Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions

doi:https://doi.org/10.1080/08927022.2018.1557328

Title: Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions

Abstract

We investigate the effects of both triethylene glycol (TEG) and polyethylene glycol (PEG) on the structure and transport of an excess proton (H ⁺) in aqueous solution. A new reactive force field (ReaxFF) parameterisation is carried out to better describe proton transfer of H ⁺ with PEG polymers in aqueous solution via training against density functional theory (DFT) calculations. Using this ReaxFF parameterisation, reactive molecular dynamics simulations are carried out for three different systems containing H ⁺: bulk water, aqueous TEG, and aqueous PEG with a single, oriented polymer chain. The H ⁺ diffusivity is suppressed due to the presence of TEG and enhanced in the oriented chain PEG system, particularly along the axis parallel to the PEG chain, relative to bulk water. The enhancement in proton mobility along the chain axis is mainly due to the structural, rather than vehicular, component. From free energy calculations for H ⁺ transfer, the increase in proton mobility is not due to a reduction in activation energy. Finally, from pair distribution function analysis of the local structure for water and hydronium we hypothesise the increased mobility is due to an entropic effect, specifically a favourable hydrogen bond network for long range proton transportmore » due to the oriented PEG chain.« less

Authors:

^[1];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering

Publication Date:: 2018-08-26

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1546535

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Molecular Simulation

Additional Journal Information:: Journal Volume: 45; Journal Issue: 4-5; Journal ID: ISSN 0892-7022

Publisher:: Taylor & Francis

Country of Publication:: United States

Language:: English

Subject:: 73 NUCLEAR PHYSICS AND RADIATION PHYSICS; 36 MATERIALS SCIENCE; proton transport; polyethylene glycol; water; ReaxFF

Citation Formats


                    McDonnell, Marshall T., and Keffer, David J. Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions.  United States: N. p., 2018. 
        Web.  doi:10.1080/08927022.2018.1557328.

Copy to clipboard


                    McDonnell, Marshall T., & Keffer, David J. Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions.  United States.  https://doi.org/10.1080/08927022.2018.1557328

Copy to clipboard


                    McDonnell, Marshall T., and Keffer, David J. Sun .  
        "Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions".  United States.  https://doi.org/10.1080/08927022.2018.1557328.  https://www.osti.gov/servlets/purl/1546535.

Copy to clipboard


                    
@article{osti_1546535,

  title        = {Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions},

  author       = {McDonnell, Marshall T. and Keffer, David J.},

  abstractNote = {We investigate the effects of both triethylene glycol (TEG) and polyethylene glycol (PEG) on the structure and transport of an excess proton (H+) in aqueous solution. A new reactive force field (ReaxFF) parameterisation is carried out to better describe proton transfer of H+ with PEG polymers in aqueous solution via training against density functional theory (DFT) calculations. Using this ReaxFF parameterisation, reactive molecular dynamics simulations are carried out for three different systems containing H+: bulk water, aqueous TEG, and aqueous PEG with a single, oriented polymer chain. The H+ diffusivity is suppressed due to the presence of TEG and enhanced in the oriented chain PEG system, particularly along the axis parallel to the PEG chain, relative to bulk water. The enhancement in proton mobility along the chain axis is mainly due to the structural, rather than vehicular, component. From free energy calculations for H+ transfer, the increase in proton mobility is not due to a reduction in activation energy. Finally, from pair distribution function analysis of the local structure for water and hydronium we hypothesise the increased mobility is due to an entropic effect, specifically a favourable hydrogen bond network for long range proton transport due to the oriented PEG chain.},

  doi          = {10.1080/08927022.2018.1557328},

  url          = {https://www.osti.gov/biblio/1546535},
  journal      = {Molecular Simulation},

  issn         = {0892-7022},

  number       = 4-5,

  volume       = 45,

  place        = {United States},

  year         = {2018},

  month        = {8}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1080/08927022.2018.1557328

Other availability

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Effect of pegylation on pharmaceuticals
journal, March 2003

Harris, J. Milton; Chess, Robert B.
Nature Reviews Drug Discovery, Vol. 2, Issue 3
https://doi.org/10.1038/nrd1033

PEGylation, successful approach to drug delivery
journal, November 2005

Veronese, Francesco M.; Pasut, Gianfranco
Drug Discovery Today, Vol. 10, Issue 21, p. 1451-1458
https://doi.org/10.1016/S1359-6446(05)03575-0

PEG — A versatile conjugating ligand for drugs and drug delivery systems
journal, October 2014

Kolate, Atul; Baradia, Dipesh; Patil, Sushilkumar
Journal of Controlled Release, Vol. 192
https://doi.org/10.1016/j.jconrel.2014.06.046

A sol–gel synthesis of polyether-based proton conducting electrolytes
journal, October 2003

Ritchie, Jason E.; Crisp, Jeffrey A.
Analytica Chimica Acta, Vol. 496, Issue 1-2
https://doi.org/10.1016/S0003-2670(03)00990-5

Effect of Polymer Structure on Ion Transport in an Anhydrous Proton Conducting Electrolyte
journal, February 2010

Ghosh, Braja D.; Ritchie, Jason E.
Chemistry of Materials, Vol. 22, Issue 4
https://doi.org/10.1021/cm902283r

Effects of Bulky Copolymers on Ion Transport in an Anhydrous Proton-Conducting Electrolyte
journal, January 2010

Sun, Chengjun; Ritchie, Jason E.
Journal of The Electrochemical Society, Vol. 157, Issue 11
https://doi.org/10.1149/1.3478569

Star-Shaped MePEG _n Polymers as H ⁺ Conducting Electrolytes
journal, July 2011

Sun, Chengjun; Ritchie, Jason E.
The Journal of Physical Chemistry B, Vol. 115, Issue 26
https://doi.org/10.1021/jp1112153

Polyethylene glycol-functionalized polyoctahedral silsesquioxanes as H+-conducting electrolytes
journal, February 2014

