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用于合成ZnO分级结构的简便、高产率超声介导方法:形成机理、光学和光催化性能

Facile, high yield ultrasound mediated protocol for ZnO hierarchical structures synthesis: Formation mechanism, optical and photocatalytic properties.

作者信息

Carp Oana, Tirsoaga Alina, Ene Ramona, Ianculescu Adelina, Negrea Raluca F, Chesler Paul, Ionita Gabriela, Birjega Ruxandra

机构信息

"Ilie Murgulescu" Institute of Physical Chemistry, Romanian Academy, Splaiul Independentei 202, 060021 Bucharest, Romania.

University of Bucharest, Physical Chemistry Department, Bd. Elisabeta 4-12, 030018 Bucharest, Romania.

出版信息

Ultrason Sonochem. 2017 May;36:326-335. doi: 10.1016/j.ultsonch.2016.12.005. Epub 2016 Dec 10.

Abstract

Hierarchical flowers-like zinc oxide structures have been successfully obtained by a simple and fast ultrasound-assisted method performed in a ordinary ultrasonic bath using an ammonia solution and zinc acetate, in the absence of any surfactant or template. The composition, structure, crystallinity, morphology and optical properties of the materials obtained at different ultrasound irradiation times were characterized by infrared, UV-Vis and photoluminescence spectroscopy, X-ray diffraction, scanning and transmission electron microscopy investigations. It was proved that the ultrasound irradiation time manipulates both the defect content (implicit the photoluminescent properties) and morphology of the ZnO materials: shorter irradiation times leads to the synthesis of high-defected ZnO structures of flower morphology with triangular-shaped petals, while higher irradiation times favours the formation of low-defected ZnO structures with tipped rod-like petals. A plausible growth mechanism of the architectures that implies aggregation via oriented attachment followed by an Ostwald ripening is advanced based on these results. The ZnO flower-like structures present high photocatalytic activities, a total phenol mineralization being registered in the case of visible light experiments. Electron-spin resonance measurements demonstrate the generation of reactive oxygen species, namely hydroxyl radicals but also C centred radicals adducts derived most probable from the residual acetate adsorbed on ZnO surface.

摘要

通过一种简单快速的超声辅助方法,在普通超声浴中使用氨溶液和醋酸锌,在没有任何表面活性剂或模板的情况下,成功获得了分级花状氧化锌结构。通过红外、紫外可见和光致发光光谱、X射线衍射、扫描和透射电子显微镜研究,对在不同超声辐照时间下获得的材料的组成、结构、结晶度、形态和光学性质进行了表征。结果表明,超声辐照时间既影响氧化锌材料的缺陷含量(隐含光致发光性质)又影响其形态:较短的辐照时间导致合成具有三角形花瓣的花状高缺陷氧化锌结构,而较长的辐照时间有利于形成具有尖端棒状花瓣的低缺陷氧化锌结构。基于这些结果,提出了一种合理的结构生长机制,该机制意味着通过定向附着聚集,随后进行奥斯特瓦尔德熟化。氧化锌花状结构具有高光催化活性,在可见光实验中实现了总酚的矿化。电子自旋共振测量表明产生了活性氧物种,即羟基自由基以及最有可能源自吸附在氧化锌表面的残留醋酸盐的碳中心自由基加合物。

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