氮掺杂氧化钛的简易制备及可见光催化活性的研究
A simple method to prepare nitrogen-doped titania oxides with high photocatalytic activity under visible light
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摘要: 为开发对可见光响应的催化剂,以尿素为氮掺杂剂,采用简易溶胶-凝胶法制备氮掺杂氧化钛,并以2,4-DCP的降解检验其光催化活性。XRD、BET、XPS和UV-Vis漫反射光谱分析表明,随着氮/钛原子比(N/Ti)的增大,各催化剂晶粒尺寸减小,比表面积增大,锐钛矿相向金红石相的转变得到抑制,除0#样品出现金红石相外,其他催化剂均只出现锐钛矿相;掺入催化剂的N位于晶格O位点和晶格间隙,替代N和间隙N掺杂使催化剂的光吸收发生明显的红移。荧光光谱分析表明,当N/Ti在0~6范围内增加时,反应体系中·OH自由基的产生速率增加,当N/Ti增大至8时,速率则下降。相似的规律也表现在氮掺杂量对光催化活性的影响。适量氮掺杂能增强氧化钛的可见光催化活性,该改性催化剂可用于有机污染物的太阳光激催化降解。Abstract: In order to develop catalyst sensitive to visible light, nitrogen-doped titania oxides were prepared by a simple sol-gel method, with the elemental nitrogen derived from urea. Photocatalytic activity of the catalysts was tested through the degradation of aqueous 2,4dichlorophenol. XRD, BET, XPS and UV-Vis diffuse reflectance spectroscopy analysis showed that the crystallite size of the catalysts decreased and the specific surface area of ones increased with the increase of atomic ratio of nitrogen to titania(N/Ti). The transformation was restrained of anatase to rutile. Except that 0# sample consisted of anatase and rutile, other catalysts were only anatase. Nitrogen was doped into tiatnia crystal lattice, substituting lattice oxygen and siting lattice interstice. Both substitutional and interstitial nitrogendoped titania catalysts exhibited notable redshift of light-adsorbtion edge. Fluorescence spectroscopy analysis showed that the rate of ·OH forming in reactiong syetem was upgoing when N/Ti increased from 0 to 6, but was downgrade when N/Ti was upto 8. The similar rule did the effect of the N/Ti on photocatalytic activity follow. In conclusion, a certain amount of nitrogen doping can enhance the visiablelight photocatalytic activity of titania oxides. The modified catalysts can be used for organic pollutant photoderadation under sunlight.
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