Article
Chemistry, Physical
Hua Li, Jianan Wang, Gregory G. Warr, Rob Atkin
Summary: The dynamics of self-assembled liquid nanostructures of ionic liquids near a mica surface were determined using video-rate atomic force microscopy (AFM) data. The AFM videos revealed that the nanostructures near the surface diffused much slower than individual ions in the bulk. This finding has important implications for processes involving concentrated electrolyte interfacial dynamics.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Biochemistry & Molecular Biology
Isabella DeStefano, Gabriella DeStefano, Nicholas J. Paradis, Roshani Patel, Austin K. Clark, Hunter Gogoj, Gurvir Singh, Keertana S. Jonnalagadda, Aashka Y. Patel, Chun Wu, Gregory A. Caputo, Timothy D. Vaden
Summary: The study investigated the thermal unfolding of the copper redox protein azurin in the presence of four different amino acid-based ionic liquids (ILs), showing that these ILs destabilize the protein structure and decrease its melting temperature. ILs with alcohol side chains have a stronger impact on protein stability, while those with acidic side chains have weaker effects.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2021)
Article
Chemistry, Multidisciplinary
Leonhard Winter, Radha G. Bhuin, Florian Maier, Hans-Peter Steinrueck
Summary: This study explores the interaction of molecules at the gas/ionic liquid surface and investigates the dynamics of this process through measuring the trapping probabilities of gases on IL surfaces. The results show that desorption energy increases with longer alkyl chain length and smaller anion size, while the adsorption energy is dependent on the properties of the adsorbing molecules.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Engineering, Chemical
Jingyu Qin, Yanlei Wang, Zhongdong Gan, Weili Ma, Feng Huo, Yi Nie, Chao Yang, Hongyan He
Summary: This study investigates the flow behavior and controlling mechanism of ionic liquids (ILs) driven by an electric field through molecular dynamics simulations. The results reveal that during the flow process, cations tend to locate at the interface in a perpendicular configuration, while anions distribute randomly. The size of the nanochannel has a larger impact on the velocity and flux of confined ILs compared to pressure and surface charging density.
CHEMICAL ENGINEERING SCIENCE
(2022)
Article
Electrochemistry
Jingyu Qin, Mi Wang, Yanlei Wang, Chenlu Wang, Yumiao Lu, Feng Huo, Hongyan He
Summary: This study reveals that the structure variation of ionic liquids near electrodes, including the accumulation and expulsion of anions, the evolution of layered structure of cations and anions, as well as the impact of side-chain elongation and sulfonic modification, can provide practical guidelines for the design and management of ionic liquids in electrochemical processes.
Article
Chemistry, Physical
Andrei Filippov, Oleg N. Antzutkin
Summary: Some ILs containing nitrate anion exhibit unique dynamic behavior of cations when confined between glass plates. By using O-17 and N-15 NMR spectroscopy, we investigated the state and transformations of isotopically enriched nitrate anion in ethylammonium nitrate (EAN) enclosed between glass plates. Our results indicate that EAN forms an ordered phase similar to a liquid crystal, with preferential orientation of nitrate anions and no predominant orientation of cations. The phase also exhibits altered local and translational dynamics, as well as slow transformation under an external magnetic field.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Olga D. Bakulina, Mikhail Yu. Ivanov, Sergey A. Prikhod'ko, Nicolay Yu. Adonin, Matvey V. Fedin
Summary: Ionic liquids (ILs) can form various nanostructures due to their amphiphilic nature. In this study, we investigate the structural anomalies in zwitterionic IL glasses (ZILs), where the cation and anion are bound in a single molecule. The binding restricts mutual diffusion of cations and anions, leading to modification of nano-ordering and structural anomalies compared to common ILs. This work expands the understanding of structural anomalies in IL glasses and suggests new routes to tune their properties.
Article
Biochemistry & Molecular Biology
Andrea Amadei, Andrea Ciccioli, Antonello Filippi, Caterina Fraschetti, Massimiliano Aschi
Summary: A theoretical-computational procedure based on the quasi-Gaussian entropy theory and molecular dynamics simulations is proposed. It can construct an analytical model of the most relevant thermodynamic properties within a wide temperature range by automatically sampling the entire conformational repertoire of highly flexible systems. The method's reliability mainly depends on the quality of the force field used in the simulations and the ability to distinguish between semi-classical and quantum degrees of freedom in a physically coherent way.
