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易于合成共价修饰有 ZnO 纳米棒的碳纳米管,用于增强染料的光降解。

Facile synthesis of carbon nanotubes covalently modified with ZnO nanorods for enhanced photodecomposition of dyes.

机构信息

Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province, School of Advanced Materials and Energy, Institute of Surface Micro and Nanomaterials, Xuchang University, Xuchang, Henan 461000, China; Henan Joint International Research Laboratory of Nanomaterials for Energy and Catalysis, Xuchang University, Xuchang, Henan 461000, China.

Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province, School of Advanced Materials and Energy, Institute of Surface Micro and Nanomaterials, Xuchang University, Xuchang, Henan 461000, China; Henan Joint International Research Laboratory of Nanomaterials for Energy and Catalysis, Xuchang University, Xuchang, Henan 461000, China.

出版信息

J Colloid Interface Sci. 2019 Mar 1;537:652-660. doi: 10.1016/j.jcis.2018.11.042. Epub 2018 Nov 13.

Abstract

Utilizing a one-pot solvothermal procedure novel one-dimensional zinc oxide-carbon nanotube nanohybrids (ZnCT) were synthesized in alcohol-alkali solution, free of catalytic assistance. The ZnCT hybrids were prepared through covalent modification of zinc oxide nanorods (ZnO NRs) with functionalized carbon nanotubes (f-CNTs). The morphology and microstructure of as-prepared ZnCT hybrids were characterized by scanning electron microscopy (SEM), powder X-ray diffraction, Raman, X-ray photoelectron and UV-vis absorption spectroscopies. SEM images of the ZnCT hybrids indicated that the ZnO NRs grew longer along the vertical radial (0 0 0 1) surface and aggregated to a lesser extent than the analogous ZnO NRs. Photodegradation analysis showed that the off-white ZnCT hybrid with ascendant UV-visible light absorption had displayed superior photocatalytic activity towards Rhodamine B (RhB) dyes than either pure ZnO, ZnO NRs or ZnCT hybrid, among which the photocatalytic activity of ZnO NRs was better than that of ZnO NRs. Raman and X-ray photoelectron spectroscopy analyses confirmed a strong interaction between f-CNTs and ZnO NRs in ZnCT hybrid, in which Zn ions were chemically bonded to negatively charged oxygen-containing groups at the graphene-like surface of f-CNTs. The enhanced separation lifetime of the photogenerated electron-hole observed by surface photovoltage and photocurrent measurements of the ZnCT hybrid was attributed to the efficient covalent linking of ZnOC and close contact configuration between the f-CNTs and ZnO NRs. Further controlled photodegradation and electron spin resonance (ESR) analyses revealed that the photodegradation of RhB dyes resulted from photogenerated holes, and radical species, such as O, OH, which were formed in-situ. Details of the photocatalytic mechanism were also explored herein.

摘要

利用一锅溶剂热法,在无催化辅助的醇-碱溶液中合成了新型一维氧化锌-碳纳米管纳米杂化材料(ZnCT)。ZnCT 杂化材料是通过氧化锌纳米棒(ZnO NRs)与功能化碳纳米管(f-CNTs)的共价修饰制备的。采用扫描电子显微镜(SEM)、粉末 X 射线衍射、拉曼、X 射线光电子能谱和紫外-可见吸收光谱对所制备的 ZnCT 杂化材料的形貌和微观结构进行了表征。SEM 图像表明,ZnO NRs 沿着垂直的径向(0001)表面生长得更长,并且比类似的 ZnO NRs聚集程度更小。光降解分析表明,具有上升的紫外-可见光吸收的灰白色 ZnCT 杂化材料对罗丹明 B(RhB)染料表现出比纯 ZnO、ZnO NRs 或 ZnCT 杂化材料更高的光催化活性,其中 ZnO NRs 的光催化活性优于 ZnO NRs。拉曼和 X 射线光电子能谱分析证实了 f-CNTs 和 ZnO NRs 在 ZnCT 杂化材料中的强相互作用,其中 Zn 离子与 f-CNTs 类石墨烯表面带负电荷的含氧基团发生化学结合。表面光电压和光电流测量观察到光生电子-空穴的分离寿命增强,这归因于 ZnOC 的有效共价连接以及 f-CNTs 和 ZnO NRs 之间的紧密接触结构。进一步的控制光降解和电子顺磁共振(ESR)分析表明,RhB 染料的光降解是由光生空穴和原位形成的自由基物种,如 O、OH 等引起的。本文还探讨了光催化机制的细节。

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