{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T15:04:31Z","timestamp":1786719871577,"version":"build-2736575974"},"reference-count":49,"publisher":"American Chemical Society (ACS)","issue":"15","license":[{"start":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T00:00:00Z","timestamp":1785801600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"name":"European Research Council (ERC), European Union\u2019s Horizon 2020 research and innovation program","award":["864982"],"award-info":[{"award-number":["864982"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,14]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Polyelectrolyte complexes (PECs), formed by electrostatic association of oppositely charged polyelectrolytes, are promising low-environmental-impact materials. However, their extreme brittleness in the absence of water and a general lack of stimuli-responsive functionality severely limit practical applications. Here, we introduce a strategy to overcome both limitations by designing liquid crystalline polyelectrolyte complexes (LCPECs). Main-chain liquid crystalline (LC) polyanions with systematically varied charge densities and neutral flexible domains are first synthesized via a facile one-pot two-step polymerization combining Michael addition and thiol\u2013ene chemistry. The LC polyanions are then complexed with poly(diallyldimethylammonium chloride) (PDADMAC) to form LCPECs with tunable properties. X-ray scattering reveals a fractal-like network with nanoscale phase separation between electrostatically associated and neutral flexible domains, alongside nematic ordering of the mesogens. Increasing the neutral monomer content lowers the glass transition temperature from 58 \u00b0C to \u221210 \u00b0C and transforms the mechanical response from stiff and brittle to soft and highly stretchable, achieving an elongation of 1160%, far exceeding the stretchability of any previously reported water- and salt-free PEC. Rheological analysis shows that higher charge density raises both moduli and delays chain relaxation, confirming that electrostatic interactions function as tunable physical cross-links. Uniaxial stretching induces macroscopic mesogen alignment, enabling reversible thermal actuation with 20% dimensional change upon cycling across the LC\u2013isotropic transition. Furthermore, well-defined mesh structures are successfully prepared by melt electrowriting, demonstrating the processability of these materials through advanced additive manufacturing. This work establishes tuning of ionic cross-link density and backbone flexibility as a general strategy for transforming inherently brittle PECs into mechanically robust, stimuli-responsive, and processable materials.<\/jats:p>","DOI":"10.1021\/acsapm.6c01534","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T18:02:50Z","timestamp":1785866570000},"page":"12440-12448","source":"Crossref","is-referenced-by-count":0,"title":["Stretchable Water-Free\nLiquid Crystalline Polyelectrolyte\nComplexes"],"prefix":"10.1021","volume":"8","author":[{"given":"Xiaohong","family":"Liu","sequence":"first","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]},{"name":"KINGFA Sci. & Tech. Co. Ltd. , No. 33, Kefeng Road, Science Town , ,","place":["Guangzhou, China, 510663"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1541-6784","authenticated-orcid":true,"given":"Yuxuan","family":"Zhang","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1201-5042","authenticated-orcid":true,"given":"Xixi","family":"Wu","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]},{"name":"Huzhou University , , No. 759, Erhuan East Road , ,","place":["Huzhou, China, 313000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Li","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1650-8429","authenticated-orcid":true,"given":"Daniele","family":"Parisi","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4903-3159","authenticated-orcid":true,"given":"Giuseppe","family":"Portale","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0520-4534","authenticated-orcid":true,"given":"Marleen","family":"Kamperman","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8147-2637","authenticated-orcid":true,"given":"Julien","family":"Es Sayed","sequence":"additional","affiliation":[{"name":"The Silesian University of Technology , , B. Krzywoustego 8 , ,","place":["Gliwice, Poland, 44-100"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,4]]},"reference":[{"issue":"15","key":"2026081410141975900_cit1","doi-asserted-by":"publisher","first-page":"2420","DOI":"10.1002\/adma.201500176","article-title":"Saloplastics: Processing Compact Polyelectrolyte Complexes","volume":"27","author":"Schaaf","year":"2015","journal-title":"Adv. Mater."},{"issue":"9","key":"2026081410141975900_cit2","doi-asserted-by":"publisher","first-page":"1923","DOI":"10.1002\/adfm.201102787","article-title":"Extruded\nSaloplastic Polyelectrolyte\nComplexes","volume":"22","author":"Shamoun","year":"2012","journal-title":"Adv. Funct. Mater"},{"issue":"87","key":"2026081410141975900_cit3","doi-asserted-by":"publisher","first-page":"46675","DOI":"10.1039\/C4RA08733J","article-title":"Tough strained\nfibers of a polyelectrolyte complex:\npretensioned polymers","volume":"4","author":"Wang","year":"2014","journal-title":"RSC Adv."},{"issue":"7","key":"2026081410141975900_cit4","doi-asserted-by":"publisher","first-page":"2612","DOI":"10.1021\/acsapm.0c00255","article-title":"Polyelectrolyte\nComplex Membranes via Salinity Change Induced Aqueous Phase Separation","volume":"2","author":"Durmaz","year":"2020","journal-title":"ACS Appl. Polym. Mater."},{"key":"2026081410141975900_cit5","doi-asserted-by":"publisher","first-page":"110015","DOI":"10.1016\/j.eurpolymj.2020.110015","article-title":"Weak polyanion and\nstrong polycation complex based membranes: Linking aqueous phase separation\nto traditional membrane fabrication","volume":"139","author":"Durmaz","year":"2020","journal-title":"Eur. Polym.\nJ."},{"issue":"9","key":"2026081410141975900_cit6","doi-asserted-by":"publisher","first-page":"3108","DOI":"10.1021\/ma500500q","article-title":"The Polyelectrolyte\nComplex\/Coacervate Continuum","volume":"47","author":"Wang","year":"2014","journal-title":"Macromolecules"},{"key":"2026081410141975900_cit7","doi-asserted-by":"publisher","first-page":"8832","DOI":"10.1039\/D3SM01114C","article-title":"Hydrophobically modified complex\ncoacervates for designing aqueous pressure-sensitive adhesives","volume":"19","author":"van Westerveld","year":"2023","journal-title":"Soft Matter."},{"issue":"2","