吉林大学学报(地球科学版) ›› 2020, Vol. 50 ›› Issue (1): 234-242.doi: 10.13278/j.cnki.jjuese.20180302

• 地质工程与环境工程 • 上一篇    

还原氧化石墨烯复合方式对Ag-TiO2基光电极电子传输性能的影响

董双石1, 付绍珠1, 于洋2, 李超群1, 初义聪2   

  1. 1. 地下水资源与环境教育部重点实验室(吉林大学), 长春 130021;
    2. 东北师范大学环境学院, 长春 130117
  • 收稿日期:2019-04-25 发布日期:2020-02-11
  • 作者简介:董双石(1980-),男,教授,博士生导师,主要从事水处理技术及资源化研究,E-mail:sdong@jlu.edu.cn
  • 基金资助:
    国家自然科学基金项目(51678270)

Effect of Reduced Graphene Oxide Composite Method on Electron Transport Performance of Ag-TiO2 Based Photoelectrodes

Dong Shuangshi1, Fu Shaozhu1, Yu Yang2, Li Chaoqun1, Chu Yicong2   

  1. 1. Key Lab of Groundwater Resources and Environment(Jilin University), Ministry of Education, Changchun 130021, China;
    2. School of Environment, Northeast Normal University, Changchun 130117, China
  • Received:2019-04-25 Published:2020-02-11
  • Supported by:
    Supported by National Natural Science Foundation of China (51678270)

摘要: 为进一步提高Ag-TiO2光催化效能,制备了还原氧化石墨烯(rGO)复合Ag-TiO2基的光电极。先通过对比不同的复合方式探究rGO对Ag-TiO2光催化剂表面电子传输和四环素降解效能的影响;再通过电化学阻抗谱测量、莫特-肖特基曲线等电化学手段对电极进行表征。结果表明:分层复合方式主要降低载体表面控制电极双层/薄膜的界面电阻,而全混复合方式主要降低总电荷转移电阻;分层电极的电子供体浓度随rGO质量分数增加而增大;在rGO质量分数为0.45%和0.25%时,分层复合和全混复合材料对四环素的降解速率分别比Ag-TiO2提高11.4%和2.3%;在外加0.5 V偏压下,分层复合电极LG6降解效率比未加外偏压时提高了5.3%,而全混复合电极MG2效率没有提升。分层复合方式能更有效地提高光催化剂表面电子传输效能。

关键词: 还原氧化石墨烯, 光催化, Ag-TiO2, 复合方式, 盐酸四环素

Abstract: The reduced graphene oxide (rGO) doped and Ag-TiO2 based photoelectrodes were prepared to study the effect of the composite method on the electron transport and tetracycline degradation by photocatalyst. The electrodes were characterized by electrochemical impedance spectroscopy and Mott-Schottky curve. The results showed that the interface resistance of the double-layer/thin film was reduced by the layered composite method on the surface of the carrier; while the total charge transfer resistance was mainly reduced by the fully mixed composite method. In addition, the concentration of the electron donor increased with the increasing of composite amount. When the rGO mass fraction was 0.45% and 0.25%, the degradation rate of tetracycline by the layered composite and the fully mixed doped electrode was 11.4% and 2.3% higher than that of Ag-TiO2, respectively. Under the applied 0.5 V bias voltage, the LG6 degradation efficiency of the layered composite electrode was increased by 5.3%; while the MG2 efficiency of the fully mixed composite electrode was not improved. The layered composite method can improve the electron transport efficiency more effectively on the surface of photocatalyst.

Key words: reduced graphene oxide, photocatalysis, Ag-TiO2, composite method, tetracycline hydrochloride

中图分类号: 