Sun, Chengjun; Ritchie, Jason E.
Journal of Solid State Electrochemistry, Vol. 18, Issue 6
https://doi.org/10.1007/s10008-014-2409-z

Volume Fraction of Ether Is a Significant Factor in Controlling Conductivity in Proton Conducting Polyether Based Polymer Sol–Gel Electrolytes
journal, October 2014

Yancey, Benjamin; Jones, Jonathan; Ritchie, Jason E.
The Journal of Physical Chemistry B, Vol. 118, Issue 45
https://doi.org/10.1021/jp5072082

High temperature proton exchange membranes with enhanced proton conductivities at low humidity and high temperature based on polymer blends and block copolymers of poly(1,3-cyclohexadiene) and poly(ethylene glycol)
journal, October 2015

Deng, Shawn; Hassan, Mohammad K.; Nalawade, Amol
Polymer, Vol. 77
https://doi.org/10.1016/j.polymer.2015.09.033

Structure and Diffusion in Cross-Linked and Sulfonated Poly(1,3-cyclohexadiene)/Polyethylene Glycol-Based Proton Exchange Membranes
journal, March 2013

Wang, Qifei; Keffer, David J.; Deng, Suxiang
The Journal of Physical Chemistry C, Vol. 117, Issue 10
https://doi.org/10.1021/jp309793z

Computational Design of Oligopeptide Containing Poly(ethylene glycol) Brushes for Stimuli-Responsive Drug Delivery
journal, October 2015

Stanzione, Francesca; Jayaraman, Arthi
The Journal of Physical Chemistry B, Vol. 119, Issue 42
https://doi.org/10.1021/acs.jpcb.5b06838

Stimuli-responsive nanocarriers for drug delivery
journal, October 2013

Mura, Simona; Nicolas, Julien; Couvreur, Patrick
Nature Materials, Vol. 12, Issue 11
https://doi.org/10.1038/nmat3776

The Grotthuss mechanism
journal, October 1995

Agmon, Noam
Chemical Physics Letters, Vol. 244, Issue 5-6
https://doi.org/10.1016/0009-2614(95)00905-J

Proton Transfer 200 Years after von Grotthuss: Insights from Ab Initio Simulations
journal, September 2006

Marx, Dominik
ChemPhysChem, Vol. 7, Issue 9
https://doi.org/10.1002/cphc.200600128

An analysis of hydrated proton diffusion in ab initio molecular dynamics
journal, January 2015

Tse, Ying-Lung Steve; Knight, Chris; Voth, Gregory A.
The Journal of Chemical Physics, Vol. 142, Issue 1
https://doi.org/10.1063/1.4905077

Proton mobility in aqueous systems: combining ab initio accuracy with millisecond timescales
journal, January 2017

Kabbe, Gabriel; Dreßler, Christian; Sebastiani, Daniel
Physical Chemistry Chemical Physics, Vol. 19, Issue 42
https://doi.org/10.1039/C7CP05632J

Protons and Hydroxide Ions in Aqueous Systems
journal, April 2016

Agmon, Noam; Bakker, Huib J.; Campen, R. Kramer
Chemical Reviews, Vol. 116, Issue 13
https://doi.org/10.1021/acs.chemrev.5b00736

Proton Transfer, Acid-Base Catalysis, and Enzymatic Hydrolysis. Part I: ELEMENTARY PROCESSES
journal, January 1964

Eigen, M.
Angewandte Chemie International Edition in English, Vol. 3, Issue 1
https://doi.org/10.1002/anie.196400011

Aqueous solutions: state of the art in ab initio molecular dynamics
journal, March 2014

Hassanali, Ali A.; Cuny, Jérôme; Verdolino, Vincenzo
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 372, Issue 2011
https://doi.org/10.1098/rsta.2012.0482

The Role of Quantum Effects on Structural and Electronic Fluctuations in Neat and Charged Water
journal, November 2014

Giberti, Federico; Hassanali, Ali A.; Ceriotti, Michele
The Journal of Physical Chemistry B, Vol. 118, Issue 46
https://doi.org/10.1021/jp507752e

Role of Presolvation and Anharmonicity in Aqueous Phase Hydrated Proton Solvation and Transport
journal, November 2015

Biswas, Rajib; Tse, Ying-Lung Steve; Tokmakoff, Andrei
The Journal of Physical Chemistry B, Vol. 120, Issue 8
https://doi.org/10.1021/acs.jpcb.5b09466

Ultrafast Vibrational and Structural Dynamics of the Proton in Liquid Water
journal, April 2006

Woutersen, Sander; Bakker, Huib J.
Physical Review Letters, Vol. 96, Issue 13
https://doi.org/10.1103/PhysRevLett.96.138305

Ultrafast 2D IR spectroscopy of the excess proton in liquid water
journal, October 2015

Thämer, Martin; De Marco, Luigi; Ramasesha, Krupa
Science, Vol. 350, Issue 6256
https://doi.org/10.1126/science.aab3908

The acid test for water structure
journal, February 2016

Agmon, Noam
Nature Chemistry, Vol. 8, Issue 3
https://doi.org/10.1038/nchem.2465

Ab Initio Molecular Dynamics Simulations of an Excess Proton in a Triethylene Glycol–Water Solution: Solvation Structure, Mechanism, and Kinetics
journal, May 2016

McDonnell, Marshall T.; Xu, Haixuan; Keffer, David J.
The Journal of Physical Chemistry B, Vol. 120, Issue 23
https://doi.org/10.1021/acs.jpcb.6b02445

A coarse-grained model for polyethylene glycol polymer
journal, December 2011

Wang, Qifei; Keffer, David J.; Nicholson, Donald M.
The Journal of Chemical Physics, Vol. 135, Issue 21
https://doi.org/10.1063/1.3664623

A Coarse-Grained Implicit Solvent Model for Poly(ethylene oxide), Cn E m Surfactants, and Hydrophobically End-Capped Poly(ethylene oxide) and Its Application to Micelle Self-Assembly and Phase Behavior
journal, October 2015

