Are NaTFSI and NaFSI Salt-Based Water-in-Salt Electrolytes Structurally Similar or Different?

Water-in-salt electrolytes (WiSEs) are a promising class of electrolytes due to their wide electrochemical stability window and nonflammability. In this study, we explore the structural organization of sodium bis(trifluoromethylsulfonyl)imide (NaTFSI) and sodium bis(fluorosulfonyl)imide (NaFSI) salt-based aqueous electrolytes, covering dilute to highly concentrated regions, by employing an all-atom molecular dynamics simulation. For the NaTFSI-based electrolyte, we observe that Na ions are mostly surrounded by water molecules at all the salt concentrations due to the very strong interaction between them.

Stability of Cytoplasmic Membrane of Bacteria in Aqueous and Ethanolic Environment.

The mechanism of action of any antibacterial agent or disinfectant depends largely on their interaction with the bacterial membrane. Herein, we use the SPICA (surface property fitting coarse graining) force-field and develop a coarse-grained (CG) model for the structure of the cytoplasmic membrane of () and its interaction with water and ethanol. We elucidate the impact of different concentrations of ethanol on the cytoplasmic membrane bilayers and vesicles of using the CG molecular dynamics (CG MD) simulations.

Mechanism of hydrophobic gating in the acetylcholine receptor channel pore.

Neuromuscular acetylcholine receptors (AChRs) are hetero-pentameric, ligand-gated ion channels. The binding of the neurotransmitter acetylcholine (ACh) to two target sites promotes a global conformational change of the receptor that opens the channel and allows ion conduction through the channel pore. Here, by measuring free-energy changes from single-channel current recordings and using molecular dynamics simulations, we elucidate how a constricted hydrophobic region acts as a "gate" to regulate the channel opening in the pore of AChRs.

Solvation Shell Anatomy of HS and CO Dissolved in Reline and Ethaline Deep Eutectic Solvents.

Rising atmospheric concentrations of anthropogenic hydrogen sulfide (HS) and carbon monoxide (CO) as a result of industrialization have encouraged researchers to explore innovative technologies for capturing these gases. Deep eutectic solvents (DESs) are an alternative media for mitigating HS and CO emissions. Herein, we have employed ab initio molecular dynamics simulations to investigate the structures of the nearest-neighbor solvation shells surrounding HS and CO when they are dissolved in reline and ethaline DESs.

Origin of structural and dynamic heterogeneity in thymol and coumarin-based hydrophobic deep eutectic solvents as revealed by molecular dynamics.

Hydrophobic deep eutectic solvents (HDESs) have recently emerged as a class of water-immiscible solvents with greener starting materials and inherent hydrophobic character, opening the gates to various new promising applications. Herein, we have carried out all-atom molecular dynamics simulations to comprehend the bulk phase structural organization and dynamic behavior of thymol and coumarin-based HDESs at two molar ratios of the constituent components. The simulated X-ray and neutron scattering structure functions (()s) indicate a prepeak signifying that these HDESs possess nanoscale heterogeneity or intermediate range ordering.

Wrapping-Trapping versus Extraction Mechanism of Bactericidal Activity of MoS Nanosheets against Bacterial Membrane.

The promising broad-spectrum antibacterial activity of two-dimensional molybdenum disulfide (2D MoS) has been widely recognized in the past decade. However, a comprehensive understanding of how the antibacterial pathways opted by the MoS nanosheets varies with change in lipid compositions of different bacterial strains is imperative to harness their full antibacterial potential and remains unexplored thus far. Herein, we present an atomistic molecular dynamics (MD) study to investigate the distinct modes of antibacterial action of MoS nanosheets against () under varying conditions.

Microstructures of Choline Amino Acid based Biocompatible Ionic Liquids.

Bio-compatible ionic liquids (Bio-ILs) represent a class of solvents with peculiar properties and exhibit huge potential for their applications in different fields of chemistry. Ever since they were discovered, researchers have used bio-ILs in diverse fields such as biomass dissolution, CO sequestration, and biodegradation of pesticides. This review highlights the ongoing research studies focused on elucidating the microscopic structure of bio-ILs based on cholinium cation ([Ch] ) and amino acid ([AA] ) anions using the state-of-the-art and classical molecular dynamics (MD) simulations.

How NaFTA salt affects the structural landscape and transport properties of PyrrFTA ionic liquid.

Recently, it has been demonstrated that ionic liquids (ILs) with an asymmetric anion render a wider operational temperature range and can be used as a solvent in sodium ion batteries. In the present study, we examine the microscopic structure and dynamics of pure 1-methyl-1-propylpyrrolidinium fluorosulfonyl(trifluoromethylsulfonyl)amide (PyrrFTA) IL using atomistic molecular dynamics simulations. How the addition of the sodium salt (NaFTA) having the same anion changes the structural landscape and transport properties of the pure IL has also been explored.

