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      Ambipolar zinc-polyiodide electrolyte for a high-energy density aqueous redox flow battery

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          Abstract

          Redox flow batteries are receiving wide attention for electrochemical energy storage due to their unique architecture and advantages, but progress has so far been limited by their low energy density (~25 Wh l −1). Here we report a high-energy density aqueous zinc-polyiodide flow battery. Using the highly soluble iodide/triiodide redox couple, a discharge energy density of 167 Wh l −1 is demonstrated with a near-neutral 5.0 M ZnI 2 electrolyte. Nuclear magnetic resonance study and density functional theory-based simulation along with flow test data indicate that the addition of an alcohol (ethanol) induces ligand formation between oxygen on the hydroxyl group and the zinc ions, which expands the stable electrolyte temperature window to from −20 to 50 °C, while ameliorating the zinc dendrite. With the high-energy density and its benign nature free from strong acids and corrosive components, zinc-polyiodide flow battery is a promising candidate for various energy storage applications.

          Abstract

          Conventional redox flow batteries have low energy densities. Here the authors present an aqueous redox flow battery with an ambipolar and bifunctional zinc-polyiodide electrolyte, which exhibits an energy density approaching to that of lithium ion batteries.

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          Chemistry with ADF

          G. te Velde, F. M. Bickelhaupt, E J Baerends … (2001)
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            Redox flow batteries: a review

            Jeffrey T. Gostick, Adam Z Weber, Matthew M. Mench … (2011)
            Article 0 comments Cited 315 times – based on 0 reviews     Review now
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              Characteristics of the iodide/triiodide redox mediator in dye-sensitized solar cells.

              Gerrit Boschloo, Anders Hagfeldt (2009)
              Dye-sensitized solar cells (DSCs) have gained widespread interest because of their potential for low-cost solar energy conversion. Currently, the certified record efficiency of these solar cells is 11.1%, and measurements of their durability and stability suggest lifetimes exceeding 10 years under operational conditions. The DSC is a photoelectrochemical system: a monolayer of sensitizing dye is adsorbed onto a mesoporous TiO(2) electrode, and the electrode is sandwiched together with a counter electrode. An electrolyte containing a redox couple fills the gap between the electrodes. The redox couple is a key component of the DSC. The reduced part of the couple regenerates the photo-oxidized dye. The formed oxidized species diffuses to the counter electrode, where it is reduced. The photovoltage of the device depends on the redox couple because it sets the electrochemical potential at the counter electrode. The redox couple also affects the electrochemical potential of the TiO(2) electrode through the recombination kinetics between electrons in TiO(2) and oxidized redox species. This Account focuses on the special properties of the iodide/triiodide (I(-)/I(3)(-)) redox couple in dye-sensitized solar cells. It has been the preferred redox couple since the beginning of DSC development and still yields the most stable and efficient DSCs. Overall, the iodide/triiodide couple has good solubility, does not absorb too much light, has a suitable redox potential, and provides rapid dye regeneration. But what distinguishes I(-)/I(3)(-) from most redox mediators is the very slow recombination kinetics between electrons in TiO(2) and the oxidized part of the redox couple, triiodide. Certain dyes adsorbed at TiO(2) catalyze this recombination reaction, presumably by binding iodine or triiodide. The standard potential of the iodide/triiodide redox couple is 0.35 V (versus the normal hydrogen electrode, NHE), and the oxidation potential of the standard DSC-sensitizer (Ru(dcbpy)(2)(NCS)(2)) is 1.1 V. The driving force for reduction of oxidized dye is therefore as large as 0.75 V. This process leads to the largest internal potential loss in DSC devices. We expect that overall efficiencies above 15% might be achieved if half of this internal potential loss could be gained. The regeneration of oxidized dye with iodide leads to the formation of the diiodide radical (I(2)(-*)). The redox potential of the I(2)(-*)/I(-) couple must therefore be considered when determining the actual driving force for dye regeneration. The formed I(2)(-*) disproportionates to I(3)(-) and I(-), which leads to a large loss in potential energy.
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                Author and article information

                Journal
                Journal ID (nlm-ta): Nat Commun
                Journal ID (iso-abbrev): Nat Commun
                Title: Nature Communications
                Publisher: Nature Pub. Group
                ISSN (Electronic): 2041-1723
                Publication date (Electronic): 24 February 2015
                Volume: 6
                Electronic Location Identifier: 6303
                Affiliations
                [1 ]Energy and Environment Directorate, Pacific Northwest National Laboratory , PO Box 999, Richland, Washington 99352, USA
                Author notes
                Article
                Publisher Item ID: ncomms7303
                DOI: 10.1038/ncomms7303
                PMC ID: 4346617
                PubMed ID: 25709083
                SO-VID: c3828197-4e18-4015-ac74-0f5741404b1f
                Copyright © Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.
                License:

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                Date received : 24 October 2014
                Date accepted : 14 January 2015
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