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