Wang, Shihu; Larson, Ronald G.
Macromolecules, Vol. 48, Issue 20
https://doi.org/10.1021/acs.macromol.5b01587

A Coarse-Grained Model for Polyethylene Oxide and Polyethylene Glycol: Conformation and Hydrodynamics
journal, October 2009

Lee, Hwankyu; de Vries, Alex H.; Marrink, Siewert-Jan
The Journal of Physical Chemistry B, Vol. 113, Issue 40
https://doi.org/10.1021/jp9058966

Coarse-Grained Model for PEGylated Lipids: Effect of PEGylation on the Size and Shape of Self-Assembled Structures
journal, June 2011

Lee, Hwankyu; Pastor, Richard W.
The Journal of Physical Chemistry B, Vol. 115, Issue 24
https://doi.org/10.1021/jp2020148

A Coarse-Grained MARTINI Model of Polyethylene Glycol and of Polyoxyethylene Alkyl Ether Surfactants
journal, November 2012

Rossi, G.; Fuchs, P. F. J.; Barnoud, J.
The Journal of Physical Chemistry B, Vol. 116, Issue 49
https://doi.org/10.1021/jp3095165

Coarse-Grained Models for Aqueous Polyethylene Glycol Solutions
journal, December 2013

Choi, Eunsong; Mondal, Jagannath; Yethiraj, Arun
The Journal of Physical Chemistry B, Vol. 118, Issue 1
https://doi.org/10.1021/jp408392b

Effect of Chain Length on the Partition Properties of Poly(ethylene oxide): Comparison between MARTINI Coarse-Grained and Atomistic Models
journal, February 2017

Taddese, Tseden; Carbone, Paola
The Journal of Physical Chemistry B, Vol. 121, Issue 7
https://doi.org/10.1021/acs.jpcb.6b10858

Hybrid Atomistic and Coarse-Grained Molecular Dynamics Simulations of Polyethylene Glycol (PEG) in Explicit Water
journal, April 2016

Stanzione, Francesca; Jayaraman, Arthi
The Journal of Physical Chemistry B, Vol. 120, Issue 17
https://doi.org/10.1021/acs.jpcb.6b02327

Multistate Empirical Valence Bond Model for Proton Transport in Water
journal, July 1998

Schmitt, Udo W.; Voth, Gregory A.
The Journal of Physical Chemistry B, Vol. 102, Issue 29
https://doi.org/10.1021/jp9818131

The computer simulation of proton transport in water
journal, November 1999

Schmitt, Udo W.; Voth, Gregory A.
The Journal of Chemical Physics, Vol. 111, Issue 20
https://doi.org/10.1063/1.480032

A second generation multistate empirical valence bond model for proton transport in aqueous systems
journal, September 2002

Day, Tyler J. F.; Soudackov, Alexander V.; Čuma, Martin
The Journal of Chemical Physics, Vol. 117, Issue 12
https://doi.org/10.1063/1.1497157

Theoretical studies of enzymic reactions: Dielectric, electrostatic and steric stabilization of the carbonium ion in the reaction of lysozyme
journal, May 1976

Warshel, A.; Levitt, M.
Journal of Molecular Biology, Vol. 103, Issue 2
https://doi.org/10.1016/0022-2836(76)90311-9

Adaptive-Partitioning QM/MM for Molecular Dynamics Simulations: 4. Proton Hopping in Bulk Water
journal, May 2015

Pezeshki, Soroosh; Lin, Hai
Journal of Chemical Theory and Computation, Vol. 11, Issue 6
https://doi.org/10.1021/ct501019y

A Reactive Molecular Dynamics Algorithm for Proton Transport in Aqueous Systems
journal, June 2010

Selvan, Myvizhi Esai; Keffer, David J.; Cui, Shengting
The Journal of Physical Chemistry C, Vol. 114, Issue 27
https://doi.org/10.1021/jp101680q

Proton transport in water confined in carbon nanotubes: a reactive molecular dynamics study
journal, June 2010

Esai Selvan, M.; Keffer, D. J.; Cui, S.
Molecular Simulation, Vol. 36, Issue 7-8
https://doi.org/10.1080/08927021003752887

Reactive Molecular Dynamics Study of Proton Transport in Polymer Electrolyte Membranes
journal, September 2011

Selvan, Myvizhi Esai; Keffer, David J.; Cui, Shengting
The Journal of Physical Chemistry C, Vol. 115, Issue 38
https://doi.org/10.1021/jp203443c

Molecular dynamics simulation of proton transport with quantum mechanically derived proton hopping rates (Q-HOP MD)
journal, November 2001

Lill, Markus A.; Helms, Volkhard
The Journal of Chemical Physics, Vol. 115, Issue 17
https://doi.org/10.1063/1.1407293

ReaxFF: A Reactive Force Field for Hydrocarbons
journal, October 2001

van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois
The Journal of Physical Chemistry A, Vol. 105, Issue 41
https://doi.org/10.1021/jp004368u

The ReaxFF reactive force-field: development, applications and future directions
journal, March 2016

Senftle, Thomas P.; Hong, Sungwook; Islam, Md Mahbubul
npj Computational Materials, Vol. 2, Issue 1
https://doi.org/10.1038/npjcompumats.2015.11

Computational aspects of many-body potentials
journal, May 2012

Plimpton, Steven J.; Thompson, Aidan P.
MRS Bulletin, Vol. 37, Issue 5
https://doi.org/10.1557/mrs.2012.96

Second-Generation ReaxFF Water Force Field: Improvements in the Description of Water Density and OH-Anion Diffusion
journal, June 2017

Zhang, Weiwei; van Duin, Adri C. T.
The Journal of Physical Chemistry B, Vol. 121, Issue 24
https://doi.org/10.1021/acs.jpcb.7b02548

Confinement effects on the thermal stability of poly(ethylene oxide)/graphene nanocomposites: A reactive molecular dynamics simulation study
journal, April 2017

