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“光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响

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王徐越, 孙振亚, 谢裕兴, 杨红刚. “光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响[J]. 环境化学, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
引用本文: 王徐越, 孙振亚, 谢裕兴, 杨红刚. “光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响[J]. 环境化学, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
shu
WANG Xuyue, SUN Zhenya, XIE Yuxing, YANG Honggang. “Photocatalysis Iron Cycling” effect on the photocatalytic activity of self-assembled TiO2-FeOOH nano-films[J]. Environmental Chemistry, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
Citation: WANG Xuyue, SUN Zhenya, XIE Yuxing, YANG Honggang. “Photocatalysis Iron Cycling” effect on the photocatalytic activity of self-assembled TiO2-FeOOH nano-films[J]. Environmental Chemistry, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
shu

“光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响

  • 1.

    武汉理工大学 资源与环境工程学院, 武汉, 430070;

  • 2.

    武汉理工大学 材料研究与测试中心, 武汉, 430070;

  • 3.

    中国葛洲坝集团水务运营有限公司, 武汉, 430000

  • 基金项目:

    国家自然科学基金（41372054）资助.

“Photocatalysis Iron Cycling” effect on the photocatalytic activity of self-assembled TiO2-FeOOH nano-films

  • 1.

    School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan, 430070, China;

  • 2.

    Centre for Materials Research and Analysis, Wuhan University of Technology, Wuhan, 430070, China;

  • 3.

    China Gezhouba Group Water Operation Co., LTD., Wuhan, 430000, China

  • Fund Project: Supported by the National Natural Foundation of China (41372054).

  • 摘要: 通过分子自组装法，制备了改性钠基蒙脱石基负载不同层序TiO2-FeOOH纳米复合膜，以甲砜霉素溶液为目标污染物，研究自然光下复合膜的光催化活性.采用透射电镜（TEM）、紫外-可见光吸收光谱（UV-Vis）、傅里叶变换红外光谱（FT-IR）对实验样品进行表征.结果表明，由锐钛矿和针铁矿纳米晶构成的复合膜将材料光谱响应范围扩展至可见光区.铁在外层时，复合膜具有更高的光降解效率.在光降解甲砜霉素过程中，以菲啰嗪作为分子探针，测定溶液中Fe2+的相对含量；用X射线光电子能谱（XPS）测定固体表面铁和其他元素的化学态及其相应含量的变化.研究铁的反应动力学发现，与其他光催化剂不同，含铁催化剂在光催化过程中于固液界面上发生了一种"光催化铁循环"作用.即单层膜和复合膜，在固液界面上都存在由光催化引发的，铁的多重氧化还原反应协同作用循环驱动的动态过程，且铁循环反应加速了目标污染物的光催化降解.分析光催化反应前后Ti 2p、O 1s XPS谱图，发现反应后复合膜的表面未产生低价态钛离子，仅含高活性Ti4+，表明"光催化铁循环"作用有利于维持催化剂的光催化活性.这为今后设计高效光催化剂提供了新的思路.
    Abstract: In this paper, different sequence TiO2-FeOOH nanocompsite films on Na-modifying montmorillonite (MdMmt) substrate were prepared by a molecular self-assembly method. The photocatalytic activity of TiO2-FeOOH composite films under natural light irradiation in the thiamphenicol solution was studied. The samples were carried out to characterize with TEM, UV-Vis, FT-IR. The results indicated that the TiO2-FeOOH nano-films were composed of anatase and goethite, their UV-Vis spectras response range in photocatalysis extended to visible light region. When goethite coating in the outer layer, the composite films had higher photodegradation rate. During photodegradation of thiamphenicol, the relative content of Fe2+ in solution was determined by using ferrozine as a molecular probe, chemical states and their corresponding content changes of iron and other elements on the solid surface were determined with XPS. Being different with other photocatalysts, we found that iron-containing catalysts had "Photocatalysis Iron Cycling" at solid-liquid interface by studying the reaction kinetics of iron during the photocatalysis. That is, the dynamic process existed in goethite monolayer and iron-titanium composite membrane, that was induced by photocatalysis and driven by the multiple redox reactions of iron at solid-liquid interface. And the reaction of iron cycling in the process could improve the degradation rate of the pollutants. Through analyzing the Ti 2p and O 1s XPS spectra of pre-and post-photocatalytic reaction, we found that the surface of the composite film contained only Ti4+, didn't produce low-valent titanium. So the results showed that the "Photocatalysis Iron Cycling" was conducive to maintain the photocatalytic activity of the materials. The experimental results could provide the new ideas for the design of high-efficiency photocatalysts.
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  • [1] 林婵. TiO2纳米材料的制备、改性及其光催化性能研究[D]. 青岛:中国海洋大学, 2014, 1-15. LIN C. Preparation, modification of TiO2 nanomaterials and their photocatalytic performance study[D].Qingdao:Ocean University of China, 2014

