{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,22]],"date-time":"2026-09-22T13:04:32Z","timestamp":1790082272135,"version":"4.0.1"},"reference-count":69,"publisher":"American Chemical Society (ACS)","issue":"18","license":[{"start":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T00:00:00Z","timestamp":1789344000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/100000078","name":"Division of Materials Research","doi-asserted-by":"publisher","award":["2119672"],"award-info":[{"award-number":["2119672"]}],"id":[{"id":"10.13039\/100000078","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000078","name":"Division of Materials Research","doi-asserted-by":"publisher","award":["2119673"],"award-info":[{"award-number":["2119673"]}],"id":[{"id":"10.13039\/100000078","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000928","name":"Welch Foundation","doi-asserted-by":"publisher","award":["A-2070"],"award-info":[{"award-number":["A-2070"]}],"id":[{"id":"10.13039\/100000928","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,22]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Non-conjugated redox-active polymers (NC-RAPs) in the dissolved state are important for future energy applications such as redox flow batteries. However, there remains a knowledge gap in understanding factors that strongly influence the redox kinetics and mechanisms of NC-RAPs. Here, we determine how concentration and backbone structure of phthalimide-based NC-RAPs influence the solution-state electrochemical activity, as described by the apparent diffusion coefficient (Dapp) and the homogeneous (kex,app) and heterogeneous (k0) rate constants. Three phthalimide-containing polymers with epichlorohydrin, methacrylate, and vinylbenzene backbones are compared experimentally and computationally. As polymer concentration increases from the dilute to the semidilute regimes, the diffusion and kinetics slow down. Interestingly, the polymer backbone does not strongly influence the redox kinetics of these phthalimide-based polymers. In total, these results show that, above the overlap concentration, single-file diffusion and interdependent flux of redox species lead to slower diffusion and kinetics. These findings provide mechanistic insights into the future molecular design of NC-RAPs in the dissolved state, enabling energy storage systems such as redox flow batteries with improved kinetics.<\/jats:p>","DOI":"10.1021\/acs.chemmater.6c01965","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T14:01:30Z","timestamp":1789394490000},"page":"9530-9541","source":"Crossref","is-referenced-by-count":0,"title":["Deciphering\nConcentration and Backbone Identity Effects\non the Redox Properties of Phthalimide-Based Polymers"],"prefix":"10.1021","volume":"38","author":[{"given":"Khirabdhi Tannaya","family":"Mohanty","sequence":"first","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8189-1073","authenticated-orcid":true,"given":"Sheila","family":"Keating","sequence":"additional","affiliation":[{"name":"University of Chicago , , , ,","place":["Chicago, Illinois, United States, 60637"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kha","family":"Trinh","sequence":"additional","affiliation":[{"name":"University of Chicago , , , ,","place":["Chicago, Illinois, United States, 60637"]},{"name":"New York University , , , ,","place":["Brooklyn, New York, United States, 11201"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1948-5311","authenticated-orcid":true,"given":"Riccardo","family":"Alessandri","sequence":"additional","affiliation":[{"name":"KU Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8680-6667","authenticated-orcid":true,"given":"Daniel P.","family":"Tabor","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77840"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8176-0594","authenticated-orcid":true,"given":"Stuart J.","family":"Rowan","sequence":"additional","affiliation":[{"name":"University of Chicago , , , ,","place":["Chicago, Illinois, United States, 60637"]},{"name":"University of Chicago , , , ,","place":["Chicago, Illinois, United States, 60637"]},{"name":"New York University , , , ,","place":["New York, New York, United States, 10012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juan J.","family":"de Pablo","sequence":"additional","affiliation":[{"name":"University