纳米TiO2薄膜耦合光催化氧化还原反应脱除水中无机氮

doi:10.7517/j.issn.1674-0475.2006.01.17

影像科学与光化学 ›› 2006, Vol. 24 ›› Issue (1): 17-27.DOI: 10.7517/j.issn.1674-0475.2006.01.17

纳米TiO₂薄膜耦合光催化氧化还原反应脱除水中无机氮

马慧¹, 柳丽芬^1,2, 杨凤林¹, 张兴文¹, 余济美³

1. 大连理工大学, 环境与生命学院, 辽宁, 大连, 116023;
2. 大连理工大学, 纳米材料科学研究中心, 辽宁, 大连, 116023;
3. 香港中文大学, 化学系, 香港, 沙田

收稿日期:2005-08-01 修回日期:2005-10-08 出版日期:2006-01-23 发布日期:2006-01-23
通讯作者: 柳丽芬
基金资助:
国家自然科学基金(20477006).

Immobilized TiO₂ and its Photocatalytic Application in Removing Nitrogen from Water

MA Hui¹, LIU Li-fen^1,2, YANG Feng-lin¹, ZHANG Xing-wen¹, Jimmy C. Yu³

1. School of Environmental and Biological Science & Technology, Dalian University of Technology, Dalian 116023, Liaoning, P.R. China;
2. Center for Nanomaterial and Science, Dalian University of Technology, Dalian 116023, Liaoning, P.R. China;
3. Department of Chemistry, The Chinese University of Hong Kong, Shatin, HKSAR

Received:2005-08-01 Revised:2005-10-08 Online:2006-01-23 Published:2006-01-23

摘要/Abstract

摘要： 由溶胶-凝胶法制备了固定化二氧化钛薄膜,研究了薄膜催化剂光催化脱除含氨氮-亚硝酸氮混合液中无机氮的活性.考察了溶胶制备工艺、催化反应条件(尤其pH)对光催化活性的影响.实验证明:酸性条件有利于亚硝酸氮的还原,碱性条件有利于氨氮的氧化,通过调节pH可以获得光催化氧化氨氮和还原亚硝酸氮耦合效果.如果加入甲酸维持酸性务件,反应0.5 h后再将pH调回碱性,可以大大提高光催化脱氮的效果:经过2 h的光催化反应,二氧化钛膜催化总氮去除率可达50%以上.经多次试验证明附载二氧化钛薄膜不脱落,光催化活性未见减弱,可重复利用.提出了光催化脱氮的反应机理.

关键词: 溶胶-凝胶法, 二氧化钛, 光催化, 脱氮

Abstract: The photocatalytic nitrogen removal from water by coupling photocatalytic oxidation of ammonia and reduction of nitrite were studied, using an immobilized TiO₂ catalyst. The preparation of the catalyst films, their photocatalytic activities and effect of conditional factors(especially pH)on nitrogen removal were also investigated. Under N₂ flow, Nitrite reduction was the major reaction under acidic condition, while ammonia oxidation was the main reaction under basic condition. By adjusting the pH value of the solution using formic acid, photocatalysis carried out under acidic condition first for 0.5 h to 1 h, then under basic condition by adjusting pH, increased the overall nitrogen removal level. The result of the experiment showed that after 2 h irradiation, the removal of TN more than 50% by the photocatalytic process was achieved. The catalyst film can be used repeatedly without decline of activity. A reaction mechanism was proposed for photocatalytic nitrogen removal.

Key words: Sol-Gel, TiO₂, photocatalysis, nitrogen removal

中图分类号:

马慧, 柳丽芬, 杨凤林, 张兴文, 余济美. 纳米TiO₂薄膜耦合光催化氧化还原反应脱除水中无机氮[J]. 影像科学与光化学, 2006, 24(1): 17-27.

MA Hui, LIU Li-fen, YANG Feng-lin, ZHANG Xing-wen, Jimmy C. Yu. Immobilized TiO₂ and its Photocatalytic Application in Removing Nitrogen from Water[J]. Imaging Science and Photochemistry, 2006, 24(1): 17-27.