Solvation Shell Structures of Ammonia in Reline and Ethaline Deep Eutectic Solvents.

Because of increasing atmospheric anthropogenic ammonia (NH) emission, researchers are devising new techniques to capture NH. Deep eutectic solvents (DESs) are found as potential media for NH mitigation. In the present study, we have carried out molecular dynamics (AIMD) simulations to decipher the solvation shell structures of an ammonia solute in reline (1:2 mixture of choline chloride and urea) and ethaline (1:2 mixture of choline chloride and ethylene glycol) DESs.

MoS nanosheet induced destructive alterations in the bacterial membrane.

Two dimensional molybdenum disulfide (MoS) nanosheets have recently gained wide recognition for their efficient broad-spectrum antibacterial activity complemented with great biocompatibility and minimal bacterial resistance inducing capabilities. However, despite the numerous investigations, the molecular level interactions at the nano-bio interface responsible for their bactericidal activity remain obscure. Herein, through an atomistic molecular dynamics study, we attempt to seek an in-depth understanding of the atomic level details of the underlying mechanism of their antibacterial action against the () bacterial membrane.

Solvent Organization around Methane Dissolved in Archetypal Reline and Ethaline Deep Eutectic Solvents as Revealed by AIMD Investigation.

Because of the rising concentration of harmful greenhouse gases like methane in the atmosphere, researchers are striving for developing novel techniques for capturing these gases. Recently, neoteric liquids such as deep eutectic solvents (DESs) have emerged as an efficient means of sequestration of methane. Herein, we have performed molecular dynamics (AIMD) simulations to elucidate the solvation structure around a methane molecule dissolved in reline and ethaline DESs.

Heterogeneity and Nanostructure of Superconcentrated LiTFSI-EmimTFSI Hybrid Aqueous Electrolytes: Beyond the 21 m Limit of Water-in-Salt Electrolyte.

Ionic liquids such as EmimTFSI (1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide) have been found to improve the solubility of LiTFSI salt in water-in-salt electrolyte (WiSE) from 21 to 60 m. However, the molecular origin of such enhancement in the solubility is still unknown. In the present work, we elucidate the microscopic structures of LiTFSI-EmimTFSI-based hybrid aqueous electrolytes and compare them with the structure of LiTFSI-based WiSE using molecular dynamics simulations.

Anionic Lipid Clustering-Mediated Bactericidal Activity and Selective Toxicity of Quaternary Ammonium-Substituted Polycationic Pullulan against the Bacterial Membrane.

Non-amphiphilic polycations have recently been recognized to hold excellent antimicrobial potential with great mammalian cell compatibility. In a recent study, the excellent broad-spectrum bactericidal efficacy of a quaternary ammonium-substituted cationic pullulan (CP4) was demonstrated. Their selective toxicity and nominal probability to induce the acquisition of resistance among pathogens fulfill the fundamental requirements of new-generation antibacterials.

An Overview of Structure and Dynamics Associated with Hydrophobic Deep Eutectic Solvents and Their Applications in Extraction Processes.

Recent development of novel water-immiscible green solvents known as hydrophobic deep eutectic solvents (HDESs) has opened the gates for applications requiring media where the presence of water is undesirable. Ever since they were prepared, researchers have used HDESs in diverse fields such as extraction processes, CO sequestration, membrane formation, and catalysis. The structure and dynamics associated with the species comprising HDESs guide their suitability for specific applications.

Structural adaptations in the bovine serum albumin protein in archetypal deep eutectic solvent reline and its aqueous mixtures.

The global concern over the environmental impact and challenges associated with the use of conventional solvents in biotransformation processes have pushed the search for alternative solvents. Recently, deep eutectic solvents (DESs) have appeared as a promising replacement with better biocompatibility and have been postulated to hold great potential in protein engineering and crystallization processes. In this context, herein, we have investigated the effect of reline (a choline chloride : urea mixture in 1 : 2 proportion) DES in its pure and hydrated forms on the structural stability and conformation of the bovine serum albumin (BSA) protein using all-atom molecular dynamics simulations.

Deciphering Ethanol-Driven Swelling, Rupturing, Aggregation, and Fusion of Lipid Vesicles Using Coarse-Grained Molecular Dynamics Simulations.

Traditionally, liquid ethanol is known to enhance the permeability of lipid membranes and causes vesicle aggregation and fusion. However, how the amphiphilic ethanol molecules perturb the lipid vesicles to facilitate their aggregation or fusion has not been addressed at any level of molecular simulations. Herein, not only have we developed a coarse-grained (CG) model for liquid ethanol, its aqueous mixture, and hydrated lipid membranes for molecular dynamics (MD) simulations, but also utilized it to delineate the aggregation and fusion of lipid vesicles using CG-MD simulations with multimillion particles.

