用改良的Hummers法制得了氧化石墨烯,对其微观形貌、成分和结构进行了表征,并使用亚甲基蓝溶液测试其光催化效率。通过SEM、TEM、Raman分析表明,得到的是少层氧化石墨烯,碳氧原子数比在3∶1左右。荧光共聚焦光谱显示,所得到的氧化石墨烯在420~700nm的光波谱范围内都有特征吸收峰。氧化石墨烯能够迅速吸附亚甲基蓝分子,然后对其进行光催化降解,在亚甲基蓝浓度为40mg/L、氧化石墨烯浓度为10mg/L时,降解率能达到40%。之后,初步探究了氧化石墨烯的光催化机理。
The graphene oxide was prepared by modified Hummer method.Its microstructure,composition and structure were characterized and the photocatalytic efficiency was tested using methylene blue solution.SEM,TEM and raman analysis showed that few layer graphene oxide was obtained,and the ratio of carbon to oxygen was about 3∶1.Fluorescence confocal spectroscopy showed that the dispersion of graphene oxide had characteristic absorption peaks in the range of 420~700nm.It was found that the methylene blue molecule was rapidly adsorbed then degraded by the graphene oxide under visible light.The degradation efficiency could reach 40% when the catalyst concentration was 10mg/L and the concentration of methylene blue was 40mg/L.Its photocatalytic mechanism was also discussed then.
[1] Shannon M A,Bohn P W,Elimelech M,et al.Science and technology for water purification in the coming decades[J].Nature,2008,452(7185):301-10.
[2] Ministry of Environmental Protection of the People's Republic of China.2016 Report on the state of environment in China[R/OL].Beijing Ministry of Environmental Protection of the People's Republic of China,2017.
[3] Fujishima A,Honda K.Electrochemical photolysis of water at a semiconductor electrode[J].Nature,1972,238(5358):37.
[4] Fujishima A,Zhang X,Tryk D A.Heterogeneous photocatalysis:from water photolysis to applications in environmental cleanup[J].International Journal of Hydrogen Energy,2007,32(14):2664-2672.
[5] Pinna M V,Pusino A.Direct and indirect photolysis of cyhalofop in aqueous systems[J].Chemosphere,2011,82(6):817-821.
[6] Marinho B A,de Liz M V,Lopes Tiburtius E R,et al.TiO2 and ZnO mediated photocatalytic degradation of E2 and EE2 estrogens[J].Photochemical & Photobiological Sciences Official Journal of the European Photochemistry Association & the European Society for Photobiology,2013,12(4):678-83.
[7] An W J,Wang W N,Ramalingam B,et al.Enhanced water photolysis with Pt metal nanoparticles on single crystal TiO2 surfaces[J].Langmuir,2012,28(19):7528-7534.
[8] Xu J,Teng F,Xu C,et al.Unique anatase TiO2 twinning crystals formed by high-energy {001} facets and the improved photocatalytic activity[J].Journal of Physical Chemistry C,2015,119(23):13011-13020.
[9] Pelaez M,Nolan N T,Pillai S C,et al.A review on the visible light active titanium dioxide photocatalysts for environmental applications[J].Applied Catalysis B Environmental,2012,125(33):331-349.
[10] Vinodgopal K,Kamat P V.Enhanced rates of photocatalytic degradation of an azo dye using SnO2/TiO2 coupled semiconductor thin films[J].Environmental Science & Technology,1995,29(3):841-5.
[11] Tobiska W K.Developments in modeling solar 2000 VUV irradiances associated with the atmosphere and ionosphere[J].Spacewx Com,2004.
[12] Yang L X.High efficient photocatalytic degradation of p-nitrophenol on a unique Cu2O/TiO2 p-n heterojunction network catalyst[J].Environmental Science & Technology,2010,44(19):7641-6.
[13] Morawski A W,Kusiak-Nejman E,Wanag A,et al.Photocatalytic degradation of acetic acid in the presence of visible light-active TiO2-reduced graphene oxide photocatalysts[J].Catalysis Today,2017,280:108-113.
[14] Beura R,Thangadurai P.Structural,optical and photocatalytic properties of graphene-ZnO nanocomposites for varied compositions[J].Journal of Physics & Chemistry of Solids,2017,102:168-177.
[15] Parameshwari R,Jothivenkatachalam K,Banks C E,et al.Acid-free co-operative self-assembly of graphene-ZnO nanocomposites and its defect mediated visible light photocatalytic activities[J].Physica B Condensed Matter,2017,506:32-41.
[16] Lee J E,Khoa N T,Kim S W,et al.Fabrication of Au/GO/ZnO composite nanostructures with excellent photocatalytic performance[J].Materials Chemistry & Physics,2015,164:29-35.
[17] Pawar R C,Lee C S.Single-step sensitization of reduced graphene oxide sheets and CdS nanoparticles on ZnO nanorods as visible-light photocatalysts[J].Applied Catalysis B Environmental,2014,144(1):57-65.
[18] Sun H,Liu S,Liu S,et al.A comparative study of reduced graphene oxide modified TiO2,ZnO and Ta2O5,in visible light photocatalytic/photochemical oxidation of methylene blue[J].Applied Catalysis B Environmental,2014,146(3):162-168.
[19] Dubey P K,Tiwari R S,Tripathi P,et al.Synthesis of reduced graphene oxide-TiO2 nanoparticle composite systems and its application in hydrogen production[J].International Journal of Hydrogen Energy,2014,39(29):16282-16292.
[20] Yeh T F,Syu J M,Cheng C,et al.Graphite oxide as a photocatalyst for hydrogen production from water[J].Advanced Functional Materials,2010,20(14):2255-2262.
[21] Yeh T F,Chan F F,Hsieh C T,et al.Graphite oxide with different oxygenated levels for hydrogen and oxygen production from water under illumination:the band positions of graphite oxide[J].Journal of Physical Chemistry C,2011,115(45):22587-22597.
[22] Jr W S H,Offeman R E.Preparation of graphitic oxide[J].Journal of the American Chemical Society,1958,80(6):1339.
[23] Su C Y,Lu A Y,Xu Y,et al.High-quality thin graphene films from fast electrochemical exfoliation[J].Acs Nano,2011,5(3):2332-9.
[24] Lei Y,Chen F,Luo Y,et al.Synthesis of three-dimensional graphene oxide foam for the removal of heavy metal ions[J].Chemical Physics Letters,2014,593(6):122-127.
[25] Zhang W,Zhou C,Zhou W,et al.Fast and considerable adsorption of methylene blue dye onto graphene oxide[J].Bull Environ Contam Toxicol,2011,87(1):86-90.