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用于高效非均相光芬顿氧化的高度分散的二氧化钛负载氧化铁催化剂:影响因素、协同效应及机理洞察

Highly dispersed titania-supported iron oxide catalysts for efficient heterogeneous photo-Fenton oxidation: Influencing factors, synergistic effects and mechanism insight.

作者信息

Zhang Yadong, Wu Lei, Wang Ying, Zhang Yi, Wang Hao, Wang Xiaoning, Chen Xiao Dong, Wu Zhangxiong

机构信息

Particle Engineering Laboratory, School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou City, Jiangsu 215123, PR China.

Particle Engineering Laboratory, School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou City, Jiangsu 215123, PR China.

出版信息

J Colloid Interface Sci. 2021 Apr;587:467-478. doi: 10.1016/j.jcis.2020.12.008. Epub 2020 Dec 7.

Abstract

Titania (TiO) supported iron oxides (Fe-TiO) are ideal catalysts to be applied in heterogeneous photo-Fenton oxidation (HPFO) for wastewater treatment because of the capabilities of TiO in photocatalysis and iron oxides in interfacial HO activation. It is important to understand the influences of the structural parameters of Fe-TiO catalysts and the complicated interplay between TiO and iron oxides on the performance of HPFO. In this paper, a series of Fe-TiO catalysts are obtained through a facile solid-phase synthesis method. The iron loading content and the calcination temperature are systematically adjusted to tune the crystal phase, size, anatase/rutile ratio and density of oxygen vacancy (O) site of TiO, the dispersing state of iron species, and the interfacial structure of the Fe-TiO catalysts. Then, the performance of these catalysts in HPFO for degrading methylene blue (MB) are comparatively studied. Correlations between the performance and various structural properties of the catalysts are clarified. The interplay between TiO and iron oxides in the HPFO process is elucidated. The insight reaction mechanism is also discussed. Under optimized conditions (an iron loading of 1 wt% and a temperature of 600 °C), Fe-TiO catalysts with iron lattice doping, well-dispersed ultrasmall α-FeO nanoparticles, appropriate anatase/rutile ratios and abundant O sites can be obtained. The anatase-rutile-FeO heterojunction, ultrasmall α-FeO nanoparticles and O sites in the optimized catalysts work synergistically to improve the charge migration and interfacial activation of HO, leading to superior HPFO performance for MB degradation and mineralization.

摘要

二氧化钛(TiO)负载的铁氧化物(Fe-TiO)是应用于非均相光芬顿氧化(HPFO)处理废水的理想催化剂,因为TiO具有光催化能力,而铁氧化物具有界面羟基(HO)活化能力。了解Fe-TiO催化剂的结构参数以及TiO与铁氧化物之间复杂的相互作用对HPFO性能的影响非常重要。本文通过一种简便的固相合成方法制备了一系列Fe-TiO催化剂。系统地调节铁负载量和煅烧温度,以调控TiO的晶相、尺寸、锐钛矿/金红石比例和氧空位(O)位点密度、铁物种的分散状态以及Fe-TiO催化剂的界面结构。然后,对这些催化剂在HPFO降解亚甲基蓝(MB)中的性能进行了比较研究。阐明了催化剂性能与各种结构性质之间的相关性。阐明了HPFO过程中TiO与铁氧化物之间的相互作用。还讨论了深入的反应机理。在优化条件下(铁负载量为1 wt%,温度为600 °C),可以获得具有铁晶格掺杂、分散良好的超小α-FeO纳米颗粒、合适的锐钛矿/金红石比例和丰富O位点的Fe-TiO催化剂。优化后的催化剂中的锐钛矿-金红石-FeO异质结、超小α-FeO纳米颗粒和O位点协同作用,改善了HO的电荷迁移和界面活化,从而在MB降解和矿化方面表现出优异的HPFO性能。

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