    , 1-15(in Chinese).

    [2] 张明, 成杰民, 董文平,等. TiO2光催化剂失活机理与再生研究进展[J]. 硅酸盐通报, 2013, 32(10):2068-2074.

    6MING Z, CHENG J, DONG W, et al. Research progress of deactivation mechanism and regeneration of titanium oxide photocatalyst[J]. Bulletin of the Chinese Ceramic Society, 2013, 32(10):2068-2074(in Chinese).

    [3] 孙振亚, 祝春水, 龚文琪. 铁(氢)氧化物矿物对有机污染物的光催化氧化作用[J]. 矿物学报, 2003, 23(4):341-348.

    SUN Z Y, ZHU C S, GONG W Q. Photocatalysis of organic contaminants by iron (hydr) oxide minerals in water[J]. Acta Mineralogica Sinica, 2003, 23(4):341-348(in Chinese).

    [4] 刘承帅, 李芳柏, 陈曼佳,等. Fe(Ⅱ)催化水铁矿晶相转变过程中Pb的吸附与固定[J]. 化学学报, 2017, 75(6):621-628.

    LIU C S, LI F B, CHEN M J, et al. Adsorption and stabilization of lead during Fe(Ⅱ)-catalyzed phase transformation of ferrihydrite[J]. Acta Chimica Sinica -Chinese Edition-, 2017, 75(6):621-628(in Chinese).

    [5] LATTA D E, BACHMAN J E, SCHERER M M. Fe electron transfer and atom exchange in goethite:influence of Al-substitution and anion sorption.[J]. Environmental Science & Technology, 2012, 46(19):10614-10623.
    [6] TISHCHENKO V, MEILE C, SCHERER M M, et al. Fe2+ catalyzed iron atom exchange and re-crystallization in a tropical soil[J]. Geochimica Et Cosmochimica Acta, 2015, 148(10):191-202.
    [7] LATTA D E, GORSKI C A, SCHERER M M. Influence of Fe2+-catalysed iron oxide recrystallization on metal cycling.[J]. Biochemical Society Transactions, 2012, 40(6):1191-1197.
    [8] LARESECASANOVA P, CWIERTNY D M, SCHERER M M. Nanogoethite formation from oxidation of Fe(Ⅱ) sorbed on aluminum oxide:implications for contaminant reduction[J]. Environmental Science & Technology, 2010, 44(10):3765-3771.
    [9] 谢裕兴, 孙振亚, 李涵,等. 石英基多层纳米TiO2-FeOOH复合材料的制备和显微结构的表征[J]. 电子显微学报, 2017, 36(3):207-213.

    14XIE Y X, SUN Z Y, HAN L, et al. Study on the photocatalysis coupling enhancement effect of quartz based nano TiO2-FeOOH composite layer[J]. Journal of Chinese Electron Microscopy Society, 2017, 36(3):207-213(in Chinese).

    [10] SUN Z Y, HE X, DU J, et al. Synergistic effect of photocatalysis and adsorption of nano-TiO2 self-assembled onto sulfanyl/activated carbon composite.[J]. Environmental Science & Pollution Research International, 2016, 23(21):1-8.
    [11] VIOLLIER E, INGLETT P W, HUNTER K, et al. The ferrozine method revisited:Fe(Ⅱ)/Fe(Ⅲ) determination in natural waters[J]. Applied Geochemistry, 2000, 15(6):785-790.
    [12] 李媛, 陈奇洲, 欧国荣,等. 菲咯嗪分光光度法测定水中的总铁[J]. 解放军预防医学杂志, 2003, 21(1):30-32.