Rahmani, Farzin; Mahdavi, Mina; Nouranian, Sasan
Journal of Polymer Science Part B: Polymer Physics, Vol. 55, Issue 13
https://doi.org/10.1002/polb.24355

Exploring the conformational and reactive dynamics of biomolecules in solution using an extended version of the glycine reactive force field
journal, January 2013

Monti, Susanna; Corozzi, Alessandro; Fristrup, Peter
Physical Chemistry Chemical Physics, Vol. 15, Issue 36
https://doi.org/10.1039/c3cp51931g

Development of a ReaxFF Reactive Force Field for Glycine and Application to Solvent Effect and Tautomerization
journal, January 2011

Rahaman, Obaidur; van Duin, Adri C. T.; Goddard, William A.
The Journal of Physical Chemistry B, Vol. 115, Issue 2
https://doi.org/10.1021/jp108642r

NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations
journal, September 2010

Valiev, M.; Bylaska, E. J.; Govind, N.
Computer Physics Communications, Vol. 181, Issue 9, p. 1477-1489
https://doi.org/10.1016/j.cpc.2010.04.018

Evaluation of B3LYP, X3LYP, and M06-Class Density Functionals for Predicting the Binding Energies of Neutral, Protonated, and Deprotonated Water Clusters
journal, March 2009

Bryantsev, Vyacheslav S.; Diallo, Mamadou S.; van Duin, Adri C. T.
Journal of Chemical Theory and Computation, Vol. 5, Issue 4
https://doi.org/10.1021/ct800549f

The individual and collective effects of exact exchange and dispersion interactions on the ab initio structure of liquid water
journal, August 2014

DiStasio, Robert A.; Santra, Biswajit; Li, Zhaofeng
The Journal of Chemical Physics, Vol. 141, Issue 8
https://doi.org/10.1063/1.4893377

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications
journal, March 2017

Hermann, Jan; DiStasio, Robert A.; Tkatchenko, Alexandre
Chemical Reviews, Vol. 117, Issue 6
https://doi.org/10.1021/acs.chemrev.6b00446

General Multiobjective Force Field Optimization Framework, with Application to Reactive Force Fields for Silicon Carbide
journal, March 2014

Jaramillo-Botero, Andres; Naserifar, Saber; Goddard, William A.
Journal of Chemical Theory and Computation, Vol. 10, Issue 4
https://doi.org/10.1021/ct5001044

OGOLEM: Global cluster structure optimisation for arbitrary mixtures of flexible molecules. A multiscaling, object-oriented approach
journal, February 2010

Dieterich, Johannes M.; Hartke, Bernd
Molecular Physics, Vol. 108, Issue 3-4
https://doi.org/10.1080/00268970903446756

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Plimpton, Steve
Journal of Computational Physics, Vol. 117, Issue 1
https://doi.org/10.1006/jcph.1995.1039

Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals
journal, June 1984

Daw, Murray S.; Baskes, M. I.
Physical Review B, Vol. 29, Issue 12
https://doi.org/10.1103/PhysRevB.29.6443

Second-generation charge-optimized many-body potential for $Si / {SiO}_{2}$ and amorphous silica
journal, December 2010

Shan, Tzu-Ray; Devine, Bryce D.; Hawkins, Jeffery M.
Physical Review B, Vol. 82, Issue 23
https://doi.org/10.1103/PhysRevB.82.235302

Classical atomistic simulations of surfaces and heterogeneous interfaces with the charge-optimized many body (COMB) potentials
journal, September 2013

Liang, Tao; Shan, Tzu-Ray; Cheng, Yu-Ting
Materials Science and Engineering: R: Reports, Vol. 74, Issue 9
https://doi.org/10.1016/j.mser.2013.07.001

A third-generation charge optimized many body (COMB3) potential for nitrogen-containing organic molecules
journal, November 2017

Martinez, Jackelyn; Liang, Tao; Sinnott, Susan B.
Computational Materials Science, Vol. 139
https://doi.org/10.1016/j.commatsci.2017.07.019

Multiscale modeling of soft matter: scaling of dynamics
journal, January 2011

Fritz, Dominik; Koschke, Konstantin; Harmandaris, Vagelis A.
Physical Chemistry Chemical Physics, Vol. 13, Issue 22
https://doi.org/10.1039/c1cp20247b

Optimized pseudopotentials
journal, January 1990

Rappe, Andrew M.; Rabe, Karin M.; Kaxiras, Efthimios
Physical Review B, Vol. 41, Issue 2
https://doi.org/10.1103/PhysRevB.41.1227

Designed nonlocal pseudopotentials for enhanced transferability
journal, May 1999

Ramer, Nicholas J.; Rappe, Andrew M.
Physical Review B, Vol. 59, Issue 19
https://doi.org/10.1103/PhysRevB.59.12471

Excited-state proton transfer to methanol-water mixtures
journal, December 1991

Agmon, Noam; Huppert, Dan; Masad, Asnat
The Journal of Physical Chemistry, Vol. 95, Issue 25
https://doi.org/10.1021/j100178a030

PACKMOL: A package for building initial configurations for molecular dynamics simulations
journal, October 2009

Martínez, L.; Andrade, R.; Birgin, E. G.
Journal of Computational Chemistry, Vol. 30, Issue 13
https://doi.org/10.1002/jcc.21224

Molecular dynamics with coupling to an external bath
journal, October 1984

Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F.
The Journal of Chemical Physics, Vol. 81, Issue 8
https://doi.org/10.1063/1.448118

Dynamical properties of liquid water from ab initio molecular dynamics performed in the complete basis set limit
journal, April 2007

Lee, Hee-Seung; Tuckerman, Mark E.
The Journal of Chemical Physics, Vol. 126, Issue 16
https://doi.org/10.1063/1.2718521

Extraction of self-diffusivity in systems with nondiffusive short-time behavior
journal, October 2013

Shanbhag, Sachin
Physical Review E, Vol. 88, Issue 4
https://doi.org/10.1103/PhysRevE.88.042816

