Atomistic Insight into Orthoborate-Based Ionic Liquids: Force Field Development and Evaluation

Wang, Yong‐Lei; Shah, Faiz Ullah; Glavatskih, Sergei; Antzutkin, Oleg N.; Laaksonen, Aatto

doi:10.1021/jp503029d

Cited by 62 publications

(115 citation statements)

References 80 publications

(158 reference statements)

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“…38,57 A set of force field parameters developed for tetraalkylphosphonium cations in our previous work 57 is directly adopted in the present study without further modification. The non-covalent interactions are described in the last term, including van der Waals (vdW) and Coulombic interactions of atom-centered point charges.…”

Section: B Atomistic Ionic Modelsmentioning

confidence: 99%

“…37,38,57 In the present work, all SDFs are visualized using the gOpenMol package. 37,38,57 In the present work, all SDFs are visualized using the gOpenMol package.…”

Section: B Microscopic Structuresmentioning

confidence: 99%

“…As expected, Cl anions coordinate with [P 6,6,6,14 ] cations in a tetrahedral region due to strong electrostatic interactions and distinct steric effects of four alkyl substituents in [P 6,6,6,14 ] cations. 57,58 It was suggested in previous studies that different anionic groups preferentially interact with the HP atoms in [P 6,6,6,14 ] cations due to their expected hydrogen bonded interactions. 5.…”

Section: B Microscopic Structuresmentioning

confidence: 99%

“…First-principles quantum mechanics (QM) calculations can provide accurate microstructural information without any experimental support. 37,[55][56][57] These force fields, to some extent, can qualitatively predict physicochemical and structural properties of model ILs compared with experimental data. 44,[52][53][54] Molecular simulations at an atomistic level are widely used in predicting thermodynamic, structural, and dynamic properties of various IL systems.…”

Section: Introductionmentioning

confidence: 99%

“…35,[44][45][46][47][48][49][50] However, due to their computationally demanding nature, these methods are usually adopted to derive effective interactions of ion pairs, 35,46,50,51 and to determine delicate interactions with solute molecules in small systems and short time scales. In our previous work, a high-quality atomistic force field was developed for ILs consisting of the tetraalkylphosphonium cations and the chelated orthoborate anions, 57 and validated against the available experimental measurements. The quality of atomistic simulation predictions mainly depends on the reliability of the adopted force fields, which refer to the inter-and intramolecular potential parameters used to mimic interactions between atoms in model systems.…”

Section: Introductionmentioning

confidence: 99%

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Multiscale modeling of the trihexyltetradecylphosphonium chloride ionic liquid

Wang

Sarman

et al. 2015

Phys. Chem. Chem. Phys.

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A multiscale modeling protocol was sketched for the trihexyltetradecylphosphonium chloride ([P6,6,6,14]Cl) ionic liquid (IL). The optimized molecular geometries of an isolated [P6,6,6,14] cation and a tightly bound [P6,6,6,14]Cl ion pair structure were obtained from quantum chemistry ab initio calculations. A cost-effective united-atom model was proposed for the [P6,6,6,14] cation based on the corresponding atomistic model. Atomistic and coarse-grained molecular dynamics simulations were performed over a wide temperature range to validate the proposed united-atom [P6,6,6,14] model against the available experimental data. Through a systemic analysis of volumetric quantities, microscopic structures, and transport properties of the bulk [P6,6,6,14]Cl IL under varied thermodynamic conditions, it was identified that the proposed united-atom [P6,6,6,14] cationic model could essentially capture the local intermolecular structures and the nonlocal experimental thermodynamics, including liquid density, volume expansivity and isothermal compressibility, and transport properties, such as zero-shear viscosity, of the bulk [P6,6,6,14]Cl IL within a wide temperature range.

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Section: B Atomistic Ionic Modelsmentioning

confidence: 99%

“…37,38,57 In the present work, all SDFs are visualized using the gOpenMol package. 37,38,57 In the present work, all SDFs are visualized using the gOpenMol package.…”

Section: B Microscopic Structuresmentioning

confidence: 99%

Section: B Microscopic Structuresmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Multiscale modeling of the trihexyltetradecylphosphonium chloride ionic liquid

Wang

Sarman

et al. 2015

Phys. Chem. Chem. Phys.

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A Halogen‐Free and Flame‐Retardant Sodium Electrolyte Compatible with Hard Carbon Anodes

Colbin

Mogensen

Buckel

et al. 2021

Adv Materials Inter

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For sodium‐ion batteries, two pressing issues concerning electrolytes are flammability and compatibility with hard carbon anode materials. Non‐flammable electrolytes that are sufficiently stable against hard carbon have—to the authors’ knowledge—previously only been obtained by either the use of high salt concentrations or additives. Herein, the authors present a simple, fluorine‐free, and flame‐retardant electrolyte which is compatible with hard carbon: 0.38 m sodium bis(oxalato)borate (NaBOB) in triethyl phosphate (TEP). A variety of techniques are employed to characterize the physical properties of the electrolyte, and to evaluate the electrochemical performance in full‐cell sodium‐ion batteries. The results reveal that the conductivity is sufficient for battery operation, no significant self‐discharge occurs, and a satisfactory passivation is enabled by the electrolyte. In fact, a mean discharge capacity of 107 ± 4 mAh g−1 is achieved at the 1005th cycle, using Prussian white cathodes and hard carbon anodes. Hence, the studied electrolyte is a promising candidate for use in sodium‐ion batteries.

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The Effect of Phenyl Substitutions on Microstructures and Dynamics of Tetraalkylphosphonium Bis(trifluoro‐ methylsulfonyl)imide Ionic Liquids

Wang

Laaksonen

et al. 2020

ChemPhysChem

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Extensive atomistic simulations demonstrated that a gradual substitution of hexyl chains with phenyl groups in tetraalkylphosphonium cations results in remarkable changes in hydrogen bonding interactions, liquid structures and scattering structural functions, and rotational dynamics of hexyl chains and phenyl groups in tetraalkylphosphonium bis(trifluoromethylsulfonyl)imide ionic liquids. Hydrogen donor sites in hexyl chains present competitive characteristics with those in phenyl groups in coordinating anions, as well as their continuous and intermittent hydrogen bonding dynamics. Cation‐cation and anion‐anion spatial correlations show concomitant shift to short distances with decreased peak intensities with variations of cation structures, whereas cation‐anion correlations have a distinct shift to large radial distances due to decreased associations of anions with neighboring cations. These microstructural changes are qualitatively manifested in shifts of prominent peaks for prevalent charge alternations and adjacency correlations between ion species in scattering structural functions. Meanwhile, rotational dynamics of hexyl chains speed up, which, in turn, slow down rotations of phenyl groups, whereas anions exhibit imperceptible changes in their rotational dynamics. These computational results are intrinsically correlated with conformational flexibilities, molecular sizes, and steric hindrance effects of phenyl groups in comparison with hexyl chains, and constrained distributions of anions around cations in heterogeneous ionic environments.

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Atomistic Insight into Orthoborate-Based Ionic Liquids: Force Field Development and Evaluation

Cited by 62 publications

References 80 publications

Multiscale modeling of the trihexyltetradecylphosphonium chloride ionic liquid

Multiscale modeling of the trihexyltetradecylphosphonium chloride ionic liquid

A Halogen‐Free and Flame‐Retardant Sodium Electrolyte Compatible with Hard Carbon Anodes

The Effect of Phenyl Substitutions on Microstructures and Dynamics of Tetraalkylphosphonium Bis(trifluoro‐ methylsulfonyl)imide Ionic Liquids

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