Article
Chemistry, Physical
Addison Jung, David Reha, Babak Minofar, Petr Stanovsky, Mariia Pasichnyk, Michal Pribyl, Jason E. Bara, Karel Friess, Vlastimil Fila, Pavel Izak
Summary: The embedding of ionic liquids (ILs) into the polymer membrane matrix affects the morphology and properties of the material. Polymer-IL systems generally exhibit improved separation properties due to the unique nature of ILs. In this study, the CO2/CH4 separation properties of poly (vinylidene fluoride-co-hexafluoropropylene)) (poly (VDF-HFP)) with different amounts of 1-ethyl-3-methylimidazolium bis (trifluoromethylsulfonyl) imide ([EMIM] [TFSI]) were simulated using classical molecular dynamics (MD).
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Vinicius Piccoli, Leandro Martinez
Summary: Ionic liquids (ILs) are widely used in biotechnological applications for their interactions with proteins. In this study, we investigated the solvation of different ubiquitin folding states in IL aqueous solutions and found that ILs preferentially solvate protein structures and are considered denaturants. The exposure of low-polarity residues during protein denaturation allows favorable interactions with ILs, stabilizing the protein core.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Leonhard Winter, Simon Trzeciak, Cynthia C. Fernandez, Stephen Massicot, Timo Talwar, Florian Maier, Dirk Zahn, Hans-Peter Steinrueck
Summary: The SCILL concept is a promising method to enhance the selectivity of hydrogenation reactions. By studying the modification of Pt(111) surface with imidazolium ionic liquid, it is found that the IL film can effectively block the adsorption of 1-butene while not significantly affecting the adsorption of 1,3-butadiene. The densification/relaxation of the IL film is proposed as the key mechanism to control olefin adsorption.
Article
Engineering, Environmental
Qingxiang Liu, Tao Zhang, Peng Gao, Jun Gao, Dongmei Xu, Pingping Zhao, Lianzheng Zhang, Yinglong Wang
Summary: Ionic liquids with functional chemical sites can efficiently and selectively separate compounds. In this study, an IL with dual functional sites was designed and used to separate indole, with molecular dynamics simulation confirming the results.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Review
Chemistry, Multidisciplinary
Olga Lebedeva, Dmitry Kultin, Leonid Kustov
Summary: This review explores the characteristics of electrochemical synthesis of nanostructures in ionic liquids, emphasizing the production of various nanomaterials and nanoscale polymer films. It highlights the potential application of ILs as an electrochemical medium and the relative simplicity of experimental procedures.
Article
Polymer Science
Baris Demir, Gabriel Perli, Kit-Ying Chan, Jannick Duchet-Rumeau, Sebastien Livi
Summary: A new generation of polymerised ionic liquids with high thermal stability and good mechanical performances has been designed through novel CEILs, and a computational approach based on molecular dynamics simulations has been developed for predicting the thermo-mechanical properties of these materials. This provides a reproducible and reliable method for designing multi-functional thermoset polymers based on epoxidised ionic liquid monomers.
Article
Chemistry, Physical
Guilherme Ferreira Lemos Pereira, Eudes Eterno Fileti, Leonardo Jose Amaral Siqueira
Summary: Graphene oxide (GO) has been widely studied for its improved properties compared to pure graphene, which make it suitable for electrochemical energy storage applications. The oxygenated groups on the surface of GO enhance its ionic mobility and density of states while maintaining the same specific area as pure graphene. Moreover, the porous morphology of the electrode enhances electrode-electrolyte interactions and increases the contact area. This study investigates the structural aspects of porous GO electrodes in different ionic liquids using atomistic molecular dynamics simulations and provides insights into the charging mechanisms in the presence of each electrolyte.
