RGO改性介孔TiO<sub>2</sub>薄膜光催化同步去除Ni<sup>2+</sup>和SDBS

摘要
图/表
参考文献
相关文章 (15)

全文: PDF (779 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要以钛酸四丁酯（TBT）、天然鳞片石墨为原料，聚乙烯吡咯烷酮（PVP）为介孔模板剂，通过浸渍-提拉法辅助热处理和紫外辐照还原制备介孔RGO-TiO₂薄膜，利用XRD、SEM、BET、UV-Vis DRS、FT-IR等对其结构、形貌及性能进行表征.以Ni²⁺和十二烷基苯磺酸钠（SDBS）为目标污染物，考察了介孔RGO-TiO₂薄膜光催化去除Ni²⁺和SDBS的反应性能，探讨了GO加入量及pH值对其催化性能的影响.在最佳条件下，进一步研究Ni²⁺/SDBS共存体系中Ni²⁺的光催化还原和SDBS的光催化氧化.结果表明：GO的加入量为1.0wt%时，介孔RGO-TiO₂薄膜对单一体系Ni²⁺和SDBS的光催化效率最高，在此条件下，pH=7.5时Ni²⁺还原效率最高，pH=6时SDBS降解效率最高.综合以上实验条件，设定GO加入量为1.0wt%，pH≈6时，Ni²⁺/SDBS共存体系中Ni²⁺和SDBS去除效率均优于Ni²⁺和SDBS单一体系，此时，Ni²⁺还原率为87.9%，SDBS氧化率为95.5%.分析协同光催化机制，TiO₂-SDBS表面复合物在紫外光激发下，SDBS被氧化同时，光生电子及SDBS氧化产物CO₂·^-自由基同步还原Ni²⁺.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	李翠霞
	孙会珍
	金海泽
	张幽幽
	杨轩
	李文生

关键词 ：介孔RGO-TiO₂薄膜, 浸渍-提拉法, 光催化, 协同作用, Ni²⁺, SDBS

Abstract：The mesoporous RGO-TiO₂ thin films were synthesized by dipping-coating assisted heat treatment and ultraviolet lamp irradiation reduction with tetrabutyl titanate (TBT), natural flake graphite as raw materials and polyvinylpyrrolidone (PVP) as mesoporous template. The structure, morphology and properties of samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), specific surface area (BET), UV-Vis diffuse reflectance spectra (UV-Vis DRS) and Fourier transform infrared (FTIR). The reaction property of the removal of Ni²⁺and SDBS by photocatalysis of mesoporous RGO-TiO₂ thin films were evaluated with Ni²⁺ and SDBS as target pollutants. The GO amount and the effects of pH on its catalytic performance were discussed. The photocatalytic reduction of Ni²⁺ and photocatalytic oxidation of SDBS in Ni²⁺/SDBS co-existed system were further studied under the optimum condition. The results showed that the mesoporous RGO-TiO₂ thin film had the highest photocatalytic efficiency for single system Ni²⁺ and SDBS with the content of 1.0wt% GO; The reduction efficiency of Ni²⁺ and the degradation efficiency of SDBS were the highest when the pH values were 7.5 and 6, respectively. In summary, the removal efficiency of Ni²⁺ and SDBS in the co-existed system was better than that of the single system under the additions that the amount of GO was 1.0wt% and pH≈6. The reduction rate of Ni²⁺ was 87.9% and the oxidation rate of SDBS was 95.5%. In this present contribution, the mechanism of synergistic photocatalysis was further explored. It can be concluded that the Ni²⁺ synchronous reduction occured by the photogenerated electrons and the oxidation producted CO₂·^- free radical when the TiO₂-SDBS surface complex was oxidized under the excitation of ultraviolet light.

Key words： mesoporous RGO-TiO₂ thin films dipping-coating photocatalysis synergy Ni²⁺ SDBS

收稿日期: 2020-08-31

PACS:

X703.5

基金资助:国家自然科学基金资助项目（51764039）

通讯作者: 李文生,教授,liws@lut.edu.cn E-mail: liws@lut.edu.cn

作者简介: 李翠霞(1972-),女,河北卢龙人,副教授,博士,主要从事无机功能材料的制备及其在环境领域中的应用研究.发表论文30余篇.

