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Title: On the nanosecond proton dynamics in phosphoric acid–benzimidazole and phosphoric acid–water mixtures

Abstract

Combining 1H-NMR, 17O-NMR, and high-resolution backscattering QENS hydrodynamic and structural proton transport in phosphoric acid is separated. The rate limiting steps for structural proton diffusion in mixtures of acid with Brønsted bases are found to occur below the nanosecond timescale.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Max Planck Inst. for Solid State Research, Stuttgart (Germany)
  2. Inst. Laue-Langevin (ILL), Grenoble (France)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1407718
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 42; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Melchior, Jan-Patrick, and Frick, Bernhard. On the nanosecond proton dynamics in phosphoric acid–benzimidazole and phosphoric acid–water mixtures. United States: N. p., 2017. Web. doi:10.1039/C7CP04116K.
Melchior, Jan-Patrick, & Frick, Bernhard. On the nanosecond proton dynamics in phosphoric acid–benzimidazole and phosphoric acid–water mixtures. United States. doi:10.1039/C7CP04116K.
Melchior, Jan-Patrick, and Frick, Bernhard. Fri . "On the nanosecond proton dynamics in phosphoric acid–benzimidazole and phosphoric acid–water mixtures". United States. doi:10.1039/C7CP04116K. https://www.osti.gov/servlets/purl/1407718.
@article{osti_1407718,
title = {On the nanosecond proton dynamics in phosphoric acid–benzimidazole and phosphoric acid–water mixtures},
author = {Melchior, Jan-Patrick and Frick, Bernhard},
abstractNote = {Combining1H-NMR,17O-NMR, and high-resolution backscattering QENS hydrodynamic and structural proton transport in phosphoric acid is separated. The rate limiting steps for structural proton diffusion in mixtures of acid with Brønsted bases are found to occur below the nanosecond timescale.},
doi = {10.1039/C7CP04116K},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 42,
volume = 19,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
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Works referenced in this record:

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Water distribution in high temperature polymer electrolyte fuel cells
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Mass transport of phosphoric acid in water: A 1H and 31P pulsed gradient spin-echo nuclear magnetic resonance study
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NMR Studies of Mass Transport in High-Acid-Content Fuel Cell Membranes Based on Phosphoric Acid and Polybenzimidazole
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  • New Journal of Chemistry, Vol. 34, Issue 5
  • DOI: 10.1039/b9nj00718k

Structure and Proton Dynamics in Catalytic Layer of HT-PEFC
journal, April 2016


The nanosecond proton dynamics of phosphoric acid – from the solid to the melt – investigated by neutron backscattering
journal, December 2013


Ab initio molecular dynamics simulation of the solvation and transport of hydronium and hydroxyl ions in water
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  • Tuckerman, M.; Laasonen, K.; Sprik, M.
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Oxygen-17 NMR spectroscopy: Basic principles and applications (Part I)
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    Works referencing / citing this record:

    Structure and Proton Dynamics in Catalytic Layer of HT-PEFC
    journal, April 2016


    Investigation of proton-conducting solids
    journal, August 1981


    Probing phosphoric acid redistribution and anion migration in polybenzimidazole membranes
    journal, September 2017


    Observing proton motion on the nanoscale in polymeric electrolyte membranes with quasielastic neutron scattering
    journal, December 2014


    Water distribution in high temperature polymer electrolyte fuel cells
    journal, January 2016


    Influence of morphology on physical properties of poly(2,5-benzimidazole) membranes
    journal, July 2017


    Quasi-elastic neutron scattering and molecular dynamics simulation as complementary techniques for studying diffusion in zeolites
    journal, May 2007


    Oxygen-17 NMR spectroscopy: Basic principles and applications (Part I)
    journal, March 2010


    Oxygen-17 NMR spectroscopy: Basic principles and applications (part II)
    journal, July 2010


    High temperature proton exchange membranes based on polybenzimidazoles for fuel cells
    journal, May 2009


    Proton dynamics of CsH2PO4 studied by quasi-elastic neutron scattering and PFG-NMR
    journal, December 2008


    Proton conductivity and diffusion in molten phosphinic acid (H3PO2): The last member of the phosphorus oxoacid proton conductor family
    journal, March 2012


    First principles molecular dynamics study of proton dynamics and transport in phosphoric acid/imidazole (2:1) system
    journal, December 2013


    The nanosecond proton dynamics of phosphoric acid – from the solid to the melt – investigated by neutron backscattering
    journal, December 2013


    Mechanism of Efficient Proton Conduction in Diphosphoric Acid Elucidated via First-Principles Simulation and NMR
    journal, December 2015

    • Krueger, Rachel A.; Vilčiauskas, Linas; Melchior, Jan-Patrick
    • The Journal of Physical Chemistry B, Vol. 119, Issue 52
    • DOI: 10.1021/acs.jpcb.5b09684