Review
Chemistry, Multidisciplinary
Kateryna Goloviznina, Zheng Gong, Agilio A. H. Padua
Summary: This article discusses the importance of using molecular dynamics simulation and theoretical chemistry tools to study ionic liquids and eutectic solvents, as well as the use of polarizable force fields to describe their interactions and conformations. The development of polarizable force fields is a combination of science and art, with the main challenge being how to handle the diversity in chemical structures and interactions to build a model that can represent solutions, mixtures, and material interfaces effectively.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2022)
Article
Chemistry, Physical
Frederik Philippi, Kateryna Goloviznina, Zheng Gong, Sascha Gehrke, Barbara Kirchner, Agilio A. H. Padua, Patricia A. Hunt
Summary: The study focuses on the charge transfer and polarizability effects of 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide [C(4)C(1)im][NTf2] IL through classical molecular dynamics simulations. The methods for determining charge distributions and mean field charge transfer are discussed, and the impact of different charge models and scaling methods on simulations is investigated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Julian B. B. Beckmann, Daniel Rauber, Frederik Philippi, Kateryna Goloviznina, Jordan A. Ward-Williams, Andy J. Sederman, Mick D. Mantle, Agilio Padua, Christopher W. M. Kay, Tom Welton, Lynn F. Gladden
Summary: Understanding the molecular structure-property relationship of ionic liquids is crucial for practical applications. This study employs fast-field cycling and molecular dynamics simulations, combined with comprehensive physicochemical characterization, to provide insight into the molecular mechanics of ionic liquids.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Multidisciplinary
Maria Enrica Di Pietro, Kateryna Goloviznina, Adriaan van den Bruinhorst, Giselle de Araujo Lima e Souza, Margarida Costa Gomes, Agilio A. H. Padua, Andrea Mele
Summary: Deep eutectic solvents (DESs) added with lithium salts are emerging as alternative electrolytes for lithium-ion batteries. This study used experimental NMR techniques and molecular dynamics simulations to investigate the structure and dynamics of a prototype system composed of DES choline chloride:urea and lithium salt LiCl. The results reveal strong coordination between lithium cations and chloride anions, forming LiCl32- units, as well as an extensive hydrogen-bond network with other species. The effect of small quantities of water on the properties of the system is also discussed.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Thermodynamics
Diogo Machacaz, Tiago M. Eusebio, Catia Guarda, Goncalo M. C. Silva, Pedro Morgado, Luis F. G. Martins, Jose N. A. Canongia Lopes Lopes, Eduardo J. M. Filipe
Summary: The liquid density of five liquid 1H,1H-perfluorinated alcohols was measured as a function of pressure and temperature. The isothermal compressibility and isobaric thermal expansivity coefficients were calculated and compared with data from the literature for the equivalent hydrogenated alcohols. Molecular dynamics simulations provided molecular-level insight into the experimental results, particularly regarding the H-bond network and the effect of pressure on the liquid organization.
JOURNAL OF CHEMICAL AND ENGINEERING DATA
(2023)
Article
Chemistry, Medicinal
Ignazio Schino, Mariangela Cantore, Modesto de Candia, Cosimo D. Altomare, Catarina Maria, Joao Barros, Vasco Cachatra, Patricia Calado, Karina Shimizu, Adilson A. Freitas, Maria C. Oliveira, Maria J. Ferreira, Jose N. C. Lopes, Nicola A. Colabufo, Amelia P. Rauter
Summary: Alzheimer's Disease (AD) is characterized by an imbalance in cholinergic neurotransmission, and the inhibition of acetylcholinesterase (AChE) and increase of butyrylcholinesterase (BChE) activity. Novel 6-benzamide purine nucleosides that selectively target BChE and possess chelating properties were synthesized. These compounds show potential as dual target compounds for the treatment of AD.
Article
Biochemistry & Molecular Biology
Hugo Marques, Jose Nuno Canongia Lopes, Adilson Alves de Freitas, Karina Shimizu
Summary: The functionalization of polymers with sulfonate groups has diverse applications, including in biomedicine and oil recovery processes. Molecular dynamics simulations were used to study various ionic liquids (ILs) consisting of 1-alkyl-3-methylimidazolium cations [C(n)C(1)im](+) and alkyl-sulfonate anions [CmSO3](-). The analysis revealed that the structure of the ILs' polar network is largely unaffected by increasing aliphatic chain length, but shorter alkyl chains influence the nonpolar organization through electrostatic interactions and hydrogen bonding.