引用本文:

李翠霞, 孙会珍, 金海泽, 张幽幽, 杨轩, 李文生. RGO改性介孔TiO₂薄膜光催化同步去除Ni²⁺和SDBS[J]. 中国环境科学, 2021, 41(4): 1663-1671. LI Cui-xia, SUN Hui-zhen, JIN Hai-ze, ZHANG You-you, YANG Xuan, LI Wen-sheng. Simultaneous removal of Ni²⁺and SDBS by RGO modified mesoporous TiO₂ thin films photocatalytic. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(4): 1663-1671.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I4/1663

[1]	李翠霞,康伟超,任一波,等.P123对rGO/m-TiO2薄膜微观结构及光催化性能的影响[J]. 中国环境科学, 2019,39(9):3754-3760. LI C X, KANG W C, REN Y B, et al. Effect of P123 on the microstructure and photocatalytic activity of rGO/mesoporous TiO2 films[J]. China Environmental Science, 2019,39(9):3754-3760.
[2]	张志伟,徐斌,张毅敏,等.GO/(CeO2-TiO2)改性复合膜紫外光催化去除氨氮、DOC[J]. 中国环境科学, 2020,40(3):1116-1122. Zhang Z W, Xu B, Zhang Y M, et al. Ultraviolet photocatalytic removal of ammonia nitrogen and DOC by GO/(CeO2-TiO2) modified composite membrane[J]. China Environmental Science, 2020,40(3):1116-1122.
[3]	Wang T T, Lin Y C, Lin M C, et al. Au-assisted methanol-hydrogenated titanium dioxide for photocatalytic evolution of hydrogen[J]. Catalysis Today, 2017,354:250-257.
[4]	Do J Y, Chava R K, Mandari K K, et al. Selective methane production from visible-light-driven photocatalytic carbon dioxide reduction using the surface plasmon resonance effect of superfine silver nanoparticles anchored on lithium titanium dioxide nanocubes (Ag@LixTiO2)[J]. Applied Catalysis B:Environmental, 2018,237:895-910.
[5]	Rangarajan G, Panchamoorthy G K, Madhav N V, et al. Present applications of titanium dioxide for the photocatalytic removal of pollutants from water:A review[J]. Journal of Environmental Management, 2020,270(110906).
[6]	Chandra R, Mukhopadhyay S, Nath M. TiO2@ZIF-8:A novel approach of modifying micro-environment for enhanced photo-catalytic dye degradation and high usability of TiO2 nanoparticles[J]. Materials Letters, 2016,164:571-574.
[7]	Zhu Y W, Shanthi M, Cai W W, et al. Graphene and graphene oxide:synthesis, properties, and applications[J]. Cheminform, 2010,22(46):3906-3924
[8]	Zhang Y, Tan Y W, Stormer H L, et al. Experimental observation of the quantum Hall effect and Berry's phase in graphene[J]. Nature, 2005, 438(7065):201-204.
[9]	Prabhakarrao N, Chandra M R, Rao T S. Synthesis of Zr doped TiO2/reduced graphene oxide (RGO) nanocomposite material for efficient photocatalytic degradation of eosin blue dye under visible light irradiation[J]. Journal of Alloys and Compounds, 2017,694:596-606
[10]	Wang H L, Liu X H. Preparation of silver nanoparticle loaded mesoporous TiO2 and its photocatalytic property[J]. Journal of Inorganic Materials, 2016,31(5):555-560.
[11]	李翠霞,金海泽,杨志忠,等.介孔RGO/TiO2复合光催化材料的制备及光催化性能[J]. 无机材料学报, 2017,32(4):357-364. Li C X, Jin H Z, Yang Z Z, et al. Preparation and photocatalytic properties of mesoporous RGO/TiO2 composites[J]. Journal of Inorganic Materials, 2017,32(4):357-364.
[12]	吴强红.rGO-TiO2薄膜的制备及光催化性研究[D]. 兰州:兰州理工大学, 2016. Wu Q H. Study on the preparation and photocatalytic activity of rGO-TiO2 thin films[D]. Lan Zhou:Lanzhou University of Technology, 2016.
[13]	Hummers W S, Offeman R E. Preparation of graphitic oxide[J]. American Chemical Society, 1958,208:1334-1339.
[14]	Williams G, Seger B, Kamat P V. TiO2-graphene nanocomposites. uv-assisted photocatalytic reduction of graphene oxide[J]. Acs Nano, 2008,2(7):1487-1491.
[15]	Meyer J C, Geim A K, Katsnelson M I, et al. On the roughness of single-and bi-layer graphene membranes[J]. Solid State Communications, 2007,143(1/2):101-109.
[16]	李翠霞,金海泽,谭高伟,等. rGO/TiO2复合光催化剂的制备及光催化性能[J]. 中国环境科学, 2017,37(2):570-576. Li C X, Jin H Z, Tan G W, et al. The preparation and photocatalytic activity of rGO/TiO2 composite photocatalyst[J]. China Environmental Science, 2017,37(2):570-576.
[17]	Storck S, Bretinger H, Maier W F. Characterization of micro-and mesoporous solids by physisorption methods and pore-size analysis[J]. Applied Catalysis A:General, 1998,174(1/2):137-146.