  • X522
[1] Konstantinou I K, Albanis T A. TiO2-Assisted Photocatalytic Degradation of Azo Dyes in Aqueous Solution:Kinetic and Mechanistic Investigations[J]. Applied Catalysis B:Environmental, 2004, 49(1):1-14.
[2] Xue J, Shen Q, Liang W, et al. Controlled Synthesis of Coaxial Core-Shell TiO2/Cu2O Heterostructures by Electrochemical Method and Their Photoelectrochemical Properties[J]. Materials Letters, 2013, 92:239-242.
[3] Deng B, Fu S, Zhang Y, et al. Simultaneous Pollutant Degradation and Power Generation in Visible-Light Responsive Photocatalytic Fuel Cell with an Ag-TiO2 Loaded Photoanode[J]. Nano-Structures & Nano-Objects, 2018, 15:167-172.
[4] Ma Y, Xiong H, Zhao Z, et al. Model-Based Evaluation of Tetracycline Hydrochloride Removal and Mineralization in an Intimately Coupled Photocatalysis and Biodegradation Reactor[J]. Chemical Engineering Journal, 2018, 351:967-975.
[5] 陈宇溪,罗力莎,时峥,等. Ag掺杂型TiO2粉末光催化降解四环素类抗生素废水[J]. 科技创新与应用, 2018, 7(13):36-38. Chen Yuxi, Luo Lisha, Shi Zheng, et al. Photocatalytic Degradation of Tetracycline Antibiotic Wastewater by Ag-Doped TiO2 Powder[J]. Technology Innovation and Application, 2018, 7(13):36-38.
[6] Bolotin K I, Sikes K J, Jiang Z, et al. Ultrahigh Electron Mobility in Suspended Graphene[J]. Solid State Communications, 2008, 146(9/10):351-355.
[7] Park S, Ruoff R S. Chemical Methods for the Production of Graphenes[J]. Nature Nanotechnology, 2009, 4(4):217.
[8] Gadgil B, Damlin P, Kvarnström C. Graphene vs Reduced Graphene Oxide:A Comparative Study of Graphene-Based Nanoplatforms on Electrochromic Switching Kinetics[J]. Carbon, 2016, 96:377-381.
[9] Wang P, Tang Y, Dong Z, et al. Ag-AgBr/TiO2/RGO Nanocomposite for Visible-Light Photocatalytic Degradation of Penicillin G[J]. Journal of Materials Chemistry:A, 2013, 1(15):4718-4727.
[10] Wei S, Wu R, Jian J, et al. Graphene Oxide/Core-Shell Structured TiO2@TiO2-x Nanocomposites with Highly Efficient Visible-Light Photocatalytic Performance[J]. RSC Advances, 2015, 5:40348-40351.
[11] Lee J H, Kim I K, Cho D, et al. Photocatalytic Performance of Graphene/Ag/TiO2 Hybrid Nanocomposites[J]. Carbon Letters, 2015, 16(4):247-254.
[12] Li G, Wang T, Zhu, Y, et al. Preparation and Photoelectrochemical Performance of Ag/Graphene/TiO2 Composite Film[J]. Applied Surface Science, 2011, 257(15):6568-6572.
[13] Lee M S, Hong S-S, Mohseni M. Synthesis of Photocatalytic Nanosized TiO2-Ag Particles with Sol-Gel Method Using Reduction Agent[J]. Journal of Molecular Catalysis A:Chemical, 2005, 242(1/2):135-140.
[14] Xie Y, Meng Y. SERS Performance of Graphene Oxide Decorated Silver Nanoparticle/Titania Nanotube Array[J]. RSC Advance, 2014, 4:41734-41743.
[15] 朱遂一,霍明昕,杨霞,等.制备多孔镍负载TiO2薄膜光催化降解喹啉和化工废水[J].吉林大学学报(地球科学版),2012, 42(4):1151-1158. Zhu Suiyi, Huo Mingxin, Yang Xia, et al. Preparation of P-25 Films Immobilized on Porous Nickel and High Photocatalytic for the Degradation of Quinoline and Chemical Wastewater[J]. Journal of Jilin University (Earth Science Edition), 2012, 42(4):1151-1158.
