Article
Polymer Science
Noelia Esteban, Marta Juan-y-Seva, Carla Aguilar-Lugo, Jesus A. Miguel, Claudia Staudt, Jose G. de la Campa, Cristina Alvarez, Angel E. Lozano
Summary: A series of aromatic copolyimides with high molecular weight and good mechanical properties were obtained. These polymers could be used as gas separation membranes.
Article
Chemistry, Multidisciplinary
Min Liu, Ke Xie, Mitchell D. Nothling, Lianhai Zu, Shenlong Zhao, Dalton J. E. Harvie, Qiang Fu, Paul A. Webley, Greg G. Qiao
Summary: The incorporation of trace amounts of amorphous MOF nanosheets into the gutter layer of TFC assemblies can simultaneously address the limitations of thickness-dependent gas permeability of materials like PDMS and the geometric restriction effect due to limited pore accessibility of the substrate. The resulting PDMS&MOF membrane shows excellent CO2 permeance and CO2/N-2 selectivity. By leveraging this strategy, a novel TFC membrane with unprecedented gas-separation performance was successfully fabricated, demonstrating the design and fabrication potential for new TFC membrane systems.
ACS CENTRAL SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Diletta Morelli Venturi, Maria Sole Notari, Roberto Bondi, Edoardo Mosconi, Waldemar Kaiser, Giorgio Mercuri, Giuliano Giambastiani, Andrea Rossin, Marco Taddei, Ferdinando Costantino
Summary: A novel Zr-IV-based perfluorinated metal-organic framework (PF-MOF) was synthesized under solvent-free conditions, and it was found that Zr-IV can replace Zr fumarate to change the framework structure. Furthermore, introducing perfluorinated linkers through postsynthetic exchange reactions can enhance the CO2 adsorption capacity, and solid-state density functional theory calculations provided insights into the thermodynamics of CO2 adsorption.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Chemical
Menno Houben, Romy van Geijn, Machiel van Essen, Zandrie Borneman, Kitty Nijmeijer
Summary: The high-pressure behavior of supercritical carbon dioxide in glassy Matrimid (R) 5218 polymer membranes was investigated, with emphasis on the impact of CO2 fluid density and plasticization phenomena on CO2 permeability.
JOURNAL OF MEMBRANE SCIENCE
(2021)
Article
Materials Science, Multidisciplinary
Chengze Xu, Xiang Wang, Zhiyong Yu, Jianbo Gu, Xiangyang Feng, Siyuan Zhang
Summary: In order for ultra-large-scale integrated circuits to advance quickly, the demand for dielectric materials with ultra-low permittivity, excellent mechanical properties, and moisture resistance is high. Here, a series of F-SiO2/PI nanofiber films with ultralow dielectric constants have been successfully created through coaxial electrospinning and in situ sol-gel techniques, making them suitable for use in moisture conditions. The film's introduction of fluorinated substituents and high porosity allows for ultralow dielectric constants, less than 1.8 at 1 MHz, and high hydrophobicity with contact angles greater than 145 degrees. The F-SiO2/PI films offer great potential as insulating materials for electronics and microelectronics.
JOURNAL OF MATERIALS SCIENCE
(2023)
Article
Engineering, Chemical
Taejun Park, Eunhyea Chung
Summary: PEBAX 2533 membrane was used to study plasticization by low-pressure carbon dioxide (CO2). The Rest test, a new experimental technique, was introduced to reduce complex interactions caused by hydrostatic pressure and competitive sorption. During the Rest test, the permeability of the membrane increases by at least 50% when it is rested for more than 9 hours with residual CO2 after permeation. The permeability increase is influenced by factors such as the permeate side purge, rest period, fugacity and sorption of leftover CO2.
ASIA-PACIFIC JOURNAL OF CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Physical
Ioannis Tanis, David Brown, Sylvie Neyertz, Milind Vaidya, Jean-Pierre Ballaguet, Sebastien Duval, Ahmad Bahamdan
Summary: This study compared the transport of N-2 and CH4 in a polyimide precursor and its TR-PBO derivative, and found that the TR-PBO has higher diffusivities and permeabilities.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Engineering, Chemical
Can Wang, Zhili Cai, Wei Xie, Yang Jiao, Lu Liu, Lili Gong, Qi-Wei Zhang, Xiaohua Ma, Hongjun Zhang, Shuangjiang Luo
Summary: This study reports a new series of dual thermally crosslinkable polyimide membranes with excellent plasticization resistance and hierarchical microcavity size distribution. The gas transport properties of the crosslinked membranes can be tuned through chemical compositions and thermal treatment procedures.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Article
Engineering, Chemical
Tae Hoon Lee, Byung Kwan Lee, Chaewon Youn, Jun Hyeok Kang, Yu Jin Kim, Kwan Il Kim, Ye Rim Ha, Yejin Han, Ho Bum Park
Summary: This paper proposes a novel strategy to improve the interfacial compatibility between filler and matrix by integrating the diamino crosslinking of polyimide (6FDA-DAM) membranes and the fabrication of their mixed matrix membranes (MMMs). The crosslinked MMMs show enhanced interfacial compatibility and significantly improved separation performances for propylene/propane (C3H6/C3H8). The study demonstrates the potential of these novel MMMs for industrial applications.