参考文献

[1] Lee J,Park H W,Choi W.Selective photocatalytic oxidation of NH₃ to N₂ on platinized TiO₂ in water[J].Environ.Sci.Technol.,2002,(36):5462-5468.
[2] Shivaraman N,Shivaraman G.Anammox a novel microbial process for ammonia removal[J].Current Science,2003,84(12):1507-1508.
[3] 武婕,崔建国.水中无机氮的光催化处理[J].科技情报开发与经济,2005,15(5):174-176.Wu J,Cui J G.Photocatalysis degradation of inorganic nitrogen in water[J].Sci/Tech Information Development & Economy,2005,15(5):174-176.
[4] 高文亮,关新新,等.饮用水中硝酸根的催化还原研究进展[J].环境污染治理技术与设备,2004,5(5):1-5.Gao W L,Guan X X,et al.Advance in studies of catalytic reduction of nitrate in drinking water[J].Techniques and Equipment for Environmental Pollution Control,2004,5(5):1-5.
[5] 徐锐,尹卫平.光催化氧化法处理氨氮废水的研究[J].郑州工程学院学报,2003,24(3):84-87.Xu R,Yin W P.Research on the heterogeneous photocatalytic degradation of N-NH4+ from waste water[J].Journal of Zheng Zhou Institute of Technology,2003,24(3):84-87.
[6] Bems B,Jentoft F C,Schlogl R.Photoinduced decomposition of nitrate in drinking water in the presence of titania and humic acids[J].Applied Catalysis B:Environmental,1999,(20):155-163.
[7] Penpolcharoen M,Amall R,Brungs M.Degradation of sucrose and nitrate over titania coated nano-hematite photocatalysts[J].Journal of Nanoparticle Research,2001,(3):289-302.
[8] Li Y,Wasgestian F.Photocatalytic reduction of nitrate ions on TiO₂ by oxalic acid[J].J.Photochem.Photobiol.,A Chem.,1998,112(2-3):255-259.
[9] 曹广秀,刘朝辉,李贯良.纳米二氧化钛光催化处理废水中亚硝酸根的研究[J].应用化工,2004,33(1):40-42.Cao G X,Liu Z H,Li G L.Study on the treatment of content of NO₂^- in waste water through photocatalysis mechanism of nanometer titanium dioxide[J].Applied Chemical Industry,2004,33(1):40-42.
[10] 李威,柳丽芬,杨凤林.以ACF为模板制备掺氮TiO₂及其光催化脱氨氮研究[J].感光科学与光化学,2005,23(5):374-381.Li W,Liu L F,Yang F L.Preparation of N doped TiO₂ by using ACF as template and its photocatalytic application in removing nitrogen from water[J].Photographic Science and Photochemistry,2005,23(5):374-381.
[11] Xu Y,Zheng W,Liu W.Enhanced photocatalytic activity of supported TiO₂ dispersing effect of SiO₂[J].J.Photochem.Photobiol.,A.Chem.,1999,122:57-60.
[12] 余家国,赵修建,陈文梅.TiO₂多孔纳米薄膜的溶胶-凝胶法制备和光催化特性研究[J].玻璃与搪瓷,1999,27(5):9-15.Yu J G,Zhao X J,Chen W M.Photocatalytic properties of porous TiO₂ nanometer thin films prepared by the Sol-Gel method[J].Glass and Porcelain Enamel,1999,27(5):9-15.
[13] 国家环境保护总局编委会.水和废水监测分析方法[M].北京:中国环境科学出版社,2002:277-281,268-274,258-261.Editing Committee for State Environmental Protection Administration of China.Analysis Methods for Water and Wastewater Monitoring[M].Beijing:China Environmental Science Publisher,2002,258-261,268-274,277-281.
[14] 卢萍,姚明明,张颖.具有催化活性TiO₂薄膜的制备及表征[J].云南民族大学学报(自然科学版),2003,12(4):207-209.Lu P,Yao M M,Zhang Y.Preparation and characterization of photocatalytic TiO₂ film[J].Journal of Yunnan University for Nationalities(Natural Sciences Edition),2003,12(4):207-209.
[15] 余家国,赵修建.热处理工艺对TiO₂纳米薄膜光催化性能的影响[J].硅酸盐学报,1999,27(6):9-15.Yu J G,Zhao X J.Influence of heat treatment processing on the photocatalytic properties of nanometric TiO₂ thin films[J].Journal of the Chinese Ceramic Society,1999,27(6):9-15.
[16] Zhu X D,Castleberry S R,Nanny M A.Effects of pH and catalyst concentration on photocatalytic oxidation of aqueous ammonia and nitrite in titanium dioxide suspensions[J].Environ.Sci.Technol.,2005,39:3784-3791.

