorophenol on immobilized TiO2particulate films[J].Journal of Physical Chemistry,1994,98(27):6797-6803.
[11]胡海.泡沫金属负载纳米TiO2的制备、表征及其光催化性能的研究[D].上海:上海交通大学,2007.
[12]ZHANG H,LV X,LI Y,et al.P25-graphene composite as a high performance photocatalyst[J].Acs Nano,2009,4(1):380-386.
[13]ZHANG Y H,TANG Z R,FU X Z,et al.TiO2-Graphene Nanocomposites for gas-Phase photocatalytic degradation of volatile aromatic pollutant:is TiO2-Graphene truly different from Other TiO2-Carbon composite materials?[J].Acs Nano,2010,4(12):7303-7314.
[14]WEN Y Y,DING H M,SHAN Y K.Preparation and visible light photocatalytic activity of Ag/TiO2/graphene nanocomposite[J].Nanoscale,2011,3(10):4411-4417.
[15]FAN W Q,LA Q H,ZHANG Q H,et al.Nanocomposites of TiO2and reduced graphene Oxide as efficient photocatalysts for hydrogen evolution[J].Journal of Physical Chemistry C,2011,115(21):10694-10701.
[16]WILLIAMS G,SEGER B,KAMAT P V,et al.TiO2-graphene nanocomposite UV-assisted photocatalytic reduction of graphene oxide[J].Acs Nano,2008,2(7):1487-1491.
[17]MATSUO Y.Preparation of intercalation compounds of graphite oxide[J].Carbon,2007,45(12):2462.
[18]SCHN L,MCALLISTER M J,SCHNIEPP,et al.Functionalized single grapheme sheets derived from splitting graphitie oxide[J].Journal of Physical Chemistry B,2006,110(17):8535-8539.
[19]UMMER S W,OFFEMA R.Preparation of graphitic oxide[J].Journal of the American Chemical Society,1958,80(6):1339.
[20]王海娟,武娜娜,张峰.可见分光光度法测定纳米银溶液的银含量及其应用[J].沙洲职业工学院学报,2011(4):12-15.
[21]傅玲,刘洪波,邹艳红,等.Hummers法制备氧化石墨时影响氧化程度的工艺因素研究[J].炭素,2005(4):10-14.