[18]	Burda C, Chen X. The electronic origin of the visible-light absorption properties of c-, n-and s-doped TiO2 nanomaterials[J]. Journal of the American Chemical Society, 2008,130(15):5018-5019.
[19]	Vasudevan P, Thomas S, Biju P R, et al. Synthesis and structural characterization of sol-gel derived titania/poly (vinyl pyrrolidone) nanocomposites[J]. Journal of Sol Gel Science & Technology, 2012, 62(1):41-46.
[20]	尹竞,廖高祖,朱冬韵,等.G-C3N4/石墨烯复合材料的制备及光催化活性的研究[J]. 中国环境科学, 2016,36(3):735-740. Yin J, Liao G Z, Zhu D Y, et al Preparation and photocatalytic activity of g-C3N4/rGO composite[J]. China Environmental Science, 2016, 36(3):735-740.
[21]	杨勇辉,孙红娟,彭同江,等.石墨烯薄膜的制备和结构表征[J]. 物理化学学报, 2011,27(3):736-742. Yang Y H, Sun H J, Peng T J, et al. Synthesis and structural characterization of graphene-based membranes[J]. Acta Physico-Chimica Sinica, 2011,27(3):736-742.
[22]	Nethravathi C, Rajamathi M. Chemically modified graphene sheets produced by the solvothermal reduction of colloidal dispersions of graphite oxide[J]. Carbon, 2008,46(14):1994-1998.
[23]	马婷芳,史铁钧.聚乙烯吡咯烷酮的性能,合成及应用[J]. 应用化工, 2002,(3):16-19. Ma T F, Shi T J. Properties, synthesis and applications of PVP[J]. Applied Chemical Industry, 2002,(3):16-19.
[24]	Sakthivel S, Kisch H. Daylight photocatalysis by carbon-modified titanium dioxide[J]. Angewandte Chemie International Edition, 2003, 42(40):4908-4911.
[25]	Williams G, Seger B, Kamat P V. TiO2-graphene nanocomposites. UV-assisted photocatalytic reduction of graphene oxide[J]. ACS nano, 2008,2(7):1487-1491.
[26]	柴晴雯,吕艳,张周,等.Cu2O@ZnO复合光催化剂对难生物降解有机物的光降解[J]. 中国环境科学, 2019,39(7):2822-2830. Chai Q W, Lv Y, Zhang Z, et al. Photodegradation of refractory organic compounds by Cu2O@ZnO composite photocatalyst[J]. China Environmental Science, 2019,39(7):2822-2830.
[27]	Dreyer D R, Sungjinpark, Bielawski C W, et al. The chemistry of graphene oxide[J]. Chemical Society Reviews, 2009,39(1):228-240.
[28]	Xie G, Wang H, Zhou Y Y, et al. Simultaneous remediation of methylene blue and Cr(VI) by mesoporous BiVO4photocatalyst under visible-light illumination[J]. Journal of the Taiwan Institute of Chemical Engineers, 2020,112:357-365.
[29]	Chen F, Yu C, Wei L, et al. Fabrication and characterization of ZnTiO3/Zn2Ti3O8/ZnO ternary photocatalyst for synergetic removal of aqueous organic pollutants and Cr(VI) ions[J]. Science of the Total Environment, 2019,706:136026.
[30]	Liu E, Du Y, Bai X, et al. Synergistic improvement of Cr (VI) reduction and RhB degradation using RP/g-C3N4 photocatalyst under visible light irradiation[J]. Arabian Journal of Chemistry, 2020,13(2):3836-3848.
[31]	Shao N, Li S, Yan F, et al. An all-in-one strategy for the adsorption of heavy metal ions and photodegradation of organic pollutants using steel slag-derived calcium silicate hydrate[J]. Journal of Hazardous Materials, 2020,382:121120.
[32]	Bano Z, Saeed R M Y, Zhu S, et al. Mesoporous CuS nanospheres decorated rGO aerogel for high photocatalytic activity towards Cr(VI) and organic pollutants[J]. Chemosphere, 2020,246:125846.
[33]	Javad Saien, Amir Azizi. Simultaneous photocatalytic treatment of Cr(VI), Ni(Ⅱ) and SDBS in aqueous solutions:Evaluation of removal efficiency and energy consumption[J]. Process Safety and Environmental Protection, 2015,95:114-125.
[34]	Wang N, Zhu L, Huang Y, et al. Drastically enhanced visible-light photocatalytic degradation of colorless aromatic pollutants over TiO2via a charge-transfer-complex path:A correlation between chemical structure and degradation rate of the pollutants[J]. Journal of Catalysis, 2009,266(2):199-206.
[35]	Dozzi M V, Saccomanni A, Selli E. Cr(VI) photocatalytic reduction:Effects of simultaneous organics oxidation and of gold nanoparticles photodeposition on TiO2[J]. Journal of Hazardous Materials, 2003,99:188-195.
[36]	Wang N, Zhu L, Deng K, et al. Visible light photocatalytic reduction of Cr(VI) on TiO2 in situ modified with small molecular weight organic acids[J]. Applied Catalysis B:Environmental, 2010,95(3/4):400-407.