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Photochemical synthesis of monodispersed ceria nanocrystals in simple cerium nitrate solution without additives

机译:不含添加剂的简单硝酸铈溶液中光化学合成单分散二氧化铈纳米晶体

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摘要

We developed a novel photochemical technique for preparation of ceria (CeO_2) nanocrystals in simple aqueous solution containing only Ce(NO_3)_3, where no additive and no heating are required. Under UV light illumination, photochemical reduction of NO_3- resulted in formation of NO_2~- accompanied by hydroxyl radicals (·OH) as intermediate species. The hydroxyl radicals could oxidize Ce~(3+) to tetravalent state (Ce(OH)_2~(2+)), then CeO_2 nuclei were formed through deprotonation. The aqueous CeO_2 sol was prepared via dialysis of the reacted solution against deionized water to remove the excess electrolyte. Since the photooxidation process homogeneously occurs over the entire solution due to high optical transmittance of the solvent, the particle size distribution becomes relatively narrow and the mean diameter can be easily controlled by adjusting the initial concentration of Ce(NO_3)_3. The prepared CeO_2 nanoparticles were potent against oxidative polymerization of phenolic derivatives (guaiacol) at room temperature. This paper clarifies the photochemical formation mechanism of CeO_2 nanocrystals in the Ce(NO_3)_3 solution, and the advantages of the proposed method are discussed in detail.
机译:我们开发了一种新颖的光化学技术,可在仅包含Ce(NO_3)_3的简单水溶液中制备二氧化铈(CeO_2)纳米晶体,而无需添加添加剂且无需加热。在紫外线照射下,NO_3-的光化学还原导致形成NO_2〜-,并伴随着羟基自由基(·OH)作为中间物种。羟基自由基可以将Ce〜(3+)氧化为四价态(Ce(OH)_2〜(2+)),然后通过去质子化反应形成CeO_2核。通过将反应后的溶液用去离子水透析以除去过量的电解质来制备CeO_2溶胶。由于溶剂的高透光率,光氧化过程在整个溶液中均匀地发生,因此粒径分布变得相对狭窄,并且可以通过调节Ce(NO_3)_3的初始浓度来轻松控制平均直径。所制备的CeO_2纳米粒子在室温下对酚类衍生物(愈创木酚)的氧化聚合具有强效作用。本文阐明了Ce(NO_3)_3溶液中CeO_2纳米晶体的光化学形成机理,并详细讨论了该方法的优点。

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