of Chicago , , , ,","place":["Chicago, Illinois, United States, 60637"]},{"name":"New York University , , , ,","place":["Brooklyn, New York, United States, 11201"]},{"name":"New York University , , , ,","place":["New York, New York, United States, 10012"]},{"name":"New York University , , , ,","place":["New York, New York, United States, 10012"]},{"name":"Argonne National Laboratory , , , ,","place":["Lemont, Illinois, United States, 60439"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2613-6016","authenticated-orcid":true,"given":"Jodie L.","family":"Lutkenhaus","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]},{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77840"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,14]]},"reference":[{"issue":"14","key":"2026092208102897800_cit1","doi-asserted-by":"publisher","first-page":"187","DOI":"10.1146\/annurev-chembioeng-092220-111121","article-title":"Nonconjugated\nRedox-Active Polymers: Electron Transfer\nMechanisms, Energy Storage, and Chemical Versatility","volume":"14","author":"Ma","year":"2023","journal-title":"Annu. Rev. Chem. Biomol. Eng."},{"key":"2026092208102897800_cit2","doi-asserted-by":"crossref","DOI":"10.1039\/9781788019743-00288","article-title":"Redox Polymers\nfor All-organic Batteries","volume-title":"Redox Polymers\nfor Energy and Nanomedicine","author":"Goujon","year":"2020"},{"key":"2026092208102897800_cit3","doi-asserted-by":"publisher","first-page":"101449","DOI":"10.1016\/j.progpolymsci.2021.101449","article-title":"Organic batteries\nbased on just redox polymers","volume":"122","author":"Goujon","year":"2021","journal-title":"Prog. Polym. Sci."},{"issue":"4","key":"2026092208102897800_cit4","doi-asserted-by":"publisher","first-page":"739","DOI":"10.1016\/j.joule.2017.08.018","article-title":"Redox-Active\nPolymers for Energy\nStorage Nanoarchitectonics","volume":"1","author":"Kim","year":"2017","journal-title":"Joule"},{"issue":"10","key":"2026092208102897800_cit5","doi-asserted-by":"publisher","first-page":"3450","DOI":"10.1021\/acsenergylett.1c01625","article-title":"Redox-Active\nPolymers Designed for the Circular Economy of Energy Storage Devices","volume":"6","author":"Tan","year":"2021","journal-title":"ACS Energy Lett."},{"issue":"16","key":"2026092208102897800_cit6","doi-asserted-by":"publisher","first-page":"8783","DOI":"10.1039\/D3TA00289F","article-title":"Water-coupled\nmonovalent and divalent\nion transport in polyviologen networks","volume":"11","author":"Easley","year":"2023","journal-title":"J. Mater.\nChem. 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Chem."},{"issue":"7576","key":"2026092208102897800_cit10","doi-asserted-by":"publisher","first-page":"78","DOI":"10.1038\/nature15746","article-title":"An aqueous, polymer-based\nredox-flow battery using non-corrosive, safe, and low-cost materials","volume":"527","author":"Janoschka","year":"2015","journal-title":"Nature"},{"issue":"12","key":"2026092208102897800_cit11","doi-asserted-by":"publisher","first-page":"10692","DOI":"10.1021\/acsami.7b00403","article-title":"Quantifying\nTEMPO Redox Polymer Charge\nTransport toward the Organic Radical Battery","volume":"9","author":"Karlsson","year":"2017","journal-title":"ACS Appl. Mater. 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Mater."},{"issue":"9","key":"2026092208102897800_cit14","doi-asserted-by":"publisher","first-page":"2232","DOI":"10.1002\/cssc.201903168","article-title":"Phenothiazine-Functionalized\nPoly (norbornene) s as High-Rate Cathode\nMaterials for Organic Batteries","volume":"13","author":"Otteny","year":"2020","journal-title":"ChemSuschem"},{"issue":"8","key":"2026092208102897800_cit15","doi-asserted-by":"publisher","first-page":"7622","DOI":"10.1021\/acsaem.1c00917","article-title":"Bridging the gap between small molecular \u03c0-interactions and\ntheir effect on phenothiazine-based redox polymers in organic batteries","volume":"4","author":"Otteny","year":"2021","journal-title":"ACS Appl. Energy Mater."},{"issue":"11","key":"2026092208102897800_cit16","doi-asserted-by":"publisher","first-page":"5295","DOI":"10.1039\/c3cp54624a","article-title":"An inter-tangled\nnetwork of redox-active and conducting polymers as a cathode for ultrafast\nrechargeable batteries","volume":"16","author":"Kim","year":"2014","journal-title":"Phys. Chem. Chem. Phys."