改性石墨烯光催化薄膜的制备及可见光光催化性能
|
摘要
根据改进的Hummers法制备了5mg/mL的改性石墨烯分散液并采用匀胶法在玻璃片上制备改性石墨烯薄膜,分别研究了转速(600～2000r/min)、滴胶时间(10～30s)、转加速度(100～500r·min~(-1)·s~(-1))、pH值(4～12)等匀胶工艺条件对改性石墨烯薄膜附着力的影响;通过拉曼光谱以及激光共聚焦光谱等方法,对改性石墨烯及其薄膜的微观形貌、成分、结构进行表征研究;以亚甲基蓝作为目标降解物,研究了改性石墨烯薄膜在可见光照射下的光催化性能,初步揭示了其可见光催化原理。结果如下:①确定了匀胶镀膜的优化工艺,成功制备的改性石墨烯薄膜对亚甲基蓝的可见光光催化降解率达35.3%。②激光共聚焦显微镜测定改性石墨烯薄膜在422nm处有最大吸收峰。
Using the Hummers method, 5 mg/mL graphene dispersion was prepared and the modified graphene film was prepared by spin coating onto the glass substrate. The effects of spin speed(600～2000 r/min), dropping time(10～30 s), spin acceleration(100～500 r·min~(-1)·s~(-1)) and pH value on the adhesion of the thin film were studied. The microstructures, compositions and structures of the graphene and film were characterized by Raman spectroscopy and laser confocal spectroscopy, etc. Methylene blue was used as a target to evaluate the photocatalytic activity of the modified graphene film under visible light irradiation, and its visible light photocatalytic principle was preliminarily revealed. The process of spin coating was optimized and the conditions were determined. The visible photocatalytic degradation rate of methylene blue by the modified graphene film is 35.3%, and the maximum absorption peak is at 422 nm.
Using the Hummers method, 5 mg/mL graphene dispersion was prepared and the modified graphene film was prepared by spin coating onto the glass substrate. The effects of spin speed(600～2000 r/min), dropping time(10～30 s), spin acceleration(100～500 r·min~(-1)·s~(-1)) and pH value on the adhesion of the thin film were studied. The microstructures, compositions and structures of the graphene and film were characterized by Raman spectroscopy and laser confocal spectroscopy, etc. Methylene blue was used as a target to evaluate the photocatalytic activity of the modified graphene film under visible light irradiation, and its visible light photocatalytic principle was preliminarily revealed. The process of spin coating was optimized and the conditions were determined. The visible photocatalytic degradation rate of methylene blue by the modified graphene film is 35.3%, and the maximum absorption peak is at 422 nm.
引文
[1] 张金水,王博,王心晨.氮化碳聚合物半导体光催化[J].化学进展,2014,26(1):19～29.
[2] Woan K,Pyrgiotakis G,Sigmund W.Photocatalytic Carbon-Nanotube-TiO2 Composites[J].Advanced Materials,2009,21(21):2233～2239.
[3] Geim A K,Novoselov K S.The Rise of Graphene[J].Nature Materials,2007,6(3):183～191.
[4] Novoselov K S,JIANG D,Schedin F,et al.Two-Dimensional Atomic Crystals[J].Proceedings of the National Academy of Sciences of the United States of America,2005,102(30):10451～10453.
[5] Pant H R,Park C H,Pokharel P,et al.ZnO Micro-Flowers Assembled on Reduced Graphene Sheets with High Photocatalytic Activity for Removal of Pollutants[J].Powder Technology,2013,235(2):853～858.
[6] 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.
[7] ZHU P N,Nair A S,PENG S J,et al.Facile Fabrication of TiO2-Graphene Composite with Enhanced Photovoltaic and Photocatalytic Properties by Electrospinning[J].Acs Applied Materials & Interfaces,2016,4(2):581～585.
[8] 毛洪凯,罗驹华,颜柱,等.高可见光活性磁性催化剂ZnO/ZnFe2O4/石墨烯的制备与表征[J].材料科学与工程学报,2017,35(3):374～379.
[9] Rokhsat E,Akhavan O.Improving the Photocatalytic Activity of Graphene Oxide/ZnO Nanorod Films by UV Irradiation[J].Applied Surface Science,2016,371:590～595.
[10] 黄思远,王罗春.CdS/石墨烯纳米复合材料研究进展[J].材料科学与工程学报,2016,34(4):667～672.
[11] Lue S J,Pai Y L,Shih C M,et al.Novel Bilayer Well-Aligned Nafion/Graphene Oxide Composite Membranes Prepared Using Spin Coating Method for Direct Liquid Fuel Cells[J].Journal of Membrane Science,2015,493(2015):212～223.
[12] WU C H,JIU J T,Araki T,et al.Rapid Self-Assembly of Ultrathin Graphene Oxide Film and Application to Silver Nanowire Flexible Transparent Electrodes[J].Rsc Advances,2016,6(19):15838～15845.
[13] GAN W,HAN N N,YANG C,et al.A Ternary Alloy Substrate to Synthesize Monolayer Graphene with Liquid Carbon Precursor[J].Acs Nano,2017,11(2):1371～1379.
