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金属有机骨架负载氮化碳:可见光增强的多溴联苯醚降解平台。

Metal-organic frameworks incorporated with CN: A visible light enhanced platform for degradation of polybromodiphenyl ethers.

机构信息

School of Chemistry and Chemical Engineering, Shaoxing University, Shaoxing 312000, China.

School of Chemistry and Chemical Engineering, Shaoxing University, Shaoxing 312000, China; School of Chemistry and Chemical Engineering, Institute of New Energy, Shaoxing University, Shaoxing 312000, China.

出版信息

J Environ Sci (China). 2023 Dec;134:44-54. doi: 10.1016/j.jes.2022.04.041. Epub 2022 May 6.

Abstract

A series of nano-photocatalysts metal-organic frameworks (MOFs)/graphitic carbon nitride (CN) (named MOFCN-x) with high activity have been synthesized by in-situ growth method. Under visible light irradiation, MOFCN-x hybrids show enhanced photocatalytic activity for the debromination of polybromodiphenyl ethers (PBDEs) compared with CN. Among all the hybrids, MOFCN-2 shows the highest reaction rate, which is 3.3 times as high as that in CN. MOFCN-x photocatalysts own stable visible light activity after recycled experiment. It indicates that a moderate amount of MOFs in MOFCN-x can largely enhance the photocatalytic ability by improved visible light absorption, larger specific surface area and better photo-generated charge carriers separation and transfer capabilities. More interestingly, the debromination pathway of PBDEs by MOFCN-x shows obvious selectivity compared with pure CN that bromines at meta-positions are much more susceptible than those at the para- and ortho-positions. The possible photoreductive mechanism has been proposed. This study shows that nanocomposite MOFCN can be an excellent candidate for dealing with halogen pollutants by solar-driven.

摘要

通过原位生长法合成了一系列具有高活性的纳米光催化剂金属-有机骨架(MOFs)/石墨相氮化碳(CN)(命名为 MOFCN-x)。在可见光照射下,MOFCN-x 杂化物对多溴二苯醚(PBDEs)的脱溴反应表现出比 CN 更高的光催化活性。在所有杂化物中,MOFCN-2 表现出最高的反应速率,是 CN 的 3.3 倍。经过回收实验,MOFCN-x 光催化剂具有稳定的可见光活性。这表明适量的 MOFs 在 MOFCN-x 中可以通过提高可见光吸收、更大的比表面积以及更好的光生载流子分离和转移能力,极大地提高光催化能力。更有趣的是,与纯 CN 相比,MOFCN-x 对 PBDEs 的脱溴途径表现出明显的选择性,间位的溴比对位和邻位的溴更容易脱除。提出了可能的光还原机理。该研究表明,纳米复合 MOFCN 可以成为一种通过太阳能驱动处理卤代污染物的优秀候选材料。

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