Special Pair Dance and Partner Selection: Elementary Steps in Proton Transport in Liquid Water
journal, August 2008

Markovitch, Omer; Chen, Hanning; Izvekov, Sergei
The Journal of Physical Chemistry B, Vol. 112, Issue 31
https://doi.org/10.1021/jp804018y

The nature of the hydrated excess proton in water
journal, February 1999

Marx, Dominik; Tuckerman, Mark E.; Hutter, Jürg
Nature, Vol. 397, Issue 6720
https://doi.org/10.1038/17579

On the Quantum Nature of the Shared Proton in Hydrogen Bonds
journal, February 1997

Tuckerman, M. E.
Science, Vol. 275, Issue 5301
https://doi.org/10.1126/science.275.5301.817

Concerted Hydrogen-Bond Dynamics in the Transport Mechanism of the Hydrated Proton: A First-Principles Molecular Dynamics Study
journal, November 2009

Berkelbach, Timothy C.; Lee, Hee-Seung; Tuckerman, Mark E.
Physical Review Letters, Vol. 103, Issue 23
https://doi.org/10.1103/PhysRevLett.103.238302

Water at hydrophobic interfaces delays proton surface-to-bulk transfer and provides a pathway for lateral proton diffusion
journal, June 2012

Zhang, C.; Knyazev, D. G.; Vereshaga, Y. A.
Proceedings of the National Academy of Sciences, Vol. 109, Issue 25
https://doi.org/10.1073/pnas.1121227109

Proton transfer through the water gossamer
journal, July 2013

Hassanali, Ali; Giberti, Federico; Cuny, Jérôme
Proceedings of the National Academy of Sciences, Vol. 110, Issue 34
https://doi.org/10.1073/pnas.1306642110

Water structure and changes in thermal stability of the system poly(ethylene oxide)–water
journal, January 1981

Kjellander, Roland; Florin, Ebba
Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 77, Issue 9
https://doi.org/10.1039/f19817702053

Elementary Steps of Lithium Ion Transport in PEO via Quantum Mechanical Calculations
journal, June 1998

Johansson, Patrik; Tegenfeldt, Jörgen; Lindgren, Jan
The Journal of Physical Chemistry A, Vol. 102, Issue 24
https://doi.org/10.1021/jp980638l

Molecular dynamics simulation of the structure of an ion-conducting PEO-based solid polymer electrolyte
journal, September 2002

Ennari, Jaana; Pietilä, Lars-Olof; Virkkunen, Ville
Polymer, Vol. 43, Issue 20
https://doi.org/10.1016/S0032-3861(02)00432-9

Similar records in OSTI.GOV collections:

Diketopyrrolopyrrole-Based Conjugated Polymer Entailing Triethylene Glycols as Side Chains with High Thin-Film Charge Mobility without Post-Treatments

Journal Article Yang, Si-Fen ; Liu, Zi-Tong ; Cai, Zheng-Xu ; ... - Advanced Science

Side chain engineering of conjugated donor-acceptor polymers is a new way to manipulate their optoelectronic properties. Two new diketopyrrolopyrrole (DPP)-terthiophene-based conjugated polymers PDPP3T-1 and PDPP3T-2, with both hydrophilic triethylene glycol (TEG) and hydrophobic alkyl chains, are reported. It is demonstrated that the incorporation of TEG chains has a significant effect on the interchain packing and thin-film morphology with noticeable effect on charge transport. Polymer chains of PDPP3T-1 in which TEG chains are uniformly distributed can self-assemble spontaneously into a more ordered thin film. As a result, the thin film of PDPP3T-1 exhibits high saturated hole mobility up to 2.6 cm(2)more »« less
https://doi.org/10.1002/advs.201700048
Final Report: Computer Simulation of Proton Transport in Fuel Cell Membranes

Technical Report Voth, Gregory A

Period of Performance: 09/01/2010 – 8/31/2018 Narrative This DOE-supported research grant focused on understanding the nature of proton transport in complex systems such as proton exchange membranes (PEMs). The most unique aspect of the research was the development and implementation of a novel multiscale reactive molecular dynamics (MS-RMD) methodology. In this approach, covalent bonds can dynamically break and form, allowing one to accurately treat the proton hopping process essential to capturing the physics of proton transport. The Voth group applied this method to proton exchange membrane systems, providing insight into their proton transport mechanism. They found that protons can diffusemore »« less
https://doi.org/10.2172/1600007

Full Text Available
Experimental vapor-liquid equilibria in the CO/sub 2/-diethylene glycol-H/sub 2/O and CO/sub 2/-triethylene glycol-H/sub 2/O systems at feasible absorption temperatures and pressures

Journal Article Takahashi, S ; Kobayashi, R ; Song, K Y - J. Chem. Eng. Data; (United States)

The water contents of compressed carbon dioxide gas in equilibrium with diethylene glycol (DEG) solutions of 3.5 and 7.0 wt % water, and with triethylene glycol (TEG) solutions of the same concentrations, have been measured at temperatures of 23.89, 37.78, and 48.89 /sup 0/C, and pressures of 2.5166, 2.8955, and 5.2745 MPa. A comparison of the dehydration capabilities of the same glycol-water solution for CO/sub 2/ with that for natural gas (or methane) indicates that the dehydration qualities for the former (CO/sub 2/) exceed those for the latter on an absolute water content basis until a reversal occurs when themore »« less
https://doi.org/10.1021/je00035a010
Complementary Semiconducting Polymer Blends: Influence of Side Chains of Matrix Polymers

Journal Article Zhao, Xikang ; Xue, Guobiao ; Qu, Ge ; ... - Macromolecules

The concept of complementary semiconducting polymer blends (c-SPBs) has been recently proposed to achieve enhanced solution processability and/or melt-processing capability for organic electronics. In the previous study, we demonstrated the impact of conjugation-break spacers of matrix polymers. In the current work, we explore the influence of the side chains of the matrix polymer on the physical properties of the pure polymers and their corresponding c-SPBs, including electrical properties and phase transition behaviors. Specifically, six diketopyrrolopyrrole (DPP)-based polymers with pentamethylene conjugation-break spacers (CBSs) and various side chains, including branched-alkyl, triethylene glycol (TEG), and siloxaneterminated side chains, were synthesized and characterized. Themore »« less
Cited by 10
https://doi.org/10.1021/acs.macromol.7b01354

