New Anderson-Based Polyoxometalate Covalent Organic Frameworks as Electrodes for Energy Storage Boosted Through Keto-Enol Tautomerization |
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Authors: | Dr. Dawid Pakulski Dr. Adam Gorczyński Daria Brykczyńska Dr. Verónica Montes-García Włodzimierz Czepa Dr. Iwona Janica Dr. Michał Bielejewski Prof. Maciej Kubicki Prof. Violetta Patroniak Prof. Paolo Samorì Dr. Artur Ciesielski |
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Affiliation: | 1. Adam Mickiewicz University Foundation, Poznań Science and Technology Park, Rubież 46, 61-612 Poznań, Poland;2. Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland;3. Université de Strasbourg, CNRS, Institut de Science et d'Ingénierie Supramoléculaires, 8 allée Gaspard Monge, 67000 Strasbourg, France;4. Institute of Molecular Physics, Polish Academy of Sciences, M. Smoluchowskiego 17, 60-179 Poznań, Poland;5. Centre for Advanced Technologies, Adam Mickiewicz University, Uniwersytetu Poznańskiego 10, 61-614 Poznań, Poland |
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Abstract: | The unique electrochemical properties of polyoxometalates (POMs) render them ideal components for the fabrication of next-generation high-performance energy storage systems. However, their practical applications have been hindered by their high solubility in common electrolytes. This problem can be overcome by the effective hybridization of POMs with other materials. Here we present the design and synthesis of two novel polyoxometalate-covalent organic frameworks (POCOF) via one-pot solvothermal strategy between an amino-functionalized Anderson-type POM and a trialdehyde-based building unit. We show that structural and functional complexity can be enriched by adding hydroxyl groups in the 2,4,6 position to the benzene-1,3,5-tricarbaldehyde allowing to exploit for the first time in POCOFs the keto-enol tautomerization as additional feature to impart greater chemical stability to the COFs and enhanced properties leading to large specific surface area (347 m2/g) and superior electrochemical performance of the POCOF-1 electrodes, when compared with POCOF-2 electrodes that possess only imine-type linkage and with pristine POM electrodes. Specifically, POCOF-1 electrodes display remarkable specific, areal, and volumetric capacitance (125 F/g, 248 mF/cm2 and 41.9 mF/cm3, respectively) at a current density of 0.5 A/g, a maximum energy density (56.2 Wh/kg), a maximum power density (3.7 kW/kg) and an outstanding cyclability (90 % capacitance retention after 5000 cycles). |
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Keywords: | Covalent Organic Framework Energy Storage Devices Functional Porous Materials Hybrid Materials Polyoxometalate |
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