    Proton Conductivity:  Materials and Applications
    journal, January 1996

    • Kreuer, Klaus-Dieter
    • Chemistry of Materials, Vol. 8, Issue 3
    • DOI: 10.1021/cm950192a

    Transport in Proton Conductors for Fuel-Cell Applications:  Simulations, Elementary Reactions, and Phenomenology
    journal, October 2004

    • Kreuer, Klaus-Dieter; Paddison, Stephen J.; Spohr, Eckhard
    • Chemical Reviews, Vol. 104, Issue 10
    • DOI: 10.1021/cr020715f

    Self-Dissociative Equilibria in Molten Phosphoric Acid
    journal, November 1964

    • Munson, Ronald A.
    • The Journal of Physical Chemistry, Vol. 68, Issue 11
    • DOI: 10.1021/j100793a045

    Influence of ionic solutes upon the conductivity of molten phosphoric acid
    journal, September 1967

    • Munson, Ronald A.; Lazarus, Michael E.
    • The Journal of Physical Chemistry, Vol. 71, Issue 10
    • DOI: 10.1021/j100869a018

    The Activation Energies of Proton Transfer Reactions in Water
    journal, November 1964

    • Luz, Z.; Meiboom, S.
    • Journal of the American Chemical Society, Vol. 86, Issue 22
    • DOI: 10.1021/ja01076a008

    The Electrical Conductivity and Viscosity of Concentrated Solutions of Orthophosphoric Acid.
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    • Smith, Alexander; Menzies, Alan W. C.
    • Journal of the American Chemical Society, Vol. 31, Issue 11
    • DOI: 10.1021/ja01941a002

    Density, electrical conductivity, and vapor pressure of concentrated phosphoric acid
    journal, July 1969

    • MacDonald, David I.; Boyack, James R.
    • Journal of Chemical & Engineering Data, Vol. 14, Issue 3
    • DOI: 10.1021/je60042a013

    Ion Conduction Mechanisms and Thermal Properties of Hydrated and Anhydrous Phosphoric Acids Studied with 1 H, 2 H, and 31 P NMR
    journal, December 2006

    • Aihara, Yuichi; Sonai, Atsuo; Hattori, Mineyuki
    • The Journal of Physical Chemistry B, Vol. 110, Issue 49
    • DOI: 10.1021/jp064452v

    Multinuclear NMR Study of the Effect of Acid Concentration on Ion Transport in Phosphoric Acid Doped Poly(benzimidazole) Membranes
    journal, October 2012

    • Suarez, Sophia; Kodiweera, N. K. A. C.; Stallworth, P.
    • The Journal of Physical Chemistry B, Vol. 116, Issue 41
    • DOI: 10.1021/jp304761t

    Ionic Conductivity and Glass Transition of Phosphoric Acids
    journal, June 2013

    • Wang, Yangyang; Lane, Nathan A.; Sun, Che-Nan
    • The Journal of Physical Chemistry B, Vol. 117, Issue 26
    • DOI: 10.1021/jp403867a

    Effect of Benzimidazole Configuration in Polybenzimidazole Chain on Interaction with Phosphoric Acid: A DFT Study
    journal, December 2014

    • Shirata, Kei; Kawauchi, Susumu
    • The Journal of Physical Chemistry B, Vol. 119, Issue 2
    • DOI: 10.1021/jp510067n

    The glass transition temperatures of phosphoric acids
    journal, October 1976


    Proton migration along the membrane surface and retarded surface to bulk transfer
    journal, August 1994

    • Heberle, Joachim; Riesle, Jens; Thiedemann, Gerd
    • Nature, Vol. 370, Issue 6488
    • DOI: 10.1038/370379a0

    The mechanism of proton conduction in phosphoric acid
    journal, April 2012

    • Vilčiauskas, Linas; Tuckerman, Mark E.; Bester, Gabriel
    • Nature Chemistry, Vol. 4, Issue 6
    • DOI: 10.1038/nchem.1329

    Why did Nature select phosphate for its dominant roles in biology?
    journal, January 2010

    • Bowler, Matthew W.; Cliff, Matthew J.; Waltho, Jonathan P.
    • New Journal of Chemistry, Vol. 34, Issue 5
    • DOI: 10.1039/b9nj00718k

    Heat capacity and glass transition in P2O5–H2O solutions: support for Mishima's conjecture on solvent water at low temperature
    journal, January 2011

    • Corti, Horacio R.; Nores-Pondal, Federico J.; Angell, C. Austen
    • Physical Chemistry Chemical Physics, Vol. 13, Issue 44
    • DOI: 10.1039/c1cp22185j

    Proton conduction mechanisms in the phosphoric acid–water system (H 4 P 2 O 7 –H 3 PO 4 ·2H 2 O): a 1 H, 31 P and 17 O PFG-NMR and conductivity study
    journal, January 2017

