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两种新型 MOFs@COFs 杂化基光催化平台结合硫酸根自由基参与的高级氧化过程用于增强双酚 A 的降解。

Two novel MOFs@COFs hybrid-based photocatalytic platforms coupling with sulfate radical-involved advanced oxidation processes for enhanced degradation of bisphenol A.

机构信息

Tianjin Key Laboratory of Food Science and Health, School of Medicine, Nankai University, Tianjin, 300071, China; College of Environmental Science and Engineering, Nankai University, Tianjin, 300071, China.

Tianjin Key Laboratory of Food Science and Health, School of Medicine, Nankai University, Tianjin, 300071, China.

出版信息

Chemosphere. 2020 Mar;243:125378. doi: 10.1016/j.chemosphere.2019.125378. Epub 2019 Nov 16.

Abstract

Nowadays, the visible-light-driven photocatalysis via advanced photocatalyst for PS activation have promising applications in wastewater treatment. Herein, for the first time, two novel MOFs@COFs hybrid materials (denoted as MIL-101-NH@TpMA and UiO-66-NH@TpMA) with nitrogen-rich building blocks were fabricated via a feasible step-by-step assembly method, and then employed as efficient photocatalytic platform coupling with sulfate radical-based advanced oxidation processes for the degradation of BPA under visible light irradiation. Detailed analyses revealed that the hybridization of MOFs and COFs could greatly boost visible light absorption, while the heterojunction formed at the interface could effectively facilitate the separation and transfer of photogenerated electron-hole pairs. More importantly, the developed solar/MOFs@COFs/PS system exhibited the excellent degradation ability toward BPA, and an incredible degradation efficiency of 99% was eventually achieved. Possible mechanism for photocatalytic degradation of BPA was also proposed. Furthermore, the prepared composites with great reusability and stability possessed a broad potential for highly effective degradation of various organic contaminants. In short, this work not only demonstrated the combination of MOFs and COFs with CN active unit was a feasible strategy for improving photocatalytic activities in the degradation of organic contaminants, but also provided some novel inspirations for constructing high-efficient photocatalysts with heterostructure.

摘要

如今,利用先进的光催化剂通过可见光驱动的光催化来激活 PS 在废水处理中具有广阔的应用前景。在此,首次通过一种可行的分步组装方法制备了两种具有富氮结构单元的新型 MOFs@COFs 杂化材料(分别表示为 MIL-101-NH@TpMA 和 UiO-66-NH@TpMA),然后将其用作与硫酸根自由基基高级氧化过程相结合的高效光催化平台,用于在可见光照射下降解 BPA。详细分析表明,MOFs 和 COFs 的杂化可以大大提高可见光吸收,而在界面形成的异质结可以有效地促进光生电子-空穴对的分离和转移。更重要的是,所开发的太阳能/MOFs@COFs/PS 系统对 BPA 表现出优异的降解能力,最终实现了令人难以置信的 99%的降解效率。还提出了光催化降解 BPA 的可能机制。此外,所制备的复合材料具有良好的可重复使用性和稳定性,对于有效降解各种有机污染物具有广阔的应用潜力。总之,这项工作不仅证明了将 MOFs 和 COFs 与 CN 活性单元结合是提高有机污染物降解中光催化活性的一种可行策略,而且为构建具有异质结构的高效光催化剂提供了一些新的启示。

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