Article
Chemistry, Physical
Adilson Alves de Freitas, Amelia M. P. S. Gonsalves da Silva, Jose Nuno Canongia Lopes, Karina Shimizu
Summary: Experimental results revealed partial miscibility between the cationic surfactant DODAB and the ionic liquid [P6 6 6 14][N(CN)2]. Molecular dynamics simulations were performed to study the interactions between a 3:1 mixture of DODAB and [P6 6 6 14][N(CN)2] at the water-vacuum interface. The simulations showed the existence of surfactant-rich and IL-rich regions at the water surface in the low-pressure regime. Further compression led to phase separation due to the displacement of the ionic liquid by the cohesion forces between the hydrocarbon chains of the surfactant.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Karina Shimizu, Masayoshi Watanabe, Jose Nuno Canongia Lopes, Adilson Alves deFreitas
Summary: Experimental data shows that cation hopping or ligand-exchange mechanism plays a significant role in Li-ion conduction in highly concentrated electrolytes. This study used molecular dynamics simulations to investigate the solution structure and Li ion diffusion in LiBF4 solutions in sulfolane at high concentrations. The results revealed the formation of different networks shared by Li ions, BF4- ions, and sulfolane molecules, with the optimal network structure occurring at a mole fraction of sulfolane of approximately 0.67. The relaxation dynamics of these solutions resemble those of supercooled glass-forming liquids near the glass transition temperature, and the deviation from the Stokes-Einstein equation is mainly attributed to the relaxation process of Li-anion pairs.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Hugo Marques, Karina Shimizu, Isabel M. Marrucho
Summary: The symmetrical and unsymmetrical conventions for the reference state of the activity coefficients were used in combination with the Pitzer-Debye-Huckel (PDH) equation and the UNIversal QUAsi-Chemical (UNIQUAC) model to accurately describe the behavior of ionic liquids (ILs) in water. This study aims to develop a modern methodology that considers ILs as charged compounds and their dissociation extent, setting the groundwork for valuable tools in various fields of science and engineering.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Julian B. Beckmann, Daniel Rauber, Frederik Philippi, Kateryna Goloviznina, Jordan A. Ward-Williams, Andy J. Sederman, Mick D. Mantle, Agilio Padua, Christopher W. M. Kay, Tom Welton, Lynn F. Gladden
Summary: Understanding the relationship between the molecular structure and properties of ionic liquids is crucial for practical applications. By using fast-field cycling and molecular dynamics simulations, we can explore the dynamics of ionic liquids and gain insight into their molecular mechanics. The results demonstrate that the curling of side chains is essential for the properties of ether-functionalized ionic liquids.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Review
Materials Science, Multidisciplinary
Jocasta Avila, Ryan Clark, Agilio A. H. Padua, Margarida Costa Gomes
Summary: After reviewing the literature, it is concluded that type III porous liquids can either be suspensions of pristine MOFs in ionic liquids and liquid polymers, or decorated MOFs in molecular solvents. These porous liquids, specifically the porous ionic liquids, have unique properties and great potential for applications requiring solvents capable of dissolving large quantities of gases or small molecules.
MATERIALS ADVANCES
(2022)
Article
Chemistry, Multidisciplinary
Frederik Philippi, Daniel Rauber, Oriele Palumbo, Kateryna Goloviznina, Jesse McDaniel, David Pugh, Sophia Suarez, Carla C. Fraenza, Agilio Padua, Christopher W. M. Kay, Tom Welton
Summary: In this study, the combination of experimental and computational techniques is used to investigate the impact of fluorination, flexibility, and mass on the transport properties of ionic liquids. The results show that fluorination and flexibility significantly affect properties like viscosity, while the influence of mass is negligible. It is also found that conformational flexibility plays a crucial role in the success of fluorination as a design element.
Article
Chemistry, Multidisciplinary
Eduards Bakis, Kateryna Goloviznina, Ines C. M. Vaz, Diana Sloboda, Daniels Hazens, Valda Valkovska, Igors Klimenkovs, Agilio Padua, Margarida Costa Gomes
Summary: The branching of ionic liquid cation sidechains utilizing silicon as the backbone was investigated, leading to fluids with low density and viscosity. The anion size had the dominant effect on argon solubility, and the results provide design principles for targeted ionic liquids with optimized free volume.
Article
Chemistry, Multidisciplinary
Diego O. Hartmann, Karina Shimizu, Maika Rothkegel, Marija Petkovic, Ricardo Ferraz, Zeljko Petrovski, Luis C. Branco, Jose N. Canongia Lopes, Cristina Silva Pereira
Summary: The study evaluated the biological activity of novel ionic liquid formulations of amphotericin B, where two formulations were found to increase the antifungal activity of the drug while maintaining its mode of action. Higher biological activity was attributed to increased interaction of the ionic liquid with the fungal membrane ergosterol.