    • Melchior, Jan-Patrick; Kreuer, Klaus-Dieter; Maier, Joachim
    • Physical Chemistry Chemical Physics, Vol. 19, Issue 1
    • DOI: 10.1039/c6cp04855b

    Why do proton conducting polybenzimidazole phosphoric acid membranes perform well in high-temperature PEM fuel cells?
    journal, January 2017

    • Melchior, Jan-Patrick; Majer, Günter; Kreuer, Klaus-Dieter
    • Physical Chemistry Chemical Physics, Vol. 19, Issue 1
    • DOI: 10.1039/c6cp05331a

    779. Anomalous conduction in phosphoric acid hemihydrate, 2H3PO4,H2O
    journal, January 1959

    • Greenwood, N. N.; Thompson, A.
    • Journal of the Chemical Society (Resumed)
    • DOI: 10.1039/jr9590003864

    Dynamics of the hydrogen and phosphate ions in proton conducting gel/D3PO4 electrolytes: A 2H and 31P nuclear magnetic resonance study
    journal, July 2003

    • Jeffrey, K. R.; Zukowska, G. Z.; Stevens, J. R.
    • The Journal of Chemical Physics, Vol. 119, Issue 4
    • DOI: 10.1063/1.1582844

    Nuclear Magnetic Resonance Study of the Proton Transfer in Water
    journal, February 1961

    • Meiboom, S.
    • The Journal of Chemical Physics, Vol. 34, Issue 2
    • DOI: 10.1063/1.1700960

    Ab initio molecular dynamics simulation of the solvation and transport of hydronium and hydroxyl ions in water
    journal, July 1995

    • Tuckerman, M.; Laasonen, K.; Sprik, M.
    • The Journal of Chemical Physics, Vol. 103, Issue 1
    • DOI: 10.1063/1.469654

    A neutron diffraction and computer modeling study of the interatomic structure of phosphoric acid
    journal, January 1999

    • Tromp, R. Hans; Spieser, Stephane H.; Neilson, George W.
    • The Journal of Chemical Physics, Vol. 110, Issue 4
    • DOI: 10.1063/1.477824

    Mass transport of phosphoric acid in water: A 1H and 31P pulsed gradient spin-echo nuclear magnetic resonance study
    journal, May 2000

    • Chung, S. H.; Bajue, S.; Greenbaum, S. G.
    • The Journal of Chemical Physics, Vol. 112, Issue 19
    • DOI: 10.1063/1.481454

    Incoherent neutron scattering functions for random jump diffusion in bounded and infinite media
    journal, February 1981


    Analysis and visualisation of neutron-scattering data
    journal, December 1996


    Why nature chose phosphates
    journal, March 1987


    Conductivity of PBI Membranes for High-Temperature Polymer Electrolyte Fuel Cells
    journal, January 2004

    • Ma, Y. -L.; Wainright, J. S.; Litt, M. H.
    • Journal of The Electrochemical Society, Vol. 151, Issue 1
    • DOI: 10.1149/1.1630037

    Electro-osmotic Drag Coefficient of Water and Methanol in Polymer Electrolytes at Elevated Temperatures
    journal, January 1996

    • Weng, D.
    • Journal of The Electrochemical Society, Vol. 143, Issue 4
    • DOI: 10.1149/1.1836626

    Acid-Doped Polybenzimidazoles: A New Polymer Electrolyte
    journal, January 1995

    • Wainright, J. S.
    • Journal of The Electrochemical Society, Vol. 142, Issue 7
    • DOI: 10.1149/1.2044337

    NMR Studies of Mass Transport in High-Acid-Content Fuel Cell Membranes Based on Phosphoric Acid and Polybenzimidazole
    journal, January 2007

    • Jayakody, J. R. P.; Chung, S. H.; Durantino, L.
    • Journal of The Electrochemical Society, Vol. 154, Issue 2
    • DOI: 10.1149/1.2405726

    [sup 1]H and [sup 31]P NMR Study of Phosphoric Acid–Doped Polybenzimidazole under Controlled Water Activity
    journal, January 2009

    • Schechter, Alex; Savinell, Robert F.; Wainright, J. S.
    • Journal of The Electrochemical Society, Vol. 156, Issue 2
    • DOI: 10.1149/1.3040211

    Recent Backscattering Instrument Developments at the ILL and SNS
    journal, February 2010

    • Frick, Bernhard; Mamontov, Eugene; Eijck, Lambert van
    • Zeitschrift für Physikalische Chemie, Vol. 224, Issue 1-2
    • DOI: 10.1524/zpch.2010.6091

    Polymer and Composite Membranes for Proton-Conducting, High-Temperature Fuel Cells: A Critical Review
    journal, June 2017

    • Quartarone, Eliana; Angioni, Simone; Mustarelli, Piercarlo
    • Materials, Vol. 10, Issue 7
    • DOI: 10.3390/ma10070687