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使用负载在碳上的双金属催化剂直接、高效还原全氟辛酸。

Direct and efficient reduction of perfluorooctanoic acid using bimetallic catalyst supported on carbon.

机构信息

State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resource and Environmental Engineering, East China University of Science and Technology, Shanghai, China.

Key Laboratory for Advanced Materials and Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China.

出版信息

J Hazard Mater. 2021 Jun 15;412:125224. doi: 10.1016/j.jhazmat.2021.125224. Epub 2021 Jan 24.

Abstract

A variety of metal elements have exhibited strong reductive and dehalogenative capabilities for the removal of persistent organic pollutants, owing to electron transfer or electron-hole activation through various methods. Herein, a bimetallic C-AlO structure (AlC) was successfully synthesized to simultaneously function as sorbent and catalyst in the reduction of perfluoroalkyl carboxylic acids (PFOA) polluted wastewater. Using a reaction period of 3 h, 98% of PFOA was removed by AlC through a mechanochemical stirring method and 70.43% of fluorine ions was released from PFOA anchored onto the surface of AlC. Both thermocatalysis and photocatalysis technologies were incorporated and compared when utilized in tandem with AlC to mitigate the PFOA. In addition, peroxymonosulfate (PMS) and sodium sulfite (NaSO) were also integrated into experiments, separately, as a strong oxidant and reductant to improve the degradation effect of PFOA. However, the degradation efficiency of both were lower than that of AlC, even when assisted by elevated temperatures and ultraviolet irradiation. The feasibility of employing AlC for PFOA degradation was further investigated at various temperature and pH conditions. The data obtained from HPLC-MS/MS, TOC, and IC with multiple characterizations of AlC/PFOA, proposed the predominant degradation pathways comprising adsorption, defluorination-hydroxylation, and decarboxylation. This study provides a valuable remediation method without utilizing chemical agents and special activation for PFOA by AlC, which can be suitable for large-scale sewage treatment applications.

摘要

多种金属元素通过各种方法(如电子转移或电子空穴激活)表现出很强的还原和脱卤能力,可用于去除持久性有机污染物。在此,成功合成了一种双金属 C-AlO 结构(AlC),它可同时作为还原剂和催化剂用于还原全氟烷基羧酸(PFOA)污染废水。在 3 小时的反应周期内,AlC 通过机械化学搅拌法去除了 98%的 PFOA,并且 70.43%的氟离子从 PFOA 上释放出来并锚定在 AlC 的表面。当与 AlC 串联使用时,同时采用热催化和光催化技术,并对其进行了比较。此外,还分别将过一硫酸盐(PMS)和亚硫酸钠(NaSO)整合到实验中,作为强氧化剂和还原剂来提高 PFOA 的降解效果。然而,它们的降解效率均低于 AlC,即使在高温和紫外线照射的辅助下也是如此。在不同的温度和 pH 条件下,进一步研究了 AlC 对 PFOA 降解的可行性。通过 HPLC-MS/MS、TOC 和 IC 对 AlC/PFOA 进行了多种表征,获得的数据提出了主要的降解途径,包括吸附、脱氟-羟化和脱羧。这项研究提供了一种有价值的修复方法,无需使用化学试剂和特殊的 AlC 激活,可适用于大规模的污水处理应用。

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