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一种用于水处理的基于两性离子水凝胶的非均相芬顿催化剂。

A Zwitterionic Hydrogel-Based Heterogeneous Fenton Catalyst for Water Treatment.

作者信息

Gokhale Devashish, Chen Ian, Wu Wan-Ni, Monne Gagnaire Arthur, Doyle Patrick S

机构信息

Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA.

Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA.

出版信息

Small. 2024 Sep;20(38):e2402525. doi: 10.1002/smll.202402525. Epub 2024 May 27.

Abstract

Persistent organic pollutants (POPs), including xenoestrogens and polyfluoroalkyl substances (PFAS), demand urgent global intervention. Fenton oxidation, catalyzed by iron ions, offers a cost-effective means to degrade POPs. However, numerous challenges like acid dependency, catalyst loss, and toxic waste generation hinder practical application. Efforts to create long-lasting heterogeneous Fenton catalysts, capable of simultaneously eliminating acid requirements, sustaining rapid kinetics, and retaining iron efficiently, have been unsuccessful. This study introduces an innovative heterogeneous zwitterionic hydrogel-based Fenton catalyst, surmounting these challenges in a cost-effective and scalable manner. The hydrogel, hosting individually complexed iron ions in a porous scaffold, exhibits substantial effective surface area and kinetics akin to homogeneous Fenton reactions. Complexed ions within the hydrogel can initiate Fenton degradation at neutral pH, eliminating acid additions. Simultaneously, the zwitterionic hydrogel scaffold, chosen for its resistance to Fenton oxidation, forms strong bonds with iron ions, enabling prolonged reuse. Diverging from existing designs, the catalyst proves compatible with UV-Fenton processes and achieves rapid self-regeneration during operation, offering a promising solution for the efficient and scalable degradation of POPs. The study underscores the efficacy of the approach by demonstrating the swift degradation of three significant contaminants-xenoestrogens, pesticides, and PFAS-across multiple cycles at trace concentrations.

摘要

持久性有机污染物(POPs),包括外源性雌激素和多氟烷基物质(PFAS),需要全球紧急干预。铁离子催化的芬顿氧化法提供了一种经济有效的降解POPs的方法。然而,诸如依赖酸性条件、催化剂损失和产生有毒废物等诸多挑战阻碍了其实际应用。制造能够同时消除对酸性条件的需求、维持快速反应动力学并有效保留铁的长效非均相芬顿催化剂的努力一直没有成功。本研究引入了一种创新的基于两性离子水凝胶的非均相芬顿催化剂,以经济有效且可扩展的方式克服了这些挑战。该水凝胶在多孔支架中容纳单独络合的铁离子,具有类似于均相芬顿反应的有效表面积和动力学。水凝胶中的络合离子可在中性pH值下引发芬顿降解,无需添加酸。同时,因其对芬顿氧化具有抗性而被选用的两性离子水凝胶支架与铁离子形成强键,从而能够长期重复使用。与现有设计不同,该催化剂被证明与紫外光芬顿工艺兼容,并在运行过程中实现快速自我再生,为高效且可扩展地降解POPs提供了一个有前景的解决方案。该研究通过展示在多个循环中对三种重要污染物——外源性雌激素、农药和PFAS——在痕量浓度下的快速降解,强调了该方法的有效性。

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