Full Text Available
Alternative (Potentially Green) Separations Media: Aqueous Biphasic and Related Systems Extending the Frontier Final Report For Period September 1, 2002 January 31, 2007

Technical Report Rogers, Robin D

Through the current DoE-BES funding, we have extended our fundamental understanding of the critical phase separation of aqueous polymer solutions at the molecular level, and have developed a similar understanding of their application as novel solvent systems. Our principal aims included mode of delivery of the aqueous biphasic system (ABS) solvent system and the application of this system to problems of reactive extraction. In the former case we have developed novel solid phase analogues, in the form of cross-linked polyethylene glycol hydrogels, and in the latter case we have examined the role that ABS might play in reaction engineering, withmore »« less
https://doi.org/10.2172/909126

Full Text Available

Similar Records

Title: Reactive molecular dynamics simulations of an excess proton in polyethylene glycol-water solutions

Abstract

Citation Formats

Effect of pegylation on pharmaceuticals journal, March 2003

PEGylation, successful approach to drug delivery journal, November 2005

PEG — A versatile conjugating ligand for drugs and drug delivery systems journal, October 2014

A sol–gel synthesis of polyether-based proton conducting electrolytes journal, October 2003

Effect of Polymer Structure on Ion Transport in an Anhydrous Proton Conducting Electrolyte journal, February 2010

Effects of Bulky Copolymers on Ion Transport in an Anhydrous Proton-Conducting Electrolyte journal, January 2010

Star-Shaped MePEG n Polymers as H + Conducting Electrolytes journal, July 2011

Polyethylene glycol-functionalized polyoctahedral silsesquioxanes as H+-conducting electrolytes journal, February 2014

Volume Fraction of Ether Is a Significant Factor in Controlling Conductivity in Proton Conducting Polyether Based Polymer Sol–Gel Electrolytes journal, October 2014

High temperature proton exchange membranes with enhanced proton conductivities at low humidity and high temperature based on polymer blends and block copolymers of poly(1,3-cyclohexadiene) and poly(ethylene glycol) journal, October 2015

Structure and Diffusion in Cross-Linked and Sulfonated Poly(1,3-cyclohexadiene)/Polyethylene Glycol-Based Proton Exchange Membranes journal, March 2013

Computational Design of Oligopeptide Containing Poly(ethylene glycol) Brushes for Stimuli-Responsive Drug Delivery journal, October 2015

Stimuli-responsive nanocarriers for drug delivery journal, October 2013

The Grotthuss mechanism journal, October 1995

Proton Transfer 200 Years after von Grotthuss: Insights from Ab Initio Simulations journal, September 2006

An analysis of hydrated proton diffusion in ab initio molecular dynamics journal, January 2015

Proton mobility in aqueous systems: combining ab initio accuracy with millisecond timescales journal, January 2017

Protons and Hydroxide Ions in Aqueous Systems journal, April 2016

Proton Transfer, Acid-Base Catalysis, and Enzymatic Hydrolysis. Part I: ELEMENTARY PROCESSES journal, January 1964

Aqueous solutions: state of the art in ab initio molecular dynamics journal, March 2014

The Role of Quantum Effects on Structural and Electronic Fluctuations in Neat and Charged Water journal, November 2014

Role of Presolvation and Anharmonicity in Aqueous Phase Hydrated Proton Solvation and Transport journal, November 2015

Ultrafast Vibrational and Structural Dynamics of the Proton in Liquid Water journal, April 2006

Ultrafast 2D IR spectroscopy of the excess proton in liquid water journal, October 2015

The acid test for water structure journal, February 2016

Ab Initio Molecular Dynamics Simulations of an Excess Proton in a Triethylene Glycol–Water Solution: Solvation Structure, Mechanism, and Kinetics journal, May 2016

A coarse-grained model for polyethylene glycol polymer journal, December 2011

A Coarse-Grained Implicit Solvent Model for Poly(ethylene oxide), Cn E m Surfactants, and Hydrophobically End-Capped Poly(ethylene oxide) and Its Application to Micelle Self-Assembly and Phase Behavior journal, October 2015

A Coarse-Grained Model for Polyethylene Oxide and Polyethylene Glycol: Conformation and Hydrodynamics journal, October 2009

Coarse-Grained Model for PEGylated Lipids: Effect of PEGylation on the Size and Shape of Self-Assembled Structures journal, June 2011

A Coarse-Grained MARTINI Model of Polyethylene Glycol and of Polyoxyethylene Alkyl Ether Surfactants journal, November 2012

Coarse-Grained Models for Aqueous Polyethylene Glycol Solutions journal, December 2013

Effect of Chain Length on the Partition Properties of Poly(ethylene oxide): Comparison between MARTINI Coarse-Grained and Atomistic Models journal, February 2017

Hybrid Atomistic and Coarse-Grained Molecular Dynamics Simulations of Polyethylene Glycol (PEG) in Explicit Water journal, April 2016

Multistate Empirical Valence Bond Model for Proton Transport in Water journal, July 1998

The computer simulation of proton transport in water journal, November 1999

A second generation multistate empirical valence bond model for proton transport in aqueous systems journal, September 2002

Theoretical studies of enzymic reactions: Dielectric, electrostatic and steric stabilization of the carbonium ion in the reaction of lysozyme journal, May 1976

Adaptive-Partitioning QM/MM for Molecular Dynamics Simulations: 4. Proton Hopping in Bulk Water journal, May 2015

A Reactive Molecular Dynamics Algorithm for Proton Transport in Aqueous Systems journal, June 2010

Proton transport in water confined in carbon nanotubes: a reactive molecular dynamics study journal, June 2010

