以钛酸四丁酯、氟化铵、硼酸为原料,采取改进的溶胶-凝胶法制备了氟、硼共掺杂的纳米二氧化钛粉体.XRD结果显示氟、硼共掺杂不仅可以抑制晶粒生长,还可以阻止锐钛矿相向金红石相的转变.当氟、硼物质的量比为5∶ 20时,其表现出更好的可见光响应.XPS 结果表明:氟和硼分别和钛形成了F-Ti键和B-Ti键,它们的形成可提高价带中光生空穴的氧化能力和拉窄二氧化钛的带隙,从而提高了其可见光照射下的光催化活性.可见光照射下降解4-氯苯酚,结果表明:经600 ℃煅烧2 h的样品,氟、硼物质的量比为5∶ 20,其降解率分别是单掺杂和纯二氧化钛的1.5到3倍.总有机碳(TOC)分析结果表明4-氯苯酚在可见光照射下被光催化剂有效地矿化.
Boron and fluorine codoped TiO_2 powders were prepared by hydrolysis of titanium tetra-n-butyl oxide in a mixed NH_4F-H_3BO_3-H_2O solution. The XRD results showed that the co-doping of boron and fluorine could not only efficiently inhibit the grain growth but also suppress the phase transition of anatase to rutile. When the molar ratios of B and F to Ti are 20∶ 100 and 5∶ 100 and calcined at 600 ℃, UV-vis spectroscopy of the sample showed better visible light responding. XPS results revealed that the Ti-B bonds and Ti-F bonds have formed which could extend the absorption spectra to visible light region and enhance visible light photocatalytic activity. When the molar ratios of B and F to Ti are 20∶ 100 and 5∶ 100 and calcined at 600 ℃, the degradation rate of 4-chlorophenol (4-CP) over the sample was about 1.5 to 3.0 times higher than that for other doped samples and undoped TiO_2. The total organic carbon (TOC) removal rates of 4-CP showed that 4-CP has been mineralized efficiently with the sample under visible light illumination.
参考文献
| [1] | Zou Z G;Ye J H;Sayama K;Arakawa H .Direct splitting of water under light light irradiation with an oxide semiconductor photocatalyst[J].Nature,2001,414(06):625-627. |
| [2] | Asahi R;Morikawa T;Ohwaki T K et al.Visible-light photocatalysis in nitrogen-doped titanium oxide[J].Science,2001,293:269-271. |
| [3] | Clemens Burda;Yongbing Lou;Xiaobo Chen;Anna C. S. Samia;John Stout;James L. Gole .Enhanced Nitrogen Doping in TiO_2 Nanoparticles[J].Nano letters,2003(8):1049-1051. |
| [4] | Chen XB;Burda C .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(15):5018-5019. |
| [5] | Suil In;Alexander Orlov;Regina Berg .Effective Visible Light-Activated B-Doped and B,N-Codoped TiO2 Photocatalysts[J].Journal of the American Chemical Society,2007(45):13790-13791. |
| [6] | Li HX;Zhang XY;Huo YN;Zhu J .Supercritical preparation of a highly active S-doped TiO2 photocatalyst for methylene blue mineralization[J].Environmental Science & Technology: ES&T,2007(12):4410-4414. |
| [7] | Chen D;Yang D;Wang Q;Jiang ZY .Effects of boron doping on photocatalytic activity and microstructure of titanium dioxide nanoparticles[J].Industrial & Engineering Chemistry Research,2006(12):4110-4116. |
| [8] | Wei Zhao;Wanhong Ma;Chuncheng Chen;Jincai Zhao;Zhigang Shuai .Efficient Degradation of Toxic Organic Pollutants with Ni_2O_3/TiO_(2-x)B_x under Visible Irradiation[J].Journal of the American Chemical Society,2004(15):4782-4783. |
| [9] | Ho W K;Yu J C;Lee S C .Synthesis of hierarchical nanoporous F-doped TiO_2 spheres with visible light photocatalytic activity[J].Chemical Communications,2006,1115-1117 |
| [10] | Kazuhiko Maeda;Yoshiki Shimodaira;Byonjin Lee .Studies on TiNxOyFz as a Visible-Light-Responsive Photocatalyst[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(49):18264-18270. |
| [11] | 陈永刚,刘素文,冯光建,张华勇,王萍,于小钧.氮镧共掺杂TiO2纳米粉的溶剂热法制备及其可见光催化性能[J].硅酸盐通报,2009(01):63-66,75. |
| [12] | Jing Li;Hua Chun Zeng .Hollowing Sn-Doped TiO2 Nanospheres via Ostwald Ripening[J].Journal of the American Chemical Society,2007(51):15839-15847. |
| [13] | Yang H G;Sun C H;Qiao S Z et al.Anatase TiO_2 single crystals with a large percentage of reactive facets[J].Nature,2008,453:638-642. |
| [14] | Zhou L;Smyth-Boyle D;O'Brien P .A facile synthesis of uniform NH4TiOF3 mesocrystals and their conversion to TiO2 mesocrystals[J].Journal of the American Chemical Society,2008(4):1309-1320. |
| [15] | Sibu C.Padmanabhan;Suresh C.Pillai;John Colreavy .A Simple Sol-Gel Processing for the Development of High-Temperature Stable Photoactive Anatase Titania[J].Chemistry of Materials: A Publication of the American Chemistry Society,2007(18):4474-4481. |
| [16] | Enrique A.Reyes-Garcia;Yanping Sun;Daniel Raftery .Solid-State Characterization of the Nuclear and Electronic Environments in a Boron-Fluoride Co-doped TiO2 Visible-Light Photocatalyst[J].The journal of physical chemistry. C, Nanomaterials and interfaces,2007(45):17146-17154. |
| [17] | Qi Xiao;Jiang Zhang;Chong Xiao;Zhichun Si;Xiaoke Tan .Solar photocatalytic degradation of methylene blue in carbon-doped TiO_2 nanoparticles suspension[J].Solar Energy,2008(8):706-713. |
| [18] | Yu JC.;Yu JU.;Ho WK.;Jiang ZT.;Zhang LH. .Effects of F- doping on the photocatalytic activity and microstructures of nanocrystalline TiO2 powders[J].Chemistry of Materials,2002(9):3808-3816. |
| [19] | Nukumizu K;Nunoshige J;Takata T et al.LaTiO_2N as a visible-light (≤600 nm)-driven photocatalyst (2)[J].Journal of Physical Chemistry B,2003,107:791-797. |
| [20] | Masahiro Miyauchi;Minoru Takashio;Hiroki Tobimatsu .Photocatalytic Activity of SrTiO_3 Codoped with Nitrogen and Lanthanum under Visible Light Illumination[J].Langmuir: The ACS Journal of Surfaces and Colloids,2004(1):232-236. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%