College of Chemistry, Research Center for Analytical Sciences, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Nankai University, Tianjin 300071, China.
School of Pharmaceutical Sciences, Shandong First Medical University & Shandong Academy of Medical Sciences, Tai'an 271016, China.
J Hazard Mater. 2022 Feb 15;424(Pt B):127485. doi: 10.1016/j.jhazmat.2021.127485. Epub 2021 Oct 9.
Microporous organic networks (MONs) have shown great potential in the removal of environmental contaminants. However, all studies have focused on the design and construction of novel and efficient adsorbents, and the recycling and reuse of adsorbates were disregarded. In this study, we report a feasible approach to synthesize renewable and reusable MONs by using target halogenated contaminants such as tetrabromobisphenol A (TBBPA), 2,3-dichlorophenol (2,3-DCP), and 2,4,6-trichlorophenol (2,4,6-TCP) as starting monomers. TBBPA, 2,3-DCP, and 2,4,6-TCP acted as hazardous contaminants and starting monomers for MONs, leading to the recycling of both adsorbents and adsorbates. The obtained TBBPA-MON, 2,3-DCP-MON, and 2,4,6-TCP-MON not only offered good reusability and large adsorption capacity for their elimination but also provided good adsorption for other phenolic contaminants relying on multiple interactions. Density functional theory calculation indicated the dominant role of π-π and hydrophobic interactions and the secondary role of hydrogen bonding interactions during the adsorption process. The used TBBPA-MON could be reused and the eluted TBBPA could be recycled and renewed for the construction of fresh MONs. This study provided a feasible approach to design and synthesize renewable MONs for environmental contaminants.
微孔有机网络(MONs)在去除环境污染物方面显示出巨大的潜力。然而,所有研究都集中在新型高效吸附剂的设计和构建上,而忽略了吸附质的回收和再利用。在本研究中,我们报告了一种通过使用目标卤代污染物(如四溴双酚 A(TBBPA)、2,3-二氯苯酚(2,3-DCP)和 2,4,6-三氯苯酚(2,4,6-TCP))作为起始单体来合成可再生和可重复使用的 MONs 的可行方法。TBBPA、2,3-DCP 和 2,4,6-TCP 既是危险污染物,也是 MONs 的起始单体,导致吸附剂和吸附质的回收。所得的 TBBPA-MON、2,3-DCP-MON 和 2,4,6-TCP-MON 不仅对其去除具有良好的可重复使用性和大的吸附容量,而且还依靠多种相互作用对其他酚类污染物具有良好的吸附作用。密度泛函理论计算表明,在吸附过程中π-π 和疏水性相互作用起主导作用,氢键相互作用起次要作用。使用过的 TBBPA-MON 可以重复使用,洗脱的 TBBPA 可以回收和更新,用于构建新的 MONs。本研究为设计和合成用于环境污染物的可再生 MONs 提供了一种可行的方法。