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Title: Roles of Chemical Functionality and Pore Curvature in the Design of Nanoporous Proton Conductors

Nanoporous proton-transporting media are critical components in fuel cells and other electrochemical devices, yet general molecular design criteria for new materials with enhanced performance remain obscure. Aqueous lyotropic liquid crystals (LLCs) comprise a platform for detailed studies of the molecular-level features governing proton transport in monodisperse, water-filled nanopores lined with well-defined chemical functionalities. Here, we report new alkylsulfonic acid LLCs that exhibit H+ conductivities as high as σ = 380 mS/cm at 80°C, which rival those of more acidic, perfluorinated polymers, thus demonstrating that the acidity of the pore functionality is not the sole determinant of proton transport. Direct experimental comparisons of LLCs with convex and concave nanopores of similar dimensions indicate that H+ conductivities therein sensitively depend on the hydration state of the acid functionalities and the pore curvature. These experiments suggest that judicious manipulation of pore curvature provides a new means for optimizing the activities of proton-exchange membranes and nanoporous solid acid catalysts.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [3]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry
  2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry; Schlumberger Technology Center, Sugar Land, TX (United States)
  3. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry; Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science
Publication Date:
Grant/Contract Number:
SC0010328; AC02-06CH11357; GUP-37637; GUP-50116; CHE-9974839; CHE-1048642; DMR-0832760; DMR-1121288
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 121; Journal Issue: 40; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Research Org:
Univ. of Wisconsin, Madison, WI (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOD; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1434037

Jackson, Grayson L., Perroni, Dominic V., and Mahanthappa, Mahesh K.. Roles of Chemical Functionality and Pore Curvature in the Design of Nanoporous Proton Conductors. United States: N. p., Web. doi:10.1021/acs.jpcb.7b06366.
Jackson, Grayson L., Perroni, Dominic V., & Mahanthappa, Mahesh K.. Roles of Chemical Functionality and Pore Curvature in the Design of Nanoporous Proton Conductors. United States. doi:10.1021/acs.jpcb.7b06366.
Jackson, Grayson L., Perroni, Dominic V., and Mahanthappa, Mahesh K.. 2017. "Roles of Chemical Functionality and Pore Curvature in the Design of Nanoporous Proton Conductors". United States. doi:10.1021/acs.jpcb.7b06366. https://www.osti.gov/servlets/purl/1434037.
@article{osti_1434037,
title = {Roles of Chemical Functionality and Pore Curvature in the Design of Nanoporous Proton Conductors},
author = {Jackson, Grayson L. and Perroni, Dominic V. and Mahanthappa, Mahesh K.},
abstractNote = {Nanoporous proton-transporting media are critical components in fuel cells and other electrochemical devices, yet general molecular design criteria for new materials with enhanced performance remain obscure. Aqueous lyotropic liquid crystals (LLCs) comprise a platform for detailed studies of the molecular-level features governing proton transport in monodisperse, water-filled nanopores lined with well-defined chemical functionalities. Here, we report new alkylsulfonic acid LLCs that exhibit H+ conductivities as high as σ = 380 mS/cm at 80°C, which rival those of more acidic, perfluorinated polymers, thus demonstrating that the acidity of the pore functionality is not the sole determinant of proton transport. Direct experimental comparisons of LLCs with convex and concave nanopores of similar dimensions indicate that H+ conductivities therein sensitively depend on the hydration state of the acid functionalities and the pore curvature. These experiments suggest that judicious manipulation of pore curvature provides a new means for optimizing the activities of proton-exchange membranes and nanoporous solid acid catalysts.},
doi = {10.1021/acs.jpcb.7b06366},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 40,
volume = 121,
place = {United States},
year = {2017},
month = {10}
}