[16] Zhang Hao, Lü Xiaojun, Li Yueming, et al. P25 Graphene Composite as a High Performance Photocatalyst[J]. ACS Nano, 2010, 4(1):380-386.
[17] 袁志军.分光光度法测定四环素片中四环素的含量探究[J]. 中国现代药物应用,2011, 5(5):101-102. Yuan Zhijun. Determination of Tetracycline in Tetracycline Tablets by Spectrophotometry[J]. Chinese Journal of Modern Drug Application, 2011, 5(5):101-102
[18] Hou Y, Gan Y, Yu Z, et al. Solar Promoted Azo Dye Degradation and Energy Production in the Bio-Photoelectrochemical System with a g-C3N4/BiOBr Heterojunction Photocathode[J]. Journal of Power Sources, 2017, 371:26-32.
[19] Ding Jie, Bu Yunfei, Ou Man, et al. Facile Decoration of Carbon Fibers with Ag Nanoparticles for Adsorption and Photocatalytic Reduction of CO2[J]. Applied Catalysis B:Environmental, 2017, 202:314-325.
[20] Yang J, Liao W, Liu Y, et al. Degradation of Rhodamine B Using a Visible-Light Driven Photocatalytic Fuel Cell[J]. Electrochimica Acta, 2014, 144:7-15.
[21] Li K, He Y, Xu Y, et al. Degradation of Rhodamine B Using an Unconventional Graded Photoelectrode with Wedge Structure[J]. Environmental Science & Technology, 2011, 45(17):7401-7407.
[22] Aïnouche L, Hamadou L, Kadri A, et al. Interfacial Barrier Layer Properties of Three Generations of TiO2 Nanotube Arrays[J]. Electrochimica Acta, 2014, 133:597-609.
[23] Sun C, Wang Y, Su Q, et al. The Impacts of Graphene Concentration and Thickness on the Photocatalytic Performance of Bi12TiO20/Graphene Composite Thin Films[J]. Materials Research Express, 2017, 4(8):1-7.
[24] 邹东雷,李婷婷,高梦薇,等. 基于响应面的可见光催化材料制备与优化[J].吉林大学学报(地球科学版),2015, 45(6):1833-1838. Zou Donglei, Li Tingting, Gao Mengwei, et al.Preparation and Optimization of the Photocatalytic Materials Under Visible Light with Response Surface Methodology[J]. Journal of Jilin University (Earth Science Edition), 2015, 45(6):1833-1838.
[25] 许颖蘅,应迪文,江璇,等. 光催化燃料电池不同二氧化钛光阳极性能的对比[J]. 环境化学,2016, 15(1):82-88. Xu Yingheng, Ying Diwen, Jiang Xuan, et al. Comparison of Different TiO2 Photoanodes in Photocatalytic Fuel Cells[J]. Environmental Chemistry, 2016, 15(1):82-88.
[1] 邹东雷, 李婷婷, 高梦薇, 钱宁, 张高瑞洋, 董双石. 基于响应面的可见光催化材料制备与优化[J]. 吉林大学学报(地球科学版), 2015, 45(6): 1833-1838.
[2] 朱遂一, 霍明昕, 杨霞, 曲海利, 邵春彦, 边德军, 董龙, 孙宏伟. 制备多孔镍负载TiO2薄膜光催化降解喹啉和化工废水[J]. J4, 2012, 42(4): 1151-1158.
[3] 王玉洁, 许双英, 赵以辛, 蒋引珊. TiO2/电气石复合物的光催化性能[J]. J4, 2012, 42(2): 514-518.
[4] 朱遂一, 霍明昕, 杨霞, 董龙, 王健, 金生威, 刘秀. 泡沫镍基P-25薄膜光催化降解水中喹啉[J]. J4, 2011, 41(5): 1554-1561.
[5] 张东丽, 沙莉, 徐泽, 赵晓媛. 掺铜TiO2/膨润土光催化剂的制备及其光催化性能研究[J]. J4, 2009, 39(5): 913-917.
[6] 谭惠,李殿超,杨殿范, 王瑛玮. 掺铁-TiO2/膨润土复合光催化材料制备及性能[J]. J4, 2007, 37(1): 204-0208.
[7] 黎娜,徐自力,于连香,王晓,李文艳,刘星娟,杜尧国. 纳米TiO2/SiO2对甲苯-SO2体系气相光催化作用的影响因素[J]. J4, 2007, 37(1): 153-0157.
[8] 牟柏林,李芳菲,侯天意,孙申美,王瑛玮,祖胜男. 天然沸石对提高TiO2光催化活性的作用[J]. J4, 2006, 36(04): 668-672.
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