[14] Lee E,Lee H C,Jo S B,et al.Heterogeneous Solid Carbon Source-Assisted Growth of High-Quality Graphene via CVD at Low Temperatures[J].Advanced Functional Materials,2016,26(4):562～568.
[15] Hummers W S,Offeman R E.Preparation of Graphitic Oxide[J].Journal of the American Chemical Society,1958,80(6):1339～1339.
[16] Muzyka R,Kwoka M,Sm?dowski ?,et al.Oxidation of Graphite by Different Modified Hummers Methods[J].New Carbon Materials,2017,32(1):15～20.
[17] 陈彧.基于玻璃基底的石墨烯薄膜的制备和性能研究[D].上海:上海交通大学,2011.
[18] Voiry D,Yang J,Kupferberg J,et al.High-Quality Graphene via Microwave Reduction of Solution-Exfoliated Graphene Oxide[J].Science,2016,353(6306):1413～1416.
[19] Akhavan O.The Effect of Heat Treatment on Formation of Graphene Thin Films from Graphene Oxide Nanosheets[J].Carbon,2010,48(2):509～519.
[20] NI Z H,WANG Y Y,YU T,et al.Raman Spectroscopy and Imaging of Graphene[J].Nano Research,2008,1(4):273～291.
[21] 刘洋洋,顾宝珊,郑艳银,等.氧化石墨烯对亚甲基蓝的可见光催化降解[J].化工新型材料,2019,3:211～215.
[2] Woan K,Pyrgiotakis G,Sigmund W.Photocatalytic Carbon-Nanotube-TiO2 Composites[J].Advanced Materials,2009,21(21):2233～2239.
[3] Geim A K,Novoselov K S.The Rise of Graphene[J].Nature Materials,2007,6(3):183～191.
[4] Novoselov K S,JIANG D,Schedin F,et al.Two-Dimensional Atomic Crystals[J].Proceedings of the National Academy of Sciences of the United States of America,2005,102(30):10451～10453.
[5] Pant H R,Park C H,Pokharel P,et al.ZnO Micro-Flowers Assembled on Reduced Graphene Sheets with High Photocatalytic Activity for Removal of Pollutants[J].Powder Technology,2013,235(2):853～858.
[6] 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.
[7] ZHU P N,Nair A S,PENG S J,et al.Facile Fabrication of TiO2-Graphene Composite with Enhanced Photovoltaic and Photocatalytic Properties by Electrospinning[J].Acs Applied Materials & Interfaces,2016,4(2):581～585.
[8] 毛洪凯,罗驹华,颜柱,等.高可见光活性磁性催化剂ZnO/ZnFe2O4/石墨烯的制备与表征[J].材料科学与工程学报,2017,35(3):374～379.
[9] Rokhsat E,Akhavan O.Improving the Photocatalytic Activity of Graphene Oxide/ZnO Nanorod Films by UV Irradiation[J].Applied Surface Science,2016,371:590～595.
[10] 黄思远,王罗春.CdS/石墨烯纳米复合材料研究进展[J].材料科学与工程学报,2016,34(4):667～672.
[11] Lue S J,Pai Y L,Shih C M,et al.Novel Bilayer Well-Aligned Nafion/Graphene Oxide Composite Membranes Prepared Using Spin Coating Method for Direct Liquid Fuel Cells[J].Journal of Membrane Science,2015,493(2015):212～223.
[12] WU C H,JIU J T,Araki T,et al.Rapid Self-Assembly of Ultrathin Graphene Oxide Film and Application to Silver Nanowire Flexible Transparent Electrodes[J].Rsc Advances,2016,6(19):15838～15845.
[13] GAN W,HAN N N,YANG C,et al.A Ternary Alloy Substrate to Synthesize Monolayer Graphene with Liquid Carbon Precursor[J].Acs Nano,2017,11(2):1371～1379.
[14] Lee E,Lee H C,Jo S B,et al.Heterogeneous Solid Carbon Source-Assisted Growth of High-Quality Graphene via CVD at Low Temperatures[J].Advanced Functional Materials,2016,26(4):562～568.
[15] Hummers W S,Offeman R E.Preparation of Graphitic Oxide[J].Journal of the American Chemical Society,1958,80(6):1339～1339.
[16] Muzyka R,Kwoka M,Sm?dowski ?,et al.Oxidation of Graphite by Different Modified Hummers Methods[J].New Carbon Materials,2017,32(1):15～20.
[17] 陈彧.基于玻璃基底的石墨烯薄膜的制备和性能研究[D].上海:上海交通大学,2011.
[18] Voiry D,Yang J,Kupferberg J,et al.High-Quality Graphene via Microwave Reduction of Solution-Exfoliated Graphene Oxide[J].Science,2016,353(6306):1413～1416.
[19] Akhavan O.The Effect of Heat Treatment on Formation of Graphene Thin Films from Graphene Oxide Nanosheets[J].Carbon,2010,48(2):509～519.
[20] NI Z H,WANG Y Y,YU T,et al.Raman Spectroscopy and Imaging of Graphene[J].Nano Research,2008,1(4):273～291.
[21] 刘洋洋,顾宝珊,郑艳银,等.氧化石墨烯对亚甲基蓝的可见光催化降解[J].化工新型材料,2019,3:211～215.