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Laser synthesized TiO2-based nanoparticles and their efficiency in the photocatalytic degradation of linear carboxylic acids

机译:激光合成TiO2基纳米粒子及其在线性羧酸光催化降解中的效率

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摘要

Titanium dioxide nanoparticles were synthesized by laser pyrolysis, their surface and electronic properties were modified by gold and/or nitrogen. These materials were characterized by different techniques like X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR). Time resolved conductivity (TRMC) was used to study the charge separation of electron/hole pairs. Altogether (XPS, EPR, TRMC), the physicochemical characterizations are well correlated with chemical photoactivity of the different samples. Their photocatalytic activity was evaluated for the degradation of linear carboxylic acids (C2-C3) under UV and visible illumination. The decomposition rate of acids was measured, it shows that the modification with gold increases the photoactivity while the presence of nitrogen slows down the process. Such observations are in good agreement with evolution of TRMC signals. A degradation pathway has been determined by identification of intermediate products by chromatography and EPR, results show different intermediate species. In particular EPR confirms the presence of NO2− paramagnetic centers and shows two novel N centered paramagnetic centers. A decrease of the degradation rate is observed with increase of carboxylic acid chain length.
机译:通过激光热解法合成二氧化钛纳米粒子,其表面和电子性能被金和/或氮改性。这些材料通过X射线衍射(XRD),X射线光电子能谱(XPS)和电子顺磁共振(EPR)等不同技术进行了表征。时间分辨电导率(TRMC)用于研究电子/空穴对的电荷分离。总的来说(XPS,EPR,TRMC),其理化特性与不同样品的化学光活性相关。在紫外线和可见光照射下,评估了它们的光催化活性以降解线性羧酸(C2-C3)。测量了酸的分解速率,结果表明金的修饰增加了光活性,而氮的存在则减慢了该过程。这样的观察与TRMC信号的演化非常吻合。通过色谱和EPR鉴定中间产物已确定了降解途径,结果显示了不同的中间物种。特别是,EPR证实了NO 2-顺磁中心的存在,并显示了两个新颖的以N为中心的顺磁中心。随着羧酸链长度的增加,观察到降解速率的降低。

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