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通过调整暴露的 FeWO 纳米片晶面在可见光照射下增强活性氧的生成,用于去除有机污染物和还原 Cr(VI)。

Enhanced Generation of Reactive Oxygen Species under Visible Light Irradiation by Adjusting the Exposed Facet of FeWO Nanosheets To Activate Oxalic Acid for Organic Pollutant Removal and Cr(VI) Reduction.

机构信息

Hubei Key Laboratory of Mineral Resources Processing and Environment, State Key Laboratory of Silicate Materials for Architectures , Wuhan University of Technology , 122 Luoshi Road , Wuhan 430070 , China.

出版信息

Environ Sci Technol. 2019 Sep 17;53(18):11023-11030. doi: 10.1021/acs.est.9b00641. Epub 2019 Sep 4.

Abstract

In this work, taking FeWO nanosheets as an example, the activation of oxalic acid (OA) based on facet engineering for the enhanced generation of active radical species was reported, revealing unprecedented surface Fenton activity for pollutant degradation. Density functional theory calculations confirmed the more efficient generation of reactive oxygen species over FeWO nanosheets with the {001} facet exposed (FWO-001) under visible light irradiation compared to the efficiency of FeWO nanosheets with the {010} facet exposed (FWO-010), which could be attributed to a higher density of iron and the efficient activation of OA on the {001} facet. The HO-derived OH tended to diffuse away from the active sites of FWO-001 into solution to favor the continuous activation of OA into the active radicals for pollutant redox reactions, but preferred to remain on FWO-010 to hinder the further activation of OA on the {010} facet. Additionally, the generation of CO endowed FeWO with a strong reduction ability. Compared with FWO-010, FWO-001 exhibited enhanced redox activity for the catalytic degradation of organic pollutants and Cr(VI) in the optimized conditions. These findings can help in understanding the facet dependent surface Fenton chemistry of catalytic redox reactions and in designing efficient catalysts for environmental decontamination.

摘要

在这项工作中,以 FeWO 纳米片为例,通过面工程激活基于草酸盐(OA)的反应活性物种,揭示了用于污染物降解的空前的表面芬顿活性。密度泛函理论计算证实,与暴露于 {010} 面的 FeWO 纳米片(FWO-010)相比,暴露于 {001} 面的 FeWO 纳米片(FWO-001)在可见光照射下更有效地生成活性氧物种,这归因于 {001} 面上更高密度的铁和 OA 的有效激活。HO 衍生的 OH 倾向于从 FWO-001 的活性位点扩散到溶液中,有利于 OA 连续激活为用于污染物氧化还原反应的活性自由基,但倾向于留在 FWO-010 上,以阻碍 OA 在 {010} 面上的进一步激活。此外,CO 的生成赋予了 FeWO 较强的还原能力。与 FWO-010 相比,在优化条件下,FWO-001 对有机污染物和 Cr(VI)的催化降解表现出增强的氧化还原活性。这些发现有助于理解催化氧化还原反应中基于面的表面芬顿化学,并设计用于环境净化的高效催化剂。

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