Collectivity in ionic liquids: a temperature dependent, polarizable molecular dynamics study

Szabadi, András; Honegger, Philipp; Schöfbeck, Flora; Sappl, Marion; Heid, Esther; Steinhauser, Othmar; Schröder, Christian

doi:10.1039/d2cp00898j

Cited by 6 publications

(5 citation statements)

References 115 publications

(183 reference statements)

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“…Difference in Potential of mean force (PMF) for s = 0.25 between this work and Joerg and Schröder (2022).…”

Section: Figure 10mentioning

confidence: 59%

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Protex—A Python utility for proton exchange in molecular dynamics simulations

Joerg

Wieder²,

Schröder³

2023

Front. Chem.

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Protex is an open-source program that enables proton exchanges of solvent molecules during molecular dynamics simulations. While conventional molecular dynamics simulations do not allow for bond breaking or formation, protex offers an easy-to-use interface to augment these simulations and define multiple proton sites for (de-)protonation using a single topology approach with two different λ-states. Protex was successfully applied to a protic ionic liquid system, where each molecule is prone to (de-)protonation. Transport properties were calculated and compared to experimental values and simulations without proton exchange.

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“…Difference in Potential of mean force (PMF) for s = 0.25 between this work and Joerg and Schröder (2022).…”

Section: Figure 10mentioning

confidence: 59%

“…The second step involves proton transfers with a particular probability. The initial probability of Table 4 are in accordance with Jacobi et al (2022) but are updated applying Eq. 4.…”

Section: Computational Setupmentioning

confidence: 99%

Protex—A Python utility for proton exchange in molecular dynamics simulations

Joerg

Wieder²,

Schröder³

2023

Front. Chem.

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“…Nevertheless, the diffusion also profits significantly from the increased number of transfers due to the larger pxr . Exchanging a proton, an ion pair becomes two neutral species, which does not increase the mobility of charge carriers per se but destroys ion cages. , Weaker ion cages enhance the mobility of individual ions. However, the newborn neutral 1-methylimidazole is still covered by several anions of the former ion cage, which puts it in an unfavorable position .…”

Section: Resultsmentioning

confidence: 99%

Updates to Protex for Simulating Proton Transfers in an Ionic Liquid

Gődény,

Joerg,

Kovar

et al. 2024

J. Phys. Chem. B

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The Python-based program Protex was initially developed for simulating proton transfers in a pure protic ionic liquid via polarizable molecular dynamics simulations. This method employs a single topology approach wherein deprotonated species retain a dummy atom, which is transformed into a real hydrogen atom during the protonation process. In this work, we extended Protex to include more intricate systems and to facilitate the simulation of the Grotthuss mechanism to enhance alignment with the empirical findings. The handling of proton transfer events within Protex was further refined for increased flexibility. In the original model, each deprotonated molecule contained a single dummy atom connected to the hydrogen acceptor atom. This model posed limitations for molecules with multiple atoms that could undergo protonation. To mitigate this issue, Protex was extended to execute a proton transfer when one of these potential atoms was within a suitable proximity for the transfer event. For the purpose of maintaining simplicity, Protex continues to utilize only a single dummy atom per deprotonated molecule. Another new feature pertains to the determination of the eligibility for a proton transfer event. A range of acceptable distances can now be defined within which the transfer probability is gradually turned off. These modifications allow for a more nuanced approach to simulating proton transfer events, offering greater accuracy and control of the modeling process.

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“…This might be rather strong in ionic liquids as cage structures are formed. 52,65 The ion cages may also influence the permanent molecular dipoles and their fluctuations. Furthermore, hydrogen bonds to the carboxylic group of acetate, for example, significantly change the C–O stretching modes.…”

Section: Resultsmentioning

confidence: 99%

“…We focus in this work on the ionic liquids 1-ethyl-3-methyl-imidazolium acetate [C 2 mim]OAc, 1-ethyl-3-methyl-imidazolium triflate [C 2 mim]OTf, 1-ethyl-3-methyl-imidazolium dicyanamide [C 2 mim]N(CN) 2 , and 1-butyl-3-methyl-imidazolium tetrafluoroborate [C 4 mim]BF 4 . Initial FF parameters for C 2 mim + , N(CN) 2 − , and OTf − were taken from ref. 52, for C 4 mim + and BF 4 − from ref.…”

Section: Methodsmentioning

confidence: 99%