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1. Data Driven Machine Learning for Estimation of PFAS Partitioning on Various Surface Materials

   Harsh V. Patel, Hyoshin Park (June 2023, AEESP Research and Education Conference 2023)

   This study, data driven machine learning model was developed to estimate the partitioning of Per- and Poly-fluoroalkyl Substances (PFAS) compounds during aqueous adsorption on various adsorbent materials with a vision to potentially replace the time-consuming and labor-intensive adsorption experiments. Various regression models were trained and tested using previously published data. 290 data points and 170 data points for activated carbon and mineral adsorbents, respectively, were mined for training the models and 10 data points were used to test the trained models. Statistical parameters, such as Root-Mean-Square Error (RSME), R-Squared, Mean Average Error (MAE), Mean Squared Error (MSE), etc., were used to compare the regression models. It was found that rational quadratic GPR (R-squared = 0.9966) and fine regression tree (R-Squared = 0.9427) models had the highest estimation accuracy for carbon-based and mineral-based adsorbents, respectively. These models were then validated for prediction accuracy using 10 data points from previous studies as an outer test set. Rational quadratic GPR was able to achieve 99% prediction accuracy for carbon-based adsorbent, while fine tree regression model was able to achieve 94% prediction accuracy. Despite such high estimation accuracy, the data mining process revealed the data shortage and the need for more research on PFAS adsorption to present real-world models. This study, as one of the first, shed a light on the determination of key parameters in aquatic chemistry with data mining and machine learning approaches. 

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2. Evaluation of a Porous Membrane as a Mass-Transfer Efficient Structure for the Adsorption of Per- and Polyfluoroalkyl Substances from Drinking Water

   https://doi.org/10.1021/acsestengg.3c00515  

   Kim, Jeein; Chernysheva, Liliya; Xu, Jialing; McClure, Matthew; Latulippe, David R; Phillip, William A; Doudrick, Kyle (May 2024, ACS ES&T Engineering)

   With drinking water regulations forthcoming for per- and polyfluoroalkyl substances (PFAS), the need for cost-effective treatment technologies has become urgent. Adsorption is a key process for removing or concentrating PFAS from water; however, conventional adsorbents operated in packed beds suffer from mass transfer limitations. The objective of this study was to assess the mass transfer performance of a porous polyamide adsorptive membrane for removing PFAS from drinking water under varying conditions. We conducted batch equilibrium and dynamic adsorption experiments for perfluorooctanesulfonic acid, perfluorooctanoic acid, perfluorobutanesulfonic acid, and undecafluoro-2-methyl-3-oxahexanoic acid (i.e., GenX). We assessed various operating and water quality parameters, including flow rate (pore velocity), pH, ionic strength (IS), and presence of dissolved organic carbon. Outcomes revealed that the porous adsorptive membrane was a mass transfer-efficient platform capable of achieving dynamic capacities similar to equilibrium capacities at fast interstitial velocities. The adsorption mechanism of PFAS to the membrane was a mixture of electrostatic and hydrophobic interactions, with pH and IS controlling which interaction was dominant. The adsorption capacity of the membrane was limited by its surface area, but its site density was approximately five times higher than that of granular activated carbon. With advances in molecular engineering to increase the capacity, porous adsorptive membranes are well suited as alternative adsorbent platforms for removing PFAS from drinking water. 

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3. Lipid membrane interactions of self-assembling antimicrobial nanofibers: effect of PEGylation

   https://doi.org/10.1039/D0RA07679A  

   Nielsen, Josefine Eilsø; König, Nico; Yang, Su; Skoda, Maximilian W.; Maestro, Armando; Dong, He; Cárdenas, Marité; Lund, Reidar (September 2020, RSC Advances)

   null (Ed.)

   Supramolecular assembly and PEGylation (attachment of a polyethylene glycol polymer chain) of peptides can be an effective strategy to develop antimicrobial peptides with increased stability, antimicrobial efficacy and hemocompatibility. However, how the self-assembly properties and PEGylation affect their lipid membrane interaction is still an unanswered question. In this work, we use state-of-the-art small angle X-ray and neutron scattering (SAXS/SANS) together with neutron reflectometry (NR) to study the membrane interaction of a series of multidomain peptides, with and without PEGylation, known to self-assemble into nanofibers. Our approach allows us to study both how the structure of the peptide and the membrane are affected by the peptide–lipid interactions. When comparing self-assembled peptides with monomeric peptides that are not able to undergo assembly due to shorter chain length, we found that the nanofibers interact more strongly with the membrane. They were found to insert into the core of the membrane as well as to absorb as intact fibres on the surface. Based on the presented results, PEGylation of the multidomain peptides leads to a slight net decrease in the membrane interaction, while the distribution of the peptide at the interface is similar to the non-PEGylated peptides. Based on the structural information, we showed that nanofibers were partially disrupted upon interaction with phospholipid membranes. This is in contrast with the considerable physical stability of the peptide in solution, which is desirable for an extended in vivo circulation time. 

