Department of Civil Engineering, University of Louisiana at Lafayette, Lafayette, LA, 70504, USA; Center for Environmental Technology, The Energy Institute of Louisiana, University of Louisiana at Lafayette, P. O. Box 43597, Lafayette, LA, 70504, USA.
Department of Civil Engineering, University of Louisiana at Lafayette, Lafayette, LA, 70504, USA; Beijing International Scientific and Technological Cooperation Base of Water Pollution Control Techniques for Antibiotics and Resistance Genes, School of Civil Engineering, Beijing Jiaotong University, Shangyuancun, Beijing, 100044, PR China.
Chemosphere. 2022 Dec;308(Pt 2):136379. doi: 10.1016/j.chemosphere.2022.136379. Epub 2022 Sep 8.
This research aimed to evaluate the adsorption behaviors and mechanisms of perfluorooctanoic acid (PFOA) onto polyethyleneimine modified graphene oxide (GO-PEI) from aqueous solutions. The adsorption capacity was significantly improved by doping polyethyleneimine (PEI) onto graphene oxide (GO). The Brunauer-Emmett-Teller (BET) isotherm model was considered as the best isotherm model in describing the PFOA adsorption onto GO-PEI3 (w/w = 3). GO-PEI3 exhibited high adsorption capacity (q = 368.2 mg/g, calculated from BET isotherm model) and excellent stability. The maximum monolayer amount of PFOA adsorption onto GO-PEI3 (q = 231.2 mg/g) was successfully evaluated. The calculated saturated concentration (C = 169.9 mg/L) of PFOA on GO-PEI3 closely agrees with its critical micelle concentration (CMC = 157.0 mg/L), suggesting the formation of multilayer hemi-micelles or micelles PFOA structures on the surface of GO-PEI3. PFOA adsorption onto GO-PEI3 was inhibited by several factors including: the presence of humic acid (HA) by competing with the adsorption sites, background salts through the double-layer compression effect, and the competition from soluble ions for the amine or amide functional groups on GO-PEI3. Finally, both the FT-IR and XPS results confirmed that the adsorption of PFOA onto GO-PEI3 was through electrostatic attraction and hydrophobic interaction (physical adsorption), but not chemical adsorption. This work provides fundamental knowledge both in understanding the adsorption behavior through the BET isotherm model and in developing a stable adsorbent for PFOA adsorption. In addition, the findings highlight the potential of PFOA remediation from wastewater systems using GO-PEI in engineering applications.
本研究旨在评估全氟辛酸(PFOA)在水溶液中于聚乙烯亚胺修饰氧化石墨烯(GO-PEI)上的吸附行为和机制。通过在氧化石墨烯(GO)上掺杂聚乙烯亚胺(PEI),吸附能力得到显著提高。BET 等温线模型被认为是描述 PFOA 在 GO-PEI3 上吸附的最佳等温线模型(w/w=3)。GO-PEI3 表现出高吸附容量(q=368.2mg/g,根据 BET 等温线模型计算)和优异的稳定性。成功评估了 PFOA 在 GO-PEI3 上吸附的最大单层量(q=231.2mg/g)。计算得到的 PFOA 在 GO-PEI3 上的饱和浓度(C=169.9mg/L)与 PFOA 的临界胶束浓度(CMC=157.0mg/L)非常接近,表明 PFOA 结构在 GO-PEI3 表面形成了多层半胶束或胶束。GO-PEI3 上 PFOA 的吸附受到多种因素的抑制,包括:与吸附位点竞争的腐殖酸(HA)的存在、通过双层压缩效应的背景盐以及可溶性离子对 GO-PEI3 上胺或酰胺官能团的竞争。最后,FT-IR 和 XPS 结果均证实 PFOA 与 GO-PEI3 的吸附是通过静电吸引和疏水相互作用(物理吸附),而不是化学吸附。这项工作为通过 BET 等温线模型理解吸附行为以及开发用于 PFOA 吸附的稳定吸附剂提供了基础知识。此外,研究结果强调了在工程应用中使用 GO-PEI 从废水系统中去除 PFOA 的潜力。