    LI Y, CHEN Q Z, OU G R, et al. Spectrophotometric determination of total iron in water with ferrozine[J]. Journal of Preventive Medicine of Chinese People's Liberation Army 2003, 21(1):30-32(in Chinese).

    [13] 周佳欣. 氯霉素类药物辐射和光解特性及机理研究[D]. 上海:上海大学, 2011, 40-60. ZHOU J X. Study on the degradation characteristics and mechanism of chloramphenicols (CAPs) induced by the radiolysis and photolysis[D].Shanghai:Shanghai University, 2011, 40

    -60(in Chinese).

    [14] 许亚改, 刘聚祥, 刘静,等. 甲砜霉素羟丙基-β-环糊精包合物的制备与鉴定[J]. 河北农业大学学报, 2009, 32(1):99-102.

    XU Y G, LIU J X, LIU J, et al. Preparation and identification of inclusion complex of thiamphenicol HP-β-cyclodextrin[J].Journal of Agricultural University of Hebei, 2009, 32(1):99-102(in Chinese).

    [15] 李娣, 施伟东. 可见光光催化降解抗生素研究进展[J].催化学报, 2016, 37(6):792-799.

    LI D, SHI W D. Recent developments in visible-light photocatalytic degradation of antibiotics[J]. Chinese Journal of Catalysis, 2016, 37(6):792-799(in Chinese).

    [16] 袁东海, 张孟群, 高士祥,等. 几种粘土矿物和粘粒土壤吸附净化磷素的性能和机理[J]. 环境化学, 2005, 24(1):7-11.

    YUAN D H, ZHANG M Q. The abilities and mechanisms of adsorption phosphorus in some clay minerls and soils[J]. Environmental Chemistry, 2005, 24(1):7-11(in Chinese).

    [17] 于洪涛, 全燮. 纳米异质结光催化材料在环境污染控制领域的研究进展[J]. 化学进展, 2009, 21(2):406-419.

    YU H T, QUAN X. Nano-heterojunction photocatalytic materials in environmental pollution controlling[J]. Progress in Chemistry, 2009, 21(2):406-419(in Chinese).

    [18] RAWAL S B, CHAKRABORTY A K, WAN I L. FeOOH/TiO2 heterojunction for visible light photocatalyst heterojunction of FeOOH and TiO2 for the formation of visible light photocatalyst[J]. Bulletin of the Korean Chemical Society, 2009, 30(11):2613-2616.
    [19] CHEN D, HU S J, LI G H. Preparation and photocatalytic activity of TiO2/FeOOH nanocomposite[J]. Advanced Materials Research, 2012, 535-537:219-222.
    [20] XU Z, ZHANG M, WU J, et al. Visible light-degradation of azo dye methyl orange using TiO2/β-FeOOH as a heterogeneous photo-Fenton-like catalyst.[J]. Water Science & Technology A Journal of the International Association on Water Pollution Research, 2013, 68(10):2178-2185..
    [21] 张德莉, 黄应平, 罗光富,等. Fenton及Photo-Fenton反应研究进展[J]. 环境化学, 2006, 25(2):121-127.

    28ZHANG D L, HUANG Y P, LUO G F, et al. Research progress of fenton and photo-fenton reaction[J]. Environmental Chemistry, 2006, 25(2):121-127(in Chinese).

    [22] 李功虎, 马胡兰, 安纬珠. 纳米二氧化钛气相光催化降解三氯乙烯[J]. 催化学报, 2000, 21(4):350-354.

    LI G H, MA H L, AN W Z. Gas phase photocatalytic oxidation of trichloroethylene on nanoscale titanium dioxide[J]. Chinese Journal of Catalysis, 2000, 21(4):350-354(in Chinese).

    [23] 陈崧哲, 张彭义, 祝万鹏,等. 钛、铝和玻璃上TiO2光催化膜的失活研究[J]. 无机化学学报, 2004, 20(11):1265-1272.

    CHEN S Z, ZHANG P Y, ZHU W P, et al. Deactivation of TiO2 films on titanium, aluminums and glass substrates[J]. Chinese Journal of Inorganic Chemistry, 2004, 20(11):1265-1272(in Chinese).

