Usman Jamilu, Abba Sani I, Baig Nadeem, Abu-Zahra Nidal, Hasan Shadi W, Aljundi Isam H
Interdisciplinary Research Centre for Membranes and Water Security (IRC-MWS), King Fahd University of Petroleum and Minerals, Dhahran 31261, Saudi Arabia.
Materials Science and Engineering Department, University of Wisconsin-Milwaukee, 3200 North Cramer Street, Milwaukee, Wisconsin 53201, United States.
ACS Appl Mater Interfaces. 2024 Apr 3;16(13):16271-16289. doi: 10.1021/acsami.4c00752. Epub 2024 Mar 21.
Significant progress has been made in designing advanced membranes; however, persistent challenges remain due to their reduced permeation rates and a propensity for substantial fouling. These factors continue to pose significant barriers to the effective utilization of membranes in the separation of oil-in-water emulsions. Metal-organic frameworks (MOFs) are considered promising materials for such applications; however, they encounter three key challenges when applied to the separation of oil from water: (a) lack of water stability; (b) difficulty in producing defect-free membranes; and (c) unresolved issue of stabilizing the MOF separating layer on the ceramic membrane (CM) support. In this study, a defect-free hydrolytically stable zirconium-based MOF separating layer was formed through a two-step method: first, by in situ growth of UiO-66-NH MOF into the voids of polydopamine (PDA)-functionalized CM during the solvothermal process, and then by facilitating the self-assembly of UiO-66-NH with PDA using a pressurized dead-end assembly. A stable MOF separating layer was attained by enriching the ceramic support with amines and hydroxyl groups using PDA, which assisted in the assembly and stabilization of UiO-66-NH. The PDA-s-UiO-66-NH-CM membrane displayed air superhydrophilicity and underwater superoleophobicity, demonstrating its oil resistance and high antifouling behavior. The PDA-s-UiO-66-NH-CM membrane has shown exceptionally high permeability and separation capacity for challenging oil-in-water emulsions. This is attributed to numerous nanochannels from the membrane and its high resistance to oil adhesion. The membranes showed excellent stability over 15 continuous test cycles, which indicates that the developed MOFs separating layers have a low tendency to be clogged by oil droplets during separation. Machine learning-based Gaussian process regression (GPR) models as nonparametric kernel-based probabilistic models were employed to predict the performance efficiency of the PDA-s-UiO-66-NH-CM membrane in oil-in-water separation. The outcomes were compared with the support vector machine (SVM) and decision tree (DT) algorithm. This efficiency includes various metrics related to its separation accuracy, and the models were developed through feature engineering to identify and utilize the most significant factors affecting the membrane's performance. The results proved the reliability of GPR optimization with the highest prediction accuracy in the validation phase. The average percentage increase of the GPR model compared to the SVM and DT model was 6.11 and 42.94%, respectively.
在先进膜的设计方面已经取得了重大进展;然而,由于其渗透率降低和容易出现严重污染的问题,仍然存在持续的挑战。这些因素继续对膜在水包油乳液分离中的有效利用构成重大障碍。金属有机框架(MOF)被认为是适用于此类应用的有前景的材料;然而,当应用于油水分离时,它们面临三个关键挑战:(a)缺乏水稳定性;(b)难以制备无缺陷的膜;(c)在陶瓷膜(CM)载体上稳定MOF分离层的问题尚未解决。在本研究中,通过两步法形成了无缺陷的水解稳定的锆基金属有机框架分离层:首先,在溶剂热过程中,通过将UiO-66-NH MOF原位生长到聚多巴胺(PDA)功能化的CM的孔隙中,然后通过加压死端组装促进UiO-66-NH与PDA的自组装。通过使用PDA使陶瓷载体富含胺基和羟基来获得稳定的MOF分离层,这有助于UiO-66-NH的组装和稳定。PDA-s-UiO-66-NH-CM膜表现出空气超亲水性和水下超疏油性,证明了其耐油性和高抗污性能。PDA-s-UiO-66-NH-CM膜对具有挑战性的水包油乳液表现出极高的渗透率和分离能力。这归因于膜中的大量纳米通道及其对油粘附的高抗性。这些膜在15个连续测试循环中表现出优异的稳定性,这表明所开发的MOF分离层在分离过程中被油滴堵塞的倾向较低。基于机器学习的高斯过程回归(GPR)模型作为基于非参数核的概率模型,被用于预测PDA-s-UiO-66-NH-CM膜在水包油分离中的性能效率。将结果与支持向量机(SVM)和决策树(DT)算法进行了比较。这种效率包括与其分离精度相关的各种指标,并且通过特征工程开发模型以识别和利用影响膜性能的最重要因素。结果证明了GPR优化在验证阶段具有最高预测精度的可靠性。与SVM和DT模型相比,GPR模型的平均百分比增幅分别为6.11%和42.94%。