},{"issue":"1","key":"2026092208102897800_cit17","doi-asserted-by":"publisher","first-page":"145","DOI":"10.1002\/(SICI)1097-4628(19991003)74:1&lt;145:AID-APP18&gt;3.0.CO;2-C","article-title":"Characteristics\nof aqueous polycarbazole\nbatteries","volume":"74","author":"Saraswathi","year":"1999","journal-title":"J. Appl. Polym. 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Adv."},{"issue":"5","key":"2026092208102897800_cit21","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202301143","article-title":"Anion-Rocking\nChair Batteries with Tuneable Voltage using Viologen-and Phenothiazine\nPolymer-based Electrodes","volume":"17","author":"Bhosale","year":"2024","journal-title":"ChemSuschem"},{"issue":"11","key":"2026092208102897800_cit22","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202500092","article-title":"Upcycling Commodity Styrofoam into\nRedox Polymer-based Electrodes","volume":"18","author":"Biying","year":"2025","journal-title":"ChemSuschem"},{"issue":"103","key":"2026092208102897800_cit23","doi-asserted-by":"publisher","first-page":"85035","DOI":"10.1039\/C5RA16839B","article-title":"RAFT polymerization\nof an alkoxyamine bearing acrylate, towards a well-defined redox active\npolyacrylate","volume":"5","author":"Aqil","year":"2015","journal-title":"RSC Adv."},{"issue":"2","key":"2026092208102897800_cit24","doi-asserted-by":"publisher","first-page":"188","DOI":"10.1021\/acsapm.8b00074","article-title":"Hydrophilic\nOrganic Redox-Active\nPolymer Nanoparticles for Higher Energy Density Flow Batteries","volume":"1","author":"Hatakeyama-Sato","year":"2019","journal-title":"ACS Appl. Polym. Mater."},{"issue":"48","key":"2026092208102897800_cit25","doi-asserted-by":"publisher","first-page":"14680","DOI":"10.1021\/la504055m","article-title":"Deformation\nof redox-active polymer gel based on polysiloxane backbone and bis\n(benzodithiolyl) bithienyl scaffold","volume":"30","author":"Ohtake","year":"2014","journal-title":"Langmuir"},{"key":"2026092208102897800_cit26","volume-title":"Polymer Physics","author":"Rubinstein","year":"2023"},{"key":"2026092208102897800_cit27","doi-asserted-by":"crossref","DOI":"10.1002\/0471224510","volume-title":"Polymer Solutions: An\nIntroduction to Physical Properties","author":"Teraoka","year":"2002"},{"key":"2026092208102897800_cit28","doi-asserted-by":"crossref","DOI":"10.1201\/9781439894156","volume-title":"Introduction to Polymers","author":"Young","year":"2011","edition":"Third"},{"issue":"11","key":"2026092208102897800_cit29","doi-asserted-by":"publisher","first-page":"2649","DOI":"10.1021\/acs.accounts.6b00341","article-title":"Redox Active\nPolymers as Soluble Nanomaterials for Energy Storage","volume":"49","author":"Burgess","year":"2016","journal-title":"Acc. Chem. Res."},{"issue":"6","key":"2026092208102897800_cit30","doi-asserted-by":"publisher","first-page":"2093","DOI":"10.1021\/jacs.7b08353","article-title":"Modulation\nof the Electrochemical Reactivity of Solubilized Redox Active Polymers\nvia Polyelectrolyte Dynamics","volume":"140","author":"Burgess","year":"2018","journal-title":"J. Am. Chem. Soc."},{"issue":"20","key":"2026092208102897800_cit31","doi-asserted-by":"publisher","first-page":"7362","DOI":"10.1021\/acs.chemmater.6b02825","article-title":"Impact of\nbackbone tether length and structure on the electrochemical performance\nof viologen redox active polymers","volume":"28","author":"Burgess","year":"2016","journal-title":"Chem. Mater."},{"issue":"19","key":"2026092208102897800_cit32","doi-asserted-by":"publisher","first-page":"8357","DOI":"10.1039\/D5SC00051C","article-title":"Redox-active polymer-grafted particles as redox mediators\nfor enhanced charge transport in solution-state electrochemical systems","volume":"16","author":"Avais","year":"2025","journal-title":"Chem. Sci."