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      Proton Conduction in a Phosphonate-Based Metal–Organic Framework Mediated by Intrinsic “Free Diffusion inside a Sphere”

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          Abstract

          Understanding the molecular mechanism of proton conduction is crucial for the design of new materials with improved conductivity. Quasi-elastic neutron scattering (QENS) has been used to probe the mechanism of proton diffusion within a new phosphonate-based metal–organic framework (MOF) material, MFM-500(Ni). QENS suggests that the proton conductivity (4.5 × 10 –4 S/cm at 98% relative humidity and 25 °C) of MFM-500(Ni) is mediated by intrinsic “free diffusion inside a sphere”, representing the first example of such a mechanism observed in MOFs.

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          MOFs as proton conductors--challenges and opportunities.

          Padmini Ramaswamy, Norman Wong, George Shimizu (2014)
          Proton conducting materials have garnered immense attention for their role as electrolytes in fuel cells. Metal Organic Frameworks (MOFs) and coordination polymers have recently been investigated as possible candidates for proton-conducting applications. Their crystallinity, chemically functionalizable pores and options for systematic structural variation are some of the factors that allow for the targeted design of better proton conductors operating over a wide variety of temperatures and/or humidity conditions. This review will examine selected examples from this nascent field, and will focus on the design and synthesis of proton conducting MOFs, their properties and conditions under which they operate.
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            Ion conductivity and transport by porous coordination polymers and metal-organic frameworks.

            Satoshi Horike, Daiki Umeyama, Susumu Kitagawa (2013)
            Ion conduction and transport in solids are both interesting and useful and are found in widely distinct materials, from those in battery-related technologies to those in biological systems. Scientists have approached the synthesis of ion-conductive compounds in a variety of ways, in the areas of organic and inorganic chemistry. Recently, based on their ion-conducting behavior, porous coordination polymers (PCPs) and metal-organic frameworks (MOFs) have been recognized for their easy design and the dynamic behavior of the ionic components in the structures. These PCP/MOFs consist of metal ions (or clusters) and organic ligands structured via coordination bonds. They could have highly concentrated mobile ions with dynamic behavior, and their characteristics have inspired the design of a new class of ion conductors and transporters. In this Account, we describe the state-of-the-art of studies of ion conductivity by PCP/MOFs and nonporous coordination polymers (CPs) and offer future perspectives. PCP/MOF structures tend to have high hydrophilicity and guest-accessible voids, and scientists have reported many water-mediated proton (H(+)) conductivities. Chemical modification of organic ligands can change the hydrated H(+) conductivity over a wide range. On the other hand, the designable structures also permit water-free (anhydrous) H(+) conductivity. The incorporation of protic guests such as imidazole and 1,2,4-triazole into the microchannels of PCP/MOFs promotes the dynamic motion of guest molecules, resulting in high H(+) conduction without water. Not only the host-guest systems, but the embedding of protic organic groups on CPs also results in inherent H(+) conductivity. We have observed high H(+) conductivities under anhydrous conditions and in the intermediate temperature region of organic and inorganic conductors. The keys to successful construction are highly mobile ionic species and appropriate intervals of ion-hopping sites in the structures. Lithium (Li(+)) and other ions can also be transported. If we can optimize the crystal structures, this could offer further improvements in terms of both conductivity and the working temperature range. Another useful characteristic of PCP/MOFs is their wide application to materials fabrication. We can easily prepare heterodomain crystal systems, such as core-shell or solid solution. Other anisotropic morphologies (thin film, nanocrystal, nanorod, etc.,) are also possible, with retention of the ion conductivity. The flexible nature also lets us design morphology-dependent ion-conduction behaviors that we cannot observe in the bulk state. We propose (1) multivalent ion and anion conductions with the aid of redox activity and defects in structures, (2) control of ion transport behavior by applying external stimuli, (3) anomalous conductivity at the hetero-solid-solid interface, and (4) unidirectional ion transport as in the ion channels in membrane proteins. In the future, scientists may use coordination polymers not only to achieve higher conductivity but also to control ion behavior, which will open new avenues in solid-state ionics.
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              One-dimensional imidazole aggregate in aluminium porous coordination polymers with high proton conductivity.

              Sareeya Bureekaew, M Higuchi, M Mizuno … (2009)
              The development of anhydrous proton-conductive materials operating at temperatures above 80 degrees C is a challenge that needs to be met for practical applications. Herein, we propose the new idea of encapsulation of a proton-carrier molecule--imidazole in this work--in aluminium porous coordination polymers for the creation of a hybridized proton conductor under anhydrous conditions. Tuning of the host-guest interaction can generate a good proton-conducting path at temperatures above 100 degrees C. The dynamics of the adsorbed imidazole strongly affect the conductivity determined by (2)H solid-state NMR. Isotope measurements of conductivity using imidazole-d4 showed that the proton-hopping mechanism was dominant for the conducting path. This work suggests that the combination of guest molecules and a variety of microporous frameworks would afford highly mobile proton carriers in solids and gives an idea for designing a new type of proton conductor, particularly for high-temperature and anhydrous conditions.
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                Author and article information

                Journal
                Journal ID (nlm-ta): J Am Chem Soc
                Journal ID (iso-abbrev): J. Am. Chem. Soc
                Journal ID (publisher-id): ja
                Journal ID (coden): jacsat
                Title: Journal of the American Chemical Society
                Publisher: American Chemical Society
                ISSN (Print): 0002-7863
                ISSN (Electronic): 1520-5126
                Publication date (Electronic): 16 May 2016
                Publication date (Print): 25 May 2016
                Volume: 138
                Issue: 20
                Pages: 6352-6355
                Affiliations
                [† ]School of Chemistry, University of Manchester , Oxford Road, Manchester M13 9PL, U.K.
                [‡ ]School of Chemistry, University of Nottingham , University Park, Nottingham NG7 2RD, U.K.
                [§ ]Diamond Light Source , Harwell Science and Innovation Campus, Oxfordshire OX11 0DE, U.K.
                [⊥ ]ISIS Pulsed Neutron and Muon Source, STFC Rutherford Appleton Laboratory , Chilton, Oxfordshire OX11 0QX, U.K.
                [∥ ]School of Chemistry, Cardiff University , Cardiff CF10 3XQ, U.K.
                [# ]Department of Mechanical, Materials and Manufacturing Engineering, University of Nottingham , University Park, Nottingham NG7 2RD, U.K.
                Author notes
                Article
                DOI: 10.1021/jacs.6b02194
                PMC ID: 4882730
                PubMed ID: 27182787
                SO-VID: ed822b92-6539-4eee-8c50-e3b2f285460d
                Copyright © Copyright © 2016 American Chemical Society
                License:

                This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.

                History
                Date received : 28 February 2016
                Categories
                Subject: Communication
                Custom metadata
                document-id-old-9 ja6b02194
                document-id-new-14 ja-2016-02194w
                ccc-price

                ScienceOpen disciplines: Chemistry
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                ScienceOpen disciplines: Chemistry

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