Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO4 at neutral pH

Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO4 at neutral pH
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BiVO4 修饰的水铁矿在中性 pH 值下增强光芬顿活性的机制

DOI:
10.1016/j.apcatb.2017.04.064
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发表时间:
2017-09
影响因子:
22.1
通讯作者:
He Hongping
He Hongping
中科院分区:
化学1区
文献类型:
--
作者:
Xu Tianyuan;Zhu Runliang;Zhu Gangqiang;Zhu Jianxi;Liang Xiaoliang;Zhu Yanping;He Hongping

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由于Fe2+的再生速率相对较低,在接近中性的pH下,非均相光fenton催化剂通常表现出非常弱的光fenton活性。本研究的目的是开发一种新型的非均相光fenton催化剂,这种催化剂可以加速Fe2+的再生,从而在接近中性的ph下具有优异的光fenton活性。在本研究中,BiVO4修饰了水合铁(Fh),合成了BiVO4/Fh复合材料,我们期望BiVO4的光生电子可以加速Fh上Fe2+的再生。对h2o2消耗机理的研究表明,bivo4的引入促进了h2o2分解为活性氧(ROS)。此外,根据EPR光谱和荧光探针工具显示的ROS形成结果,bivo4的存在阻止了o2自由基dot -的产生,加速了自由基dotOH的形成。XPS表征和1,10-菲罗啉分光光度法定量测定结果表明,BiVO4/Fh表面的Fe2+浓度高于Fh表面。这些结果表明,bivo4的引入可以通过将光电子从bivo4转移到Fh表面的Fe3+来加速Fe3+还原为Fe2+。同时,BiVO4/Fh对酸性红18的脱色效率高于Fh和纯BiVO4,验证了BiVO4的引入即使在接近中性的ph下也能显著提高Fh的光- fenton催化活性。本研究对理解半导体修饰的非均相光fenton催化剂的光fenton机理具有重要意义,并证实了半导体的引入可以提高非均相光fenton催化剂在酸性和中性pH下的光fenton催化活性。
Heterogeneous photo-Fenton catalysts generally show very weak photo-Fenton activity at near-neutral pH because of the relatively low rate of Fe2+regeneration. The aim of this work is to develop novel heterogeneous photo-Fenton catalysts, which can accelerate the regeneration of Fe2+and thus have superior photo-Fenton activity at near-neutral pH. In this study, ferrihydrite (Fh) was modified with BiVO4to synthesize BiVO4/Fh composites, and we expected that the photogenerated electrons from BiVO4would accelerate the regeneration of Fe2+on Fh. Mechanistic investigation of H2O2consumption showed that the introduction of BiVO4promoted the decomposition of H2O2into reactive oxygen species (ROS). In addition, the presence of BiVO4deterred O2radical dot−production and accelerated the formation of radical dotOH, according to the results of ROS formation, as shown with EPR spectroscopy and fluorescent probes tools. Furthermore, the Fe2+concentration on the surface of BiVO4/Fh was higher than that on Fh based on the results of XPS characterization and quantitative measurement with a 1,10-phenanthroline spectrophotometric method. These results demonstrated that the introduction of BiVO4can accelerate the reduction of Fe3+to Fe2+by transferring photogenerated electrons from BiVO4to Fe3+on the surface of Fh. Meanwhile, a higher decolorization efficiency of acid red 18 by BiVO4/Fh than by Fh and pure BiVO4verified that the introduction of BiVO4can significantly enhance the photo-Fenton catalytic activity of Fh even at near-neutral pH. Overall, our work has important implications for understanding the photo-Fenton mechanisms on semiconductor modified heterogeneous photo-Fenton catalysts and confirms that the introduction of a semiconductor can enhance the photo-Fenton catalytic activity of heterogeneous photo-Fenton catalysts in acidic and neutral pH.
BiVO4/Fe/Mt 复合材料用于可见光驱动的酸性红 18 降解
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