Quaternary ammonium substituted pullulan accelerates wound healing and disinfects infected wounds in mouse through an atypical 'non-pore forming' pathway of bacterial membrane disruption.

The emergence of multi-drug resistant pathogens has fueled the search for alternatives to the existing line of antibiotics that can eradicate pathogens without inducing resistance development. Here, we report the accelerated wound healing and disinfection potential of a non-amphiphilic quaternized fungal exopolysaccharide, pullulan, without resistance generation in pathogens. The quaternary ammonium substituted pullulan (CP) derivatives showed excellent bactericidal activity against both Gram negative (MBC = 1.

Mechanistic Insight on BioIL-Induced Structural Alterations in DMPC Lipid Bilayer.

The emerging application risks of traditional ionic liquids (ILs) toward the ecosystem have changed the perception regarding their greenness. This resulted in the exploration of their more biocompatible alternatives known as biocompatible ILs (BioILs). Here, we have investigated the impact of two such biocompatible cholinium amino acid-based ILs on the structural behavior of model homogeneous DMPC (1,2-dimyristoyl--glycero-3-phosphocholine) lipid bilayer using all-atom molecular dynamics simulation technique.

Multiple evidences of dynamic heterogeneity in hydrophobic deep eutectic solvents.

Hydrophobic deep eutectic solvents (HDESs) have gained immense popularity because of their promising applications in extraction processes. Herein, we employ atomistic molecular dynamics simulations to unveil the dynamics of DL-menthol (DLM) based HDESs with hexanoic (C6), octanoic (C8), and decanoic (C10) acids as hydrogen bond donors. The particular focus is on understanding the nature of dynamics with changing acid tail length.

Structure of cholinium glycinate biocompatible ionic liquid at graphite electrode interface.

We use constant potential molecular dynamics simulations to investigate the interfacial structure of the cholinium glycinate biocompatible ionic liquid (bio-IL) sandwiched between graphite electrodes with varying potential differences. Through number density profiles, we observe that the cation and anion densities oscillate up to ∼1.5 nm from the nearest electrode.

First-principles based theoretical investigation of impact of polyolefin structure on photooxidation behavior.

Despite their mass production and large applications, polyolefins' stability and durability toward the air, moisture, and weather resistance is a challenge for the ecosystem. After long-term exposure to ultraviolet (UV) radiation or high-temperature or erosion, polyolefins undergo degradation generating microplastics (MPs). The MPs generated after the degradation of these polyolefins are hazardous for the ecosystem.

Unique and generic structural features of cholinium amino acid-based biocompatible ionic liquids.

Cholinium amino acid-based (Ch-AA) biocompatible ionic liquids (bio-ILs) are synthesized from renewable components and are efficiently used for biomass processing. However, their microscopic structural features that lead to their application as biomass solvents remain undetermined. Herein, we use atomistic simulations to investigate the structures of six different Ch-AA bio-ILs up to the nanometer length scale and demonstrate that, depending on the anion side chain structure, the respective IL exhibits structural ordering at different length scales.

Design and synthesis of β-carboline and combretastatin derivatives as anti-neutrophilic inflammatory agents.

A series of β-carboline derivatives was synthesized by the Pictet-Spengler reaction with or without the combretastatin skeleton. The structures of these derivatives were elucidated by spectroscopic techniques. All synthesized compounds were evaluated for their anti-inflammatory activity in human neutrophils.

Intercalation-deintercalation of water-in-salt electrolytes in nanoscale hydrophobic confinement.

Intercalation-deintercalation of water-in-salt (WIS) electrolytes in nanoscale confinement is an important phenomenon relevant to energy storage and self-assembly applications. In this article, we use molecular simulations to investigate the effects of intersurface separation on the structure and free energy underlying the intercalation-deintercalation of the Li bis(trifluoromethane)sulfonimide ([Li][TFSI]) water-in-salt (WIS) electrolyte confined between nanoscale hydrophobic surfaces. We employ enhanced sampling to estimate the free energy profiles for the intercalation behaviour of WIS in confining sheets at several intersurface separations.

Distinct Solvation Structures of CO and SO in Reline and Ethaline Deep Eutectic Solvents Revealed by AIMD Simulations.

Deep eutectic solvents (DESs) are emerging as an alternative media for the sequestration of greenhouse gases such as CO and SO. Herein, we performed ab initio molecular dynamics (AIMD) simulations to elucidate the solvation structure around CO and SO in choline chloride-based DESs, namely, reline and ethaline. We show that in all four systems the structures of the nearest neighbor shells around these molecules are distinct.