Reactive Molecular Dynamics Study of Proton Transport in Polymer Electrolyte Membranes journal, September 2011

Molecular dynamics simulation of proton transport with quantum mechanically derived proton hopping rates (Q-HOP MD) journal, November 2001

ReaxFF: A Reactive Force Field for Hydrocarbons journal, October 2001

The ReaxFF reactive force-field: development, applications and future directions journal, March 2016

Computational aspects of many-body potentials journal, May 2012

Second-Generation ReaxFF Water Force Field: Improvements in the Description of Water Density and OH-Anion Diffusion journal, June 2017

Confinement effects on the thermal stability of poly(ethylene oxide)/graphene nanocomposites: A reactive molecular dynamics simulation study journal, April 2017

Exploring the conformational and reactive dynamics of biomolecules in solution using an extended version of the glycine reactive force field journal, January 2013

Development of a ReaxFF Reactive Force Field for Glycine and Application to Solvent Effect and Tautomerization journal, January 2011

NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations journal, September 2010

Evaluation of B3LYP, X3LYP, and M06-Class Density Functionals for Predicting the Binding Energies of Neutral, Protonated, and Deprotonated Water Clusters journal, March 2009

The individual and collective effects of exact exchange and dispersion interactions on the ab initio structure of liquid water journal, August 2014

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications journal, March 2017

General Multiobjective Force Field Optimization Framework, with Application to Reactive Force Fields for Silicon Carbide journal, March 2014

OGOLEM: Global cluster structure optimisation for arbitrary mixtures of flexible molecules. A multiscaling, object-oriented approach journal, February 2010

Fast Parallel Algorithms for Short-Range Molecular Dynamics journal, March 1995

Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals journal, June 1984

Second-generation charge-optimized many-body potential for Si / SiO 2 and amorphous silica journal, December 2010

Classical atomistic simulations of surfaces and heterogeneous interfaces with the charge-optimized many body (COMB) potentials journal, September 2013

A third-generation charge optimized many body (COMB3) potential for nitrogen-containing organic molecules journal, November 2017

Multiscale modeling of soft matter: scaling of dynamics journal, January 2011

Optimized pseudopotentials journal, January 1990

Designed nonlocal pseudopotentials for enhanced transferability journal, May 1999

Excited-state proton transfer to methanol-water mixtures journal, December 1991

PACKMOL: A package for building initial configurations for molecular dynamics simulations journal, October 2009

Molecular dynamics with coupling to an external bath journal, October 1984

Dynamical properties of liquid water from ab initio molecular dynamics performed in the complete basis set limit journal, April 2007

Extraction of self-diffusivity in systems with nondiffusive short-time behavior journal, October 2013

Special Pair Dance and Partner Selection: Elementary Steps in Proton Transport in Liquid Water journal, August 2008

The nature of the hydrated excess proton in water journal, February 1999

On the Quantum Nature of the Shared Proton in Hydrogen Bonds journal, February 1997

Concerted Hydrogen-Bond Dynamics in the Transport Mechanism of the Hydrated Proton: A First-Principles Molecular Dynamics Study journal, November 2009

Water at hydrophobic interfaces delays proton surface-to-bulk transfer and provides a pathway for lateral proton diffusion journal, June 2012

Proton transfer through the water gossamer journal, July 2013

Water structure and changes in thermal stability of the system poly(ethylene oxide)–water journal, January 1981

Elementary Steps of Lithium Ion Transport in PEO via Quantum Mechanical Calculations journal, June 1998

Effect of pegylation on pharmaceuticals
journal, March 2003

PEGylation, successful approach to drug delivery
journal, November 2005

PEG — A versatile conjugating ligand for drugs and drug delivery systems
journal, October 2014

A sol–gel synthesis of polyether-based proton conducting electrolytes
journal, October 2003

Effect of Polymer Structure on Ion Transport in an Anhydrous Proton Conducting Electrolyte
journal, February 2010

Effects of Bulky Copolymers on Ion Transport in an Anhydrous Proton-Conducting Electrolyte
journal, January 2010

Star-Shaped MePEG _n Polymers as H ⁺ Conducting Electrolytes
journal, July 2011

Polyethylene glycol-functionalized polyoctahedral silsesquioxanes as H+-conducting electrolytes
journal, February 2014

Volume Fraction of Ether Is a Significant Factor in Controlling Conductivity in Proton Conducting Polyether Based Polymer Sol–Gel Electrolytes
journal, October 2014

High temperature proton exchange membranes with enhanced proton conductivities at low humidity and high temperature based on polymer blends and block copolymers of poly(1,3-cyclohexadiene) and poly(ethylene glycol)
journal, October 2015

Structure and Diffusion in Cross-Linked and Sulfonated Poly(1,3-cyclohexadiene)/Polyethylene Glycol-Based Proton Exchange Membranes
journal, March 2013

Computational Design of Oligopeptide Containing Poly(ethylene glycol) Brushes for Stimuli-Responsive Drug Delivery
journal, October 2015

Stimuli-responsive nanocarriers for drug delivery
journal, October 2013

The Grotthuss mechanism
journal, October 1995

Proton Transfer 200 Years after von Grotthuss: Insights from Ab Initio Simulations
journal, September 2006

An analysis of hydrated proton diffusion in ab initio molecular dynamics
journal, January 2015

Proton mobility in aqueous systems: combining ab initio accuracy with millisecond timescales
journal, January 2017

Protons and Hydroxide Ions in Aqueous Systems
journal, April 2016

Proton Transfer, Acid-Base Catalysis, and Enzymatic Hydrolysis. Part I: ELEMENTARY PROCESSES
journal, January 1964

Aqueous solutions: state of the art in ab initio molecular dynamics
journal, March 2014

The Role of Quantum Effects on Structural and Electronic Fluctuations in Neat and Charged Water
journal, November 2014

Role of Presolvation and Anharmonicity in Aqueous Phase Hydrated Proton Solvation and Transport
journal, November 2015