    [24] BHARGAVA G, GOUZMAN I, CHUN C M, et al. Characterization of the "native" surface thin film on pure polycrystalline iron:A high resolution XPS and TEM study[J]. Applied Surface Science, 2007, 253(9):4322-4329.
    [25] ZHIDKOV I S, KURMAEV E Z, KOROTIN M A, et al. Characterization of solution processed TiOx buffer layers in inverted organic photovoltaics by XPS and DFT studies[DB OL].[2014-11-6] https://arxiv.org/abs/1411.1561,
    [26] GUEDIDI H, REINERT L, LÉVÊQUE J M, et al. The effects of the surface oxidation of activated carbon, the solution pH and the temperature on adsorption of ibuprofen[J]. Carbon, 2013, 54(29):432-443.
    [27] SUN R D, NAKAJIMA A, WATANABE I, et al. TiO2-coated optical fiber bundles used as a photocatalytic filter for decomposition of gaseous organic compounds[J]. Journal of Photochemistry & Photobiology A Chemistry, 2000, 136(1):111-116.
    [28] EINAGA H, FUTAMURA S, IBUSUKI T. Heterogeneous photocatalytic oxidation of benzene, toluene, cyclohexene and cyclohexane in humidified air:comparison of decomposition behavior on photoirradiated TiO catalyst[J]. Applied Catalysis B Environmental, 2002, 38(3):215-225.
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  • 收稿日期:  2018-01-02
  • 刊出日期:  2018-11-15
王徐越, 孙振亚, 谢裕兴, 杨红刚. “光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响[J]. 环境化学, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
引用本文: 王徐越, 孙振亚, 谢裕兴, 杨红刚. “光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响[J]. 环境化学, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
shu
WANG Xuyue, SUN Zhenya, XIE Yuxing, YANG Honggang. “Photocatalysis Iron Cycling” effect on the photocatalytic activity of self-assembled TiO2-FeOOH nano-films[J]. Environmental Chemistry, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
Citation: WANG Xuyue, SUN Zhenya, XIE Yuxing, YANG Honggang. “Photocatalysis Iron Cycling” effect on the photocatalytic activity of self-assembled TiO2-FeOOH nano-films[J]. Environmental Chemistry, 2018, 37(11): 2555-2564. doi: 10.7524/j.issn.0254-6108.2018010204
shu

“光催化铁循环作”用对自组装TiO2-FeOOH复合膜活性的影响

  • 1.  武汉理工大学 资源与环境工程学院, 武汉, 430070;
  • 2.  武汉理工大学 材料研究与测试中心, 武汉, 430070;
  • 3.  中国葛洲坝集团水务运营有限公司, 武汉, 430000
  • 收稿日期:  2018-01-02
基金项目:

国家自然科学基金（41372054）资助.

摘要: 通过分子自组装法，制备了改性钠基蒙脱石基负载不同层序TiO2-FeOOH纳米复合膜，以甲砜霉素溶液为目标污染物，研究自然光下复合膜的光催化活性.采用透射电镜（TEM）、紫外-可见光吸收光谱（UV-Vis）、傅里叶变换红外光谱（FT-IR）对实验样品进行表征.结果表明，由锐钛矿和针铁矿纳米晶构成的复合膜将材料光谱响应范围扩展至可见光区.铁在外层时，复合膜具有更高的光降解效率.在光降解甲砜霉素过程中，以菲啰嗪作为分子探针，测定溶液中Fe2+的相对含量；用X射线光电子能谱（XPS）测定固体表面铁和其他元素的化学态及其相应含量的变化.研究铁的反应动力学发现，与其他光催化剂不同，含铁催化剂在光催化过程中于固液界面上发生了一种"光催化铁循环"作用.即单层膜和复合膜，在固液界面上都存在由光催化引发的，铁的多重氧化还原反应协同作用循环驱动的动态过程，且铁循环反应加速了目标污染物的光催化降解.分析光催化反应前后Ti 2p、O 1s XPS谱图，发现反应后复合膜的表面未产生低价态钛离子，仅含高活性Ti4+，表明"光催化铁循环"作用有利于维持催化剂的光催化活性.这为今后设计高效光催化剂提供了新的思路.

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