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4. Zwitterionic copolymer additive architecture affects membrane performance: fouling resistance and surface rearrangement in saline solutions

   https://doi.org/10.1039/C8TA11553B  

   Kaner, Papatya; Dudchenko, Alexander V.; Mauter, Meagan S.; Asatekin, Ayse (February 2019, Journal of Materials Chemistry A)

   Membrane separations are simple to operate, scalable, versatile, and energy efficient, but their broader use is curtailed by fouling or performance decline due to feed component depositing on the membrane surface. Surface functionalization with groups such as zwitterions can mitigate the adsorption of organic compounds, thus limiting fouling. This can be achieved by using surface-segregating copolymer additives during membrane manufacture, but there is a need for better understanding of how the polymer structure and architecture affect the effectiveness of these additives in improving membrane performance. In this study, we aim to explore the impact of the architecture of zwitterionic copolymer additives for polyvinylidene fluoride (PVDF)-based membranes in fouling mitigation and ionic strength response. We prepared membranes from blends of PVDF with zwitterionic (ZI) copolymers with two different architectures, random and comb-shaped. As the random copolymer, we used poly(methyl methacrylate- random- sulfobetaine-2-vinyl pyridine) (PMMA- r -SB2VP) synthesized by free radical polymerization. The comb-shaped copolymer was synthesized by grafting SB2VP side-chains from a PVDF backbone by controlled radical polymerization. Membranes were fabricated from PVDF-copolymer blends containing up to 5 wt% ZI copolymer. Compared to the additive-free PVDF membrane, water permeance increased five-fold with 5 wt% addition of either copolymer. The comb copolymer additive led to better resistance to fouling by a saline oil-in-water emulsion and to simulated protein adsorption in Atomic Force Microscopy (AFM) force measurements. The additive architecture had a significant influence on how membranes respond to changes in feed salinity, which is known to affect intra- and inter-molecular interactions in zwitterionic polymers. The random copolymer containing membrane showed a small and mostly reversible decrease in its permeance with salinity. In contrast, the comb copolymer-containing membrane underwent a conformational reorganization in saline solutions that leads to an irreversible permeance decrease, increased zwitterionic group content on the membrane surface, and smoother surface topography. The higher mobility of the zwitterionic groups in the comb-shaped architecture facilitates reorganization of the zwitterionic side-chains in response to ionic strength. Overall, this study establishes a new approach for developing highly fouling resistant membranes and defines how the architecture of a zwitterionic copolymer additive impacts the ionic strength response and fouling resistance of the membrane. 

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5. Metal-organic frameworks for water vapor adsorption

   https://doi.org/10.1016/j.chempr.2023.09.005  

   Shi, Le; Kirlikovali, Kent O; Chen, Zhijie; Farha, Omar K (February 2024, Chem)

   Water is the most abundant and cleanest natural resource on earth, and it is the driving force of all nature. It not only affects food security, human health, and ecosystem integrity and maintenance, but is also an important driver of energy in industrial production and life. Importantly, water adsorption applications are considered to be highly energy-efficient and environmentally friendly technologies,1 including atmospheric water harvesting,2-4 desiccation of clean gases,5 indoor humidity control,6,7 and adsorptive heat transformation.8,9 However, current water adsorption-related applications are still constrained by properties of adsorbents, such as their low water uptake capacities, poor cyclic stabilities, limited feasibilities over a range of humidity conditions, and minimal commercial availabilities. Conventional nanoporous materials (e.g., silica gels, zeolites, and clays) were the first adsorbents used in water capture applications due to their low cost, commercial availability, and favorable water adsorption kinetics. However, these materials generally suffer from either low water uptake capacities or high regeneration temperature, limiting their use in practical water absorption applications.1,10 Metal-organic frameworks (MOFs), a class of crystalline porous materials, are assembled from inorganic nodes and organic linkers through coordination bonds.11,12 Benefiting from their exceptional porosity and surface area, tunable pore size and geometry, and highly tailorable and designable structures and functionalities, MOFs show considerable potential for gas storage and separation, heterogeneous catalysis, and other energy and environmental sustainability applications.13-17 In recent years, MOFs have also shown great potential for water vapor adsorption because of a growing understanding of the relationship between MOFs and water, as well as an increasing number of reports detailing MOFs that exhibit high water stability.1,4,9 Moreover, judicious design of the MOF structures enables control over their water adsorption properties and the water uptake capacities, which make MOFs ideal candidates for water adsorption-related applications. This review aims to provide an overview of recent advances in the development of MOFs for water adsorption, as well as to offer proposed guidelines to develop even better water adsorption materials. First, we briefly introduce the fundamentals of water adsorption, including how to ascertain key insights based on the shapes of water adsorption isotherms, descriptions of various water adsorption mechanisms, and a discussion on the stability of MOFs in water systems. Next, we discuss several recent reports have detailed how to improve water uptake capacity through the design and synthesis of MOFs. In particular, we highlight the importance of reticular chemistry in the designed synthesis of MOF-based water adsorbent materials. We then shift our focus to discussing the enormous potential of MOFs for use in selective water vapor adsorption applications with both theoretical and practical considerations considered. Finally, we offer our thoughts on the future development of this field in three aspects: chemistry and materials design, process engineering, and commercialization of MOFs for water adsorption. We hope that this review will provide fundamental insights for chemists and inspire them to synthesize MOFs with better water adsorption performance; and provide assistance to engineers researching MOF-based water adsorption devices and working towards the development of highly energy-efficient and environmentally friendly technologies with reduced carbon footprints. 

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