Ultrafast Vibrational and Structural Dynamics of the Proton in Liquid Water
journal, April 2006

Ultrafast 2D IR spectroscopy of the excess proton in liquid water
journal, October 2015

The acid test for water structure
journal, February 2016

Ab Initio Molecular Dynamics Simulations of an Excess Proton in a Triethylene Glycol–Water Solution: Solvation Structure, Mechanism, and Kinetics
journal, May 2016

A coarse-grained model for polyethylene glycol polymer
journal, December 2011

A Coarse-Grained Implicit Solvent Model for Poly(ethylene oxide), Cn E m Surfactants, and Hydrophobically End-Capped Poly(ethylene oxide) and Its Application to Micelle Self-Assembly and Phase Behavior
journal, October 2015

A Coarse-Grained Model for Polyethylene Oxide and Polyethylene Glycol: Conformation and Hydrodynamics
journal, October 2009

Coarse-Grained Model for PEGylated Lipids: Effect of PEGylation on the Size and Shape of Self-Assembled Structures
journal, June 2011

A Coarse-Grained MARTINI Model of Polyethylene Glycol and of Polyoxyethylene Alkyl Ether Surfactants
journal, November 2012

Coarse-Grained Models for Aqueous Polyethylene Glycol Solutions
journal, December 2013

Effect of Chain Length on the Partition Properties of Poly(ethylene oxide): Comparison between MARTINI Coarse-Grained and Atomistic Models
journal, February 2017

Hybrid Atomistic and Coarse-Grained Molecular Dynamics Simulations of Polyethylene Glycol (PEG) in Explicit Water
journal, April 2016

Multistate Empirical Valence Bond Model for Proton Transport in Water
journal, July 1998

The computer simulation of proton transport in water
journal, November 1999

A second generation multistate empirical valence bond model for proton transport in aqueous systems
journal, September 2002

Theoretical studies of enzymic reactions: Dielectric, electrostatic and steric stabilization of the carbonium ion in the reaction of lysozyme
journal, May 1976

Adaptive-Partitioning QM/MM for Molecular Dynamics Simulations: 4. Proton Hopping in Bulk Water
journal, May 2015

A Reactive Molecular Dynamics Algorithm for Proton Transport in Aqueous Systems
journal, June 2010

Proton transport in water confined in carbon nanotubes: a reactive molecular dynamics study
journal, June 2010

Reactive Molecular Dynamics Study of Proton Transport in Polymer Electrolyte Membranes
journal, September 2011

Molecular dynamics simulation of proton transport with quantum mechanically derived proton hopping rates (Q-HOP MD)
journal, November 2001

ReaxFF: A Reactive Force Field for Hydrocarbons
journal, October 2001

The ReaxFF reactive force-field: development, applications and future directions
journal, March 2016

Computational aspects of many-body potentials
journal, May 2012

Second-Generation ReaxFF Water Force Field: Improvements in the Description of Water Density and OH-Anion Diffusion
journal, June 2017

Confinement effects on the thermal stability of poly(ethylene oxide)/graphene nanocomposites: A reactive molecular dynamics simulation study
journal, April 2017

Exploring the conformational and reactive dynamics of biomolecules in solution using an extended version of the glycine reactive force field
journal, January 2013

Development of a ReaxFF Reactive Force Field for Glycine and Application to Solvent Effect and Tautomerization
journal, January 2011

NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations
journal, September 2010

Evaluation of B3LYP, X3LYP, and M06-Class Density Functionals for Predicting the Binding Energies of Neutral, Protonated, and Deprotonated Water Clusters
journal, March 2009

The individual and collective effects of exact exchange and dispersion interactions on the ab initio structure of liquid water
journal, August 2014

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications
journal, March 2017

General Multiobjective Force Field Optimization Framework, with Application to Reactive Force Fields for Silicon Carbide
journal, March 2014

OGOLEM: Global cluster structure optimisation for arbitrary mixtures of flexible molecules. A multiscaling, object-oriented approach
journal, February 2010

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals
journal, June 1984

Second-generation charge-optimized many-body potential for $Si / {SiO}_{2}$ and amorphous silica
journal, December 2010

Classical atomistic simulations of surfaces and heterogeneous interfaces with the charge-optimized many body (COMB) potentials
journal, September 2013

A third-generation charge optimized many body (COMB3) potential for nitrogen-containing organic molecules
journal, November 2017

Multiscale modeling of soft matter: scaling of dynamics
journal, January 2011

Optimized pseudopotentials
journal, January 1990

Designed nonlocal pseudopotentials for enhanced transferability
journal, May 1999

Excited-state proton transfer to methanol-water mixtures
journal, December 1991

PACKMOL: A package for building initial configurations for molecular dynamics simulations
journal, October 2009

Molecular dynamics with coupling to an external bath
journal, October 1984

Dynamical properties of liquid water from ab initio molecular dynamics performed in the complete basis set limit
journal, April 2007

Extraction of self-diffusivity in systems with nondiffusive short-time behavior
journal, October 2013

Special Pair Dance and Partner Selection: Elementary Steps in Proton Transport in Liquid Water
journal, August 2008

The nature of the hydrated excess proton in water
journal, February 1999

On the Quantum Nature of the Shared Proton in Hydrogen Bonds
journal, February 1997

Concerted Hydrogen-Bond Dynamics in the Transport Mechanism of the Hydrated Proton: A First-Principles Molecular Dynamics Study
journal, November 2009

Water at hydrophobic interfaces delays proton surface-to-bulk transfer and provides a pathway for lateral proton diffusion
journal, June 2012

Proton transfer through the water gossamer
journal, July 2013

Water structure and changes in thermal stability of the system poly(ethylene oxide)–water
journal, January 1981

Elementary Steps of Lithium Ion Transport in PEO via Quantum Mechanical Calculations
journal, June 1998

Molecular dynamics simulation of the structure of an ion-conducting PEO-based solid polymer electrolyte
journal, September 2002