https://hdl.handle.net/10259/4330 2026-09-09T11:34:43Z https://hdl.handle.net/10259/12052 Molecular dynamics study on the interfacial properties of mixtures of monomers of polyvinylpyrrolidone (PVP)-based battery binders on graphene and graphite surfaces Gutiérrez Vega, Alberto; Aparicio Martínez, Santiago; Pekarovicova, Alexandra; Wu, Qingliu; Atilhan, Mert This study investigates the behavior of two different mixtures of monomers of polyvinylpyrrolidone (PVP)-based battery binders, polyvinylpyrrolidone:polyvinylidene difluoride (PVP:PVDF) and polyvinylpyrrolidone:polyacrylic acid (PVP:PAA), at graphene and graphite interfaces using classical molecular dynamics simulations. The aim is to identify the best performing monomer binder blend and carbon-based material for the design of battery-optimized energy devices. The PVP:PAA monomer binder blend and graphite are found to have the best interaction energies, densification upon adsorption, and more ordered structure. The adsorption of both monomer binder blends is strongly guided by the higher affinity of PVP and PAA monomeric molecules for the surfaces compared to PVDF. The structure of adsorbed layers of PVP:PVDF monomer binder blend on graphene and graphite develops more quickly than PVP:PAA, indicating faster kinetics. This study complements a previous density functional theory study recently reported by our group and contributes to a better understanding of the nanoscopic features of relevant interfacial regions involving mixtures of monomers of PVP-based battery binders and different carbon-based materials. The effect of a blend of commonly used monomer binders on carbon-based materials is essential for obtaining tightly bound anode and cathode active materials in lithium-ion batteries, which is crucial for designing battery-optimized energy devices. 2023-07-01T00:00:00Z https://hdl.handle.net/10259/12039 Insights on the adsorption mechanism of different polyvinylpyrrolidone (PVP)-based battery binders on 2D-materials for LiPF6-Ec-Emc electrolyte via molecular simulations Wu, Qingliu; Pekarovicova, Alexandra; Aparicio Martínez, Santiago; Gutiérrez Vega, Alberto; Atilhan, Mert In this study, the adsorption mechanism of different mixtures of monomers of polyvinylpyrrolidone (PVP)-based battery binders (polyvinylpyrrolidone:polyvinylidene difluoride, PVP:PVDF; polyvinylpyrrolidone:polyacrylic acid, PVP:PAA; and polyvinylpyrrolidone:lithiated polyacrylic acid, PVP:Li-PAA) on a graphene oxide (GO) nanoparticle was investigated using density functional theory (DFT), quantum theory of atoms in molecules (QTAIM) and molecular dynamics (MD) simulations in order to identify the thermodynamic, intermolecular forces and interfacial properties of these systems within the framework of battery applications employing LiPF6-EC-EMC electrolyte. Our work focuses into the short-range interactions and electronic properties of the adsorbed binder mixtures on the GO nanoparticle, and also into their interfacial properties (considering systems with and without the electrolyte, 1.2 M LiPF6 dissolved in EC/EMC 3/7, w/w), shedding light on the fundamental interactions that govern the mechanisms of GO (and also another 2D-nanomaterial such as graphite, for reference) enabling the physical adsorption of binders (and electrolyte compounds) for obtaining strongly adhered anode and cathode active substances in Li-ion battery applications. The results of this study advance the understanding of the adsorption mechanisms of binder mixtures and electrolyte compounds on carbon-based nanomaterials, and hold significant promise for the designing battery-optimized energy devices in lithium-ion batteries. 2024-11-01T00:00:00Z https://hdl.handle.net/10259/12030 Insights into Carvone: Fatty Acid Hydrophobic NADES for Alkane Solubilization Aguilar Cuesta, Nuria; Benito, Cristina; Martel Martín, Sonia; Gutiérrez Vega, Alberto; Rozas Azcona, Sara; Marcos Villa, Pedro A.; Bol Arreba, Alfredo; Atilhan, Mert; Aparicio Martínez, Santiago The urge to adopt cleaner technologies drives the search for novel and sustainable materials such as Hydrophobic Natural Deep Eutectic Solvents (HNADESs), a new class of green solvents characterized by their low toxicity, biodegradability, and tunable properties, aiming to be applied in various fields for handling non-polar substances. In this work, the solubilization of hydrocarbons in type V HNADESs (non-ionic organic molecules) formed by mixing carvone, a natural monoterpenoid, with organic acids (hexanoic to decanoic acids) is examined by applying both experimental and theoretical approaches. The synthesis and physicochemical characterization of different HNADESs allowed us to tailor their properties, aiming for optimal interactions with desired hydrocarbons. The solubilization of hydrocarbons in CAR:C10AC (1:1) HNADES is evaluated in terms of HNADES content, temperature, and the structure of the hydrocarbon itself (C6, C10, and C14 being the selected ones). To gain deeper insights into the underlying mechanisms of interactions between the solvents and the alkanes, a comprehensive multiscale computational study was carried out to analyze the nature of the interactions, the changes upon formation of HNADESs and hydrocarbon solubilization in the fluid’s nanostructure, and the possible toxicological effects of the solvents. The findings hold the potential to significantly impact the realm of hydrocarbon exploration and utilization. 2024-12-01T00:00:00Z https://hdl.handle.net/10259/12028 Synergistic Density Functional Theory and Molecular Dynamics Approach to Elucidate PNIPAM–Water Interaction Mechanisms Alomari, Noor; Aparicio Martínez, Santiago; Meyer, Paul; Zeng, Yi; Cui, Shuang; Gutiérrez Vega, Alberto; Atilhan, Mert This study employs Density Functional Theory (DFT) and Molecular Dynamics (MD) simulations to investigate interactions between water molecules and Poly(N-isopropylacrylamide) (PNIPAM). DFT reveals preferential water binding sites, with enhanced binding energy observed in the linker zone. Quantum Theory of Atoms in Molecules (QTAIM) and electron localization function (ELF) analyses highlight the roles of hydrogen bonding and steric hindrance. MD simulations unveil temperature-dependent hydration dynamics, with structural transitions marked by changes in the radius of gyration (Rg) and the radial distribution function (RDF), aligning with DFT findings. Our work goes beyond prior studies by combining a DFT, QTAIM and MD simulations approach across different PNIPAM monomer-to-30mer structures. It introduces a systematic quantification of pseudo-saturation thresholds and explores water clustering dynamics with structural specificity, which have not been previously reported in the literature. These novel insights establish a more complete molecular-level picture of PNIPAM hydration behavior and temperature responsiveness, emphasizing the importance of amide hydrogen and carbonyl oxygen sites in hydrogen bonding, which weakens above the lower critical solution temperature (LCST), resulting in increased hydrophobicity and paving the way for understanding water sorption mechanisms, offering guidance for future applications such as dehumidification and atmospheric water harvesting. 2025-05-01T00:00:00Z