},{"issue":"12","key":"2026092208102897800_cit33","doi-asserted-by":"publisher","first-page":"2814","DOI":"10.1016\/j.chempr.2018.08.024","article-title":"Highly concentrated\nphthalimide-based anolytes for organic redox flow batteries with enhanced\nreversibility","volume":"4","author":"Zhang","year":"2018","journal-title":"Chem"},{"issue":"15","key":"2026092208102897800_cit34","doi-asserted-by":"publisher","first-page":"8273","DOI":"10.1039\/D2TA00743F","article-title":"Discovery of lead\nlow-potential radical candidates\nfor organic radical polymer batteries with machine-learning-assisted\nvirtual screening","volume":"10","author":"Li","year":"2022","journal-title":"J. Mater. Chem. A"},{"issue":"17","key":"2026092208102897800_cit35","doi-asserted-by":"publisher","first-page":"4264","DOI":"10.1021\/ja00746a029","article-title":"Cathodic reduction\nof phthalimide systems in nonaqueous\nsolutions","volume":"93","author":"Leedy","year":"1971","journal-title":"J. Am. Chem. 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Chem."},{"issue":"6","key":"2026092208102897800_cit39","doi-asserted-by":"publisher","first-page":"2300","DOI":"10.1021\/jacsau.4c00276","article-title":"Ionic,\nand Electronic Properties of Solid-State Phthalimide-Containing Polymers\nfor All-Organic Batteries","volume":"4","author":"Alessandri","year":"2024","journal-title":"JACS Au"},{"issue":"10","key":"2026092208102897800_cit40","doi-asserted-by":"publisher","first-page":"3574","DOI":"10.1021\/acs.macromol.3c00141","article-title":"Prediction of electronic\nproperties of radical-containing\npolymers at coarse-grained resolutions","volume":"56","author":"Alessandri","year":"2023","journal-title":"Macromolecules"},{"issue":"4","key":"2026092208102897800_cit41","doi-asserted-by":"publisher","first-page":"1700267","DOI":"10.1002\/macp.201700267","article-title":"Synthesis\nand Characterization of a Phthalimide-Containing Redox-Active Polymer\nfor High-Voltage Polymer-Based Redox-Flow Batteries","volume":"219","author":"Winsberg","year":"2018","journal-title":"Macromol. Chem. Phys."},{"issue":"38","key":"2026092208102897800_cit42","doi-asserted-by":"publisher","first-page":"45345","DOI":"10.1021\/acsami.3c11812","article-title":"Influence of backbone on the performance of pendant\npolymer electrode materials in Li-ion batteries","volume":"15","author":"Grignon","year":"2023","journal-title":"ACS Appl. Mater. Interfaces"},{"issue":"10","key":"2026092208102897800_cit43","doi-asserted-by":"publisher","first-page":"3539","DOI":"10.1021\/acs.macromol.8b00574","article-title":"Effect of\nthe backbone tether on the electrochemical properties of soluble cyclopropenium\nredox-active polymers","volume":"51","author":"Montoto","year":"2018","journal-title":"Macromolecules"},{"issue":"21","key":"2026092208102897800_cit44","doi-asserted-by":"publisher","first-page":"9346","DOI":"10.1021\/acs.chemmater.3c02148","article-title":"Charge\ntransfer in spatially defined organic radical polymers","volume":"35","author":"Ma","year":"2023","journal-title":"Chem. 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Chem.\nSoc."},{"issue":"18","key":"2026092208102897800_cit47","doi-asserted-by":"publisher","first-page":"7658","DOI":"10.1021\/acs.macromol.0c01672","article-title":"Mechanisms of diffusive charge transport in redox-active\npolymer solutions","volume":"53","author":"Bello","year":"2020","journal-title":"Macromolecules"},{"key":"2026092208102897800_cit48","doi-asserted-by":"publisher","first-page":"106779","DOI":"10.1016\/j.orgel.2023.106779","article-title":"Overlap concentration\ngenerates optimum device performance for DPP-based conjugated polymers","volume":"117","author":"Venkatesh","year":"2023","journal-title":"Org. 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Interfacial Electrochem."},{"key":"2026092208102897800_cit51","volume-title":"Electrochemical methods:\nfundamentals and applications","author":"Faulkner","year":"2000"},{"issue":"2","key":"2026092208102897800_cit52","doi-asserted-by":"publisher","first-page":"371","DOI":"10.1016\/0022-0728(82)85134-6","article-title":"Apparent\ndiffusion coefficients for electroactive anions\nin coatings of protonated poly (4-vinylpiridine) on graphite electrodes","volume":"139","author":"Oyama","year":"1982","journal-title":"J.Electroanalytical Chem. Interfacial Electrochem."},{"issue":"18","key":"2026092208102897800_cit53","doi-asserted-by":"publisher","first-page":"3818","DOI":"10.1021\/j100264a010","article-title":"Charge-transport rates in nafion coatings on electrodes.\nSurprisingly disparate diffusion coefficients for a single molecule\ncontaining two electroactive centers","volume":"89","author":"Tsou","year":"1985","journal-title":"J. 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