School of Civil and Environmental Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
Water Res. 2011 Oct 15;45(16):5015-26. doi: 10.1016/j.watres.2011.07.002. Epub 2011 Jul 18.
A novel carbon-sensitized and nitrogen-doped TiO2 (C/N-TiO2) was synthesized by a facile sol-gel method using titanium butoxide as both titanium precursor and carbon source, and nitric acid as nitrogen source. The calcination temperature had a great effect on the crystal phase structure, nitrogen incorporation into the TiO2 lattice and content of carbonaceous species. The incorporated carbonaceous species could serve as photosensitizer, while the nitrogen doping could lead to the remarkable red shift of absorption edge of C/N-TiO2. The C/N-TiO2 calcinated at 300 °C (T300) exhibited the highest photocatalytic activity for sulfanilamide (SNM) degradation under irradiation of visible-light-emitting diode (vis-LED). The SNM photocatalytic degradation and mineralization were more efficient in acidic conditions due to the carbon photosensitizing effect. Insignificant inhibitory effects were observed in the presence of chloride, nitrate and sulfate, while bicarbonate, phosphate and silica could inhibit the SNM mineralization to different degrees. Acetate, ammonium and sulfate were released during SNM mineralization. T300 exhibited good photochemical stability and could be reused for 5 times with less than 10% decrease in the SNM removal efficiency. The acute toxicity of SNM solution could be reduced over prolonged photocatalysis according to the Microtox assay.
一种新型的碳敏化和氮掺杂二氧化钛(C/N-TiO2)通过简便的溶胶-凝胶法合成,以钛酸丁酯为钛前体和碳源,以硝酸为氮源。煅烧温度对晶体相结构、氮掺入 TiO2 晶格的程度和碳质物质的含量有很大的影响。掺入的碳质物质可以作为光致敏化剂,而氮掺杂可以导致 C/N-TiO2 的吸收边缘显著红移。在可见光发光二极管(vis-LED)照射下,在 300°C 煅烧的 C/N-TiO2(T300)对磺胺甲恶唑(SNM)的光催化降解表现出最高的活性。由于碳敏化作用,在酸性条件下 SNM 的光催化降解和矿化效率更高。在存在氯化物、硝酸盐和硫酸盐的情况下,观察到的抑制作用不明显,而碳酸氢盐、磷酸盐和硅砂可以在不同程度上抑制 SNM 的矿化。在 SNM 矿化过程中释放出乙酸盐、铵盐和硫酸盐。T300 表现出良好的光化学稳定性,可重复使用 5 次,SNM 去除效率下降不到 10%。根据 Microtox 测定,随着光催化时间的延长,SNM 溶液的急性毒性可以降低。