JOURNAL OF MEMBRANE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Denis Andzheevich Sapegin, Danila Alexandrovich Kuznetsov, Joseph C. Bear
Summary: This article investigates the synthesis approaches and properties analysis of 1,2-disulfonimide fragment, and reveals the peculiarities of chlorination reaction and oxidation reaction.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Thermodynamics
Zhixia Deng, Shuanshi Fan, Yanhong Wang, Xuemei Lang, Gang Li, Faping Liu, Mengyang Li
Summary: In this study, the promotion effects of four different morphologies and hydrophobic properties of graphite on hydrate were compared to identify a mode for promoting CO2 hydrate formation. The results showed that fluorinated graphene with superhydrophobic nanostructure had the strongest gas storage effect by promoting hydrate nucleation and sustainable growth. When combined with surfactant SDS, the system achieved the best performance with a gas storage capacity of 5.02 mmol/g H2O. This mode of enhancing mass transfer at the gas-liquid interface provided a novel way to promote hydrate-based applications and carbon sequestration technology.
Article
Polymer Science
Weijie Hong, Lili Yuan, Yanping Ma, Chao Cui, Haoyang Zhang, Shiyong Yang, Wen-Hua Sun
Summary: Phenylethynyl-terminated aromatic polyimides are suitable for resin transfer molding (RTM) with high glass transition temperature. The relationship between the polyimide backbone structure and melting stability was investigated. Electron-withdrawing ability of oligoimide backbone significantly affects the curing reactivity of terminated phenylethynyl groups.
Article
Engineering, Chemical
Min Gu, Xi Qing, Xiaoyang Tang, Tingyu Zhuo
Summary: The adsorption kinetic behaviors of CO2 on WF shale were investigated in different pressure and temperature ranges. The results showed that the adsorption curves exhibited different types of fluctuations depending on the pressure and temperature. These behaviors were determined by the change rate of CO2 physical parameters, and exhibited fluctuation in the near-critical region.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Polymer Science
Fan Zhang, Jinhui Li, Tao Wang, Chao Huang, Fei Ji, Liang Shan, Guoping Zhang, Rong Sun, Ching-ping Wong
Summary: This study introduced an effective approach to fabricate novel fluorinated graphene/polyimide nanocomposite films, and investigated the effects of different loading amounts of fluorinated graphene on the film properties.
JOURNAL OF APPLIED POLYMER SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Junnan Li, Nikolay Kornienko
Summary: This study developed a synthetic scheme that couples CO2 and NH3 at a gas-liquid-solid boundary to produce species with C-N bonds. By using electrochemical analysis and operando spectroelectrochemical method, the reaction pathways and limitations of the current system were analyzed.
Article
Chemistry, Physical
Angelina Folberth, Swaminath Bharadwaj, Nico F. A. van der Vegt
Summary: Our study investigates the impact of TMAO on the solvation of nonpolar solutes in water through MD simulations and free-energy calculations. We find that TMAO can exhibit a surfactant-like behavior, preferring to bind to large solutes and reducing the free-energy cost of solute-cavity formation. This behavior reinforces the solvent-mediated attraction between large solutes by means of an entropic force related to the accumulation of TMAO at interfaces.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Angelina Folberth, Nico F. A. van der Vegt
Summary: The effects of trimethylamine-N-oxide (TMAO) on the solvation and interactions of methane in water were studied through Molecular Dynamics simulations. It was found that TMAO has a temperature-dependent effect on the solubility of methane. At low temperatures, TMAO reduces the solubility of methane in water, while at higher temperatures, TMAO promotes methane solubility. The analysis suggests that the reversible work of creating a repulsive methane cavity outweighs the van der Waals interactions between methane and TMAO at lower temperatures. Above a certain temperature, the van der Waals interactions between TMAO and methane become more significant. Additionally, increasing TMAO concentration enhances the attraction between dissolved methane solutes.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Madhusmita Tripathy, Swaminath Bharadwaj, Nico F. A. van der Vegt
Summary: This study investigates the effect of urea and methanol on the density fluctuations and thermodynamic properties in the solvation shell of an extended hydrophobic solute. The results show that the mode of action of urea and methanol is strongly coupled to their hydration behavior, with urea preferential accumulation quenching density fluctuations and methanol accumulation enhancing density fluctuations.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Marvin P. Bernhardt, Yuki Nagata, Nico F. A. van der Veg
Summary: The use of Lennard-Jones potential in computer simulations of aqueous electrolyte solutions is common, but it fails to accurately represent the local properties of ion hydration shells. Effective pair potentials derived from ab initio MD data offer a promising alternative to represent these properties and local interactions of specific ions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Biochemistry & Molecular Biology
Sylvie Neyertz, David Brown, Saman Salimi, Farzaneh Radmanesh, Nieck E. Benes
Summary: This work demonstrates the potential of using atomistic molecular dynamics (MD) and grandcanonical Monte Carlo (GCMC) simulations to pre-screen candidate membrane structures for gas separation under harsh conditions. The study compares the CO2/CH4 and CO2/N-2 sieving properties of hybrid networks based on different inorganic precursors at different temperatures. The simulations provide insights into the performance of the membranes under high temperature and pressure conditions, which are difficult to measure experimentally. The results contribute to the development of efficient gas separation membranes for industrial applications.
