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作 者:于福海[1,2] 王军虎[1] 赵昆峰[1,2] 尹杰 金长子[1] 刘忻
机构地区:[1]中国科学院大连化学物理研究所,辽宁大连116023 [2]中国科学院大学,北京100049
出 处:《催化学报》2013年第6期1216-1223,共8页
基 金:supported by the Chinese Academy of Sciences for "100 Talents"Project;the National Natural Science Foundation of China (11079036);the Natural Science Foundation of Liaoning Province (20092173)~~
摘 要:采用新的化学溶液法,通过不同体积的钛酸四异丙酯的2-乙二醇单乙醚溶液与一定浓度的H2O2水溶液直接反应并对生成的钛过氧化配合物进行焙烧,制备了一系列TiO2光催化剂.表征发现,所得TiO2样品为金红石和锐钛矿的纳米复合晶体,改变2-乙二醇单乙醚的体积可实现金红石相比例在0~96%广范围的调变.与商业二氧化钛P-25相比,所得的TiO2紫外-可见光吸收谱出现明显红移,间隙能降低,在可见光照射下,该样品对亚甲基蓝有良好的降解活性.当2-乙二醇单乙醚的添加量为5ml时,所得样品体相中金红石相比例接近50%,其光催化活性和吸附性能最好,可分别是P-25的3倍和5倍.拉曼光谱结合X射线衍射等表征结果表明,该样品的表面仅含少量的金红石相.TiO2纳米复合晶表面晶相的组成和分布对其光催化降解亚甲基蓝的活性及其吸附能力有直接的影响.另外,TiO2纳米复合晶的缺陷浓度也是增强其光吸收能力,提高其可见光光催化活性的原因之一.A series of novel TiO2 nanocomposite crystals with superior visible‐light‐driven photocatalytic activity were successfully prepared using a soft chemical solution process involving direct reaction of aqueous H2O2 with a 2‐ethoxyethanol solution of tetraisopropyl titanate before calcination of the resulting peroxo‐titanium complexes at 500 °C for 4 h. The synthesized TiO2 samples are composed of anatase and rutile phases, and the ratio of rutile could be continuously tuned from 0 to 96% by altering the 2‐ethoxyethanol volume. There are clear red‐shifts in the UV‐Vis absorption spectra and apparent band gap narrowing for the synthesized TiO2 in comparison with Evonik P‐25. The synthesized TiO2 samples are found to be much more efficient for methylene blue degradation under visible‐light irradiation. The optimized sample (2‐ethoxyethanol: 5 ml; rutile in bulk: 46%) exhibits 5‐fold higher adsorption capacity and 3‐fold higher photocatalytic activity than those of Evonik P‐25 (λ ≥ 400 nm). Characterizations including X‐ray diffraction and Raman spectroscopy reveal that the surface of the optimized TiO2 sample only contains a small quantity of rutile. It is concluded that the surface phase composition and distribution of the TiO2 nanocomposite crystals are essential to their greatly enhanced photocatalytic activities and strong adsorption capacities. In addition, the concentration of defects existing in the synthesized TiO2 is also regarded to account for these enhanced properties.
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