纳米TiO₂薄膜耦合光催化氧化还原反应脱除水中无机氮

Immobilized TiO₂ and its Photocatalytic Application in Removing Nitrogen from Water

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	李玥, 李红英, 常玉雪, 周宏艳, 于翔. MoS₂/TiO₂纳米管阵列的一步沉积法制备及光电性能研究[J]. 影像科学与光化学, 2018, 36(4): 331-339.
[2]	李玥, 宋育泽, 陶雁忠, 高风仙, 汤宁. CdS/TiO₂复合纳米网的制备及光催化性能研究[J]. 影像科学与光化学, 2018, 36(3): 275-282.
[3]	李玲, 杜云舒, 王璇, 韩建, 王传义. 甲醛气体在ZnO表面光降解的机理研究[J]. 影像科学与光化学, 2018, 36(2): 171-177.
[4]	吴世康. 光催化中表面等离子体与半导体间的电子转移与能量转移[J]. 影像科学与光化学, 2018, 36(1): 1-13.
[5]	Samuel Lascio, 籍海峰. 磷纳米材料的光学、光电子和光催化应用[J]. 影像科学与光化学, 2017, 35(5): 587-602.
[6]	张庆宝, 刘强. 可见光催化需氧氧化在有机合成中的应用[J]. 影像科学与光化学, 2017, 35(5): 614-625.
[7]	桂梦茜, 俞洋, 朱诚逸, 刘宏芳, 王锋. 基于金属钴配合物的均相光催化还原二氧化碳研究进展[J]. 影像科学与光化学, 2017, 35(5): 649-657.
[8]	彭成云, 陈勇. 苝衍生物光催化氧化硫醚的研究[J]. 影像科学与光化学, 2017, 35(5): 675-685.
[9]	聂坤, 杨汉培, 孙慧华, 崔素珍, 吴俊明. 新型Fe掺杂钙钛矿型KMgF₃光催化剂制备及性能[J]. 影像科学与光化学, 2017, 35(1): 61-69.
[10]	朱哲欣, 叶美英. 光催化微反应器中水样光催化降解及Cd²⁺在线检测[J]. 影像科学与光化学, 2016, 34(5): 444-451.
[11]	张亚婷, 李可可, 任绍昭, 王黛玉, 周安宁, 邱介山. 金属改性煤基石墨烯复合材料的制备及其光催化性能[J]. 影像科学与光化学, 2016, 34(5): 475-481.
[12]	王勐, 夏静, 朱丹丹, 王磊, 孟祥敏. Fe掺杂ZnO空心微球的制备与光催化性能[J]. 影像科学与光化学, 2016, 34(3): 245-251.
[13]	蒋伟, 武祥. ZnS微米花的水热合成及光催化性质研究[J]. 影像科学与光化学, 2016, 34(3): 252-256.
[14]	黄奔, 李玄泽, 王磊, 夏静, 朱丹丹, 孟祥敏. 钼网衬底上大面积硅纳米线的制备及其光催化性能研究[J]. 影像科学与光化学, 2016, 34(3): 257-264.
[15]	刘思迪, 张俊虎. 利用二氧化钛静电纺丝和透明质酸甲基丙烯酸酯构筑用于细胞培养的纤维凝胶结构[J]. 影像科学与光化学, 2016, 34(3): 281-287.