International Postgraduate Programs in Hazardous Substance and Environmental Management, Graduate School, Chulalongkorn University, Bangkok, 10330, Thailand; Center of Excellence on Hazardous Substance Management, Chulalongkorn University, Bangkok, 10330, Thailand.
National Nanotechnology Center (NANOTEC), National Science and Technology Development Agency (NSTDA), Pathum Thani, 12120, Thailand; Research Network of NANOTEC - CU on Environment, Bangkok, 10330, Thailand.
Environ Res. 2021 May;196:110335. doi: 10.1016/j.envres.2020.110335. Epub 2020 Oct 16.
In this study, we investigated the synergetic effects of coexisting electrolytes and dissolved organic matter (DOM) on Carbamazepine (CBZ) and Ciprofloxacin (CIP) adsorption on the 1D flexible structure of MIL-53(Al) and 3D rigid structure of UiO-66(Zr). The effects of electrolytes on the adsorption of CBZ and CIP on 1D flexible framework of MIL-53(Al) were more significant than those observed from the 3D framework of UiO-66(Zr). The presence of sulfate, nitrate, and phosphate anions indicates high potential to promote the adsorption of CBZ and CIP onto MIL-53(Al) and UiO-66(Zr) because of the decrease of solubility and strengthening of electrostatic interactions by substitution of oxo-anions at the metal complex node via covalent bonding. The lower hydration energy of the potassium ion enhanced CBZ adsorption on MIL-53(Al), while the higher hydration energy of calcium and magnesium ions reduced the adsorption capacity of CBZ and CIP on MIL-53(Al) and UiO-66(Zr). CBZ interacted with fractionated humic acid better than CIP. High-density carboxylic and aromatic functional groups on humic acid ensured that only humic acid larger than 1KDa was adsorbed by MIL-53(Al). Tryptophan-like and humic acid-like DOM were both detected in real hospital effluent, and their effects on CIP and CBZ adsorption onto MIL-53(Al) were investigated. The presence of tryptophan did not affect CBZ adsorption on MIL-53(Al) (except when coexisting with calcium ions). Conversely, tryptophan interfered with CIP adsorption. The presence of humic acid lower than 1KDa promoted the adsorption of CBZ and CIP by increasing the breathing effect of MIL-53(Al)'s 1D flexible framework. The presence of humic acid with molecular size greater than 1KDa enhanced both CBZ and CIP adsorption via a multilayer adsorption mechanism.
在这项研究中，我们研究了共存电解质和溶解有机物（DOM）对卡马西平（CBZ）和环丙沙星（CIP）在 MIL-53（Al）一维柔性结构和 UiO-66（Zr）三维刚性结构上吸附的协同作用。电解质对 CBZ 和 CIP 在 MIL-53（Al）一维柔性骨架上吸附的影响比在 UiO-66（Zr）三维骨架上观察到的影响更大。硫酸盐、硝酸盐和磷酸盐阴离子的存在表明，由于通过共价键取代金属配合物节点上的氧阴离子，增加了静电相互作用并降低了溶解度，因此具有促进 CBZ 和 CIP 吸附到 MIL-53（Al）和 UiO-66（Zr）的高潜力。钾离子的较低水合能增强了 CBZ 在 MIL-53（Al）上的吸附，而钙和镁离子的较高水合能降低了 CBZ 和 CIP 在 MIL-53（Al）和 UiO-66（Zr）上的吸附能力。CBZ 与腐殖酸的分级混合物相互作用优于 CIP。腐殖酸中高密度的羧酸和芳香族官能团确保只有大于 1KDa 的腐殖酸被 MIL-53（Al）吸附。在实际医院废水中检测到色氨酸样和腐殖酸样 DOM，并研究了它们对 CIP 和 CBZ 吸附到 MIL-53（Al）的影响。色氨酸的存在并不影响 CBZ 在 MIL-53（Al）上的吸附（除非与钙离子共存）。相反，色氨酸干扰了 CIP 的吸附。低于 1KDa 的腐殖酸的存在通过增加 MIL-53（Al）的 1D 柔性骨架的呼吸效应促进了 CBZ 和 CIP 的吸附。大于 1KDa 的分子大小的腐殖酸的存在通过多层吸附机制增强了 CBZ 和 CIP 的吸附。
