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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\u2010covalent organic frameworks (POCOF) via one\u2010pot solvothermal strategy between an amino\u2010functionalized Anderson\u2010type POM and a trialdehyde\u2010based 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\u20101,3,5\u2010tricarbaldehyde allowing to exploit for the first time in POCOFs the keto\u2010enol tautomerization as additional feature to impart greater chemical stability to the COFs and enhanced properties leading to large specific surface area (347\u2005m<jats:sup>2<\/jats:sup>\/g) and superior electrochemical performance of the POCOF\u20101 electrodes, when compared with POCOF\u20102 electrodes that possess only imine\u2010type linkage and with pristine POM electrodes. Specifically, POCOF\u20101 electrodes display remarkable specific, areal, and volumetric capacitance (125\u2005F\/g, 248\u2005mF\/cm<jats:sup>2<\/jats:sup> and 41.9\u2005mF\/cm<jats:sup>3<\/jats:sup>, respectively) at a current density of 0.5\u2005A\/g, a maximum energy density (56.2\u2005Wh\/kg), a maximum power density (3.7\u2005kW\/kg) and an outstanding cyclability (90\u2009% capacitance retention after 5000 cycles).<\/jats:p>","DOI":"10.1002\/anie.202305239","type":"journal-article","created":{"date-parts":[[2023,6,19]],"date-time":"2023-06-19T11:54:12Z","timestamp":1687175652000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":51,"title":["New Anderson\u2010Based Polyoxometalate Covalent Organic Frameworks as Electrodes for Energy Storage Boosted Through Keto\u2010Enol Tautomerization"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0136-6667","authenticated-orcid":false,"given":"Dawid","family":"Pakulski","sequence":"first","affiliation":[{"name":"Adam Mickiewicz University Foundation Pozna\u0144 Science and Technology Park  Rubie\u017c 46 61-612 Pozna\u0144 Poland"},{"name":"Centre for Advanced Technologies Adam Mickiewicz University  Uniwersytetu Pozna\u0144skiego 10 61-614 Pozna\u0144 Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3930-8489","authenticated-orcid":false,"given":"Adam","family":"Gorczy\u0144ski","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Adam Mickiewicz University  Uniwersytetu Pozna\u0144skiego 8 61-614 Pozna\u0144 Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8517-3768","authenticated-orcid":false,"given":"Daria","family":"Brykczy\u0144ska","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Adam Mickiewicz University  Uniwersytetu Pozna\u0144skiego 8 61-614 Pozna\u0144 Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3235-0545","authenticated-orcid":false,"given":"Ver\u00f3nica","family":"Montes\u2010Garc\u00eda","sequence":"additional","affiliation":[{"name":"Universit\u00e9 de Strasbourg CNRS Institut de Science et d'Ing\u00e9nierie Supramol\u00e9culaires  8 all\u00e9e Gaspard Monge 67000 Strasbourg France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3118-4143","authenticated-orcid":false,"given":"W\u0142odzimierz","family":"Czepa","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Adam Mickiewicz University  Uniwersytetu Pozna\u0144skiego 8 61-614 Pozna\u0144 Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1877-9545","authenticated-orcid":false,"given":"Iwona","family":"Janica","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Adam Mickiewicz University  Uniwersytetu Pozna\u0144skiego 8 61-614 Pozna\u0144 Poland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9950-1221","authenticated-orcid":false,"given":"Micha\u0142","family":"Bielejewski","sequence":"additional","affiliation":[{"name":"Institute of Molecular Physics Polish Academy of Sciences  M. 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