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三氧化钨光阳极的可控晶面用于改善原位四环素降解中按需生产过氧化氢的性能。

Controlled crystal facet of tungsten trioxide photoanode to improve on-demand hydrogen peroxide production for in-situ tetracycline degradation.

作者信息

Xu Yuntao, Lai Wei, Cui Xiaoqi, Zheng Dandan, Wang Sibo, Fang Yuanxing

机构信息

State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, PR China.

College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, PR China.

出版信息

J Colloid Interface Sci. 2024 Feb;655:822-829. doi: 10.1016/j.jcis.2023.11.071. Epub 2023 Nov 13.

Abstract

Advanced oxidation processes utilizing hydrogen peroxide (HO) are widely employed for the treatment of organic pollutions. However, the conventional anthraquinone method for HO synthesis is unsuitable for this application owing to its hazardous and costly nature. Alternative approaches involve a photoelectrochemical method. Herein, tungsten trioxide (WO) photoanode has been used for the conversion of HO into HO through oxidation reaction from a PEC system, simultaneously utilizing in-situ generated hydroxyl (OH) radicals for tetracycline degradation. By manipulating the ratio of crystal facets between (020) and (200) of the WO photoanode, a significant improvement in HO production has been achieved by increasing the proportion of (020) facet. The production rate of WO photoanode enriched with the (020) facet is approximately 1.9 times higher than that enriched with (200) facet. This enhanced HO production performance can be attributed to the improved formation of OH radicals and the accelerated desorption of HO on the (020) facet. Simultaneously, the in-situ generated OH radicals are applied for tetracycline degradation. Under illumination of sunlight stimulator for 180 min, the optimal photoanode achieves a degradation rate of 86.7% for tetracycline. Furthermore, the resulting chemicals have been analyzed, revealing that CHO and CHO were formed as the primary products. Notably, these products exhibit significantly lower toxicity compared to tetracycline. This study presents a promising approach for the rational design of WO based photoanodes for oxidation reaction, including not only HO production but also the efficient degradation of organic pollutants.

摘要

利用过氧化氢(HO)的高级氧化工艺被广泛用于处理有机污染物。然而,传统的用于合成HO的蒽醌法由于其危险性和高成本性质而不适用于此应用。替代方法涉及光电化学方法。在此,三氧化钨(WO)光阳极已被用于通过PEC系统中的氧化反应将HO转化为HO,同时利用原位生成的羟基(OH)自由基进行四环素降解。通过控制WO光阳极(020)和(200)晶面之间的比例,通过增加(020)晶面的比例,HO的产量有了显著提高。富含(020)晶面的WO光阳极的产率比富含(200)晶面的光阳极高出约1.9倍。这种增强的HO生产性能可归因于OH自由基形成的改善以及HO在(020)晶面上解吸的加速。同时,原位生成的OH自由基用于四环素降解。在阳光模拟器照射180分钟的情况下,最佳光阳极对四环素的降解率达到86.7%。此外,对生成的化学物质进行了分析,结果表明主要产物为CHO和CHO。值得注意的是,这些产物的毒性明显低于四环素。本研究提出了一种有前景的方法,用于合理设计基于WO的用于氧化反应的光阳极,不仅包括HO的生产,还包括有机污染物的有效降解。

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