Article
Chemistry, Physical
Viktor Klippenstein, Nico F. A. van der Vegt
Summary: This study develops coarse-grained implicit solvent models for the continuous Asakura-Oosawa model using a method based on generalized Langevin equations and projection operator formalism. The authors investigate the influence of different system parameters on the dynamic representability of the coarse-grained models.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Angelina Folberth, Nico F. A. van der Vegt
Summary: Studies have found that trimethylamine-N-oxide (TMAO) has a stabilizing effect on proteins under high pressure conditions. TMAO is depleted from the protein/water interface under high pressure, thus counterbalancing the unfavorable effect of elevated pressure on protein folding. TMAO also stabilizes interactions within the protein.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Marvin P. Bernhardt, Martin Hanke, Nico F. A. van der Vegt
Summary: This work investigates iterative methods for the inverse problem in structural coarse-graining. Fast Gauss-Newton schemes are derived based on integral equation theory, and can be applied to systems with bonds and mixtures. Stability problems are addressed and modified in terms of reproducing the pressure, Kirkwood-Buff integral, or the enthalpy of vaporization. The potential of this approach is demonstrated in deriving coarse-grained force fields for various solvents and mixtures.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Viktor Klippenstein, Nico F. A. van der Vegt
Summary: Molecular dynamics (MD) simulations based on coarse-grained (CG) particle models of molecular liquids misrepresent the time scales for molecular vibrations and diffusive motions. The parametrization of Generalized Langevin Equation (GLE) thermostats based on the microscopic dynamics of the fine-grained model provides a promising route to address this issue. A bottom-up dynamic coarse graining method, based on the Mori-Zwanzig formalism, accurately estimates isotropic GLE memory kernels for CG models of liquid water. In addition, an iterative optimization technique further improves the accuracy of representing the velocity autocorrelation function and structural relaxation.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Madhusmita Tripathy, Viktor Klippenstein, Nico F. A. van der Vegt
Summary: In this study, a new method of applying coarse-grained (CG) simulation models to multi-component molecular systems was investigated to represent structural, thermodynamic, and dynamic properties. The effectiveness of the method was validated through comparisons with fine-grained (FG) reference systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Varun Mandalaparthy, Madhusmita Tripathy, Nico F. A. van der Vegt
Summary: In this study, molecular dynamics simulations were used to investigate the molecular mechanism of salt-dependent dissociation of aspartic acid (Asp). It was found that increasing the size of the anion decreases the pKa of Asp, while the effect of cation size on pKa is nonmonotonic. The overall effect of salt on Asp acidity is determined by solvation and competing ion interactions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Ioannis Tanis, David Brown, Sylvie Neyertz, Milind Vaidya, Jean-Pierre Ballaguet, Sebastien Duval, Ahmad Bahamdan
Summary: This study compared the transport of N-2 and CH4 in a polyimide precursor and its TR-PBO derivative, and found that the TR-PBO has higher diffusivities and permeabilities.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yani Zhao, Swaminath Bharadwaj, Nico F. A. van der Vegt
Summary: This study investigates the combined effect of weakly hydrated and strongly hydrated ions on the lower critical solution temperature (LCST) of poly(N-isopropylacrylamide)(PNIPAM) using atomistic molecular dynamics simulations. The results show that the nonadditive ion effects on the coil-to-globule transitions of PNIPAM arise from the interplay between the depletion of strongly hydrated sulfate ions and the preferential accumulation of iodide ions on the polymer surface, leading to favorable PNIPAM-I- interactions. The depletion of sulfate ions and the binding of iodide ions are coupled through the role of cations, resulting in a mutual enhancement of both effects.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Review
Chemistry, Physical
Swaminath Bharadwaj, Bart-Jan Niebuur, Katja Nothdurft, Walter Richtering, Nico F. A. van der Vegt, Christine M. Papadakis
Summary: Cononsolvency is an intriguing phenomenon where a polymer collapses in a mixture of good solvents. It has been widely observed in different systems and has applications in various fields. In the past decade, there has been a renewed interest in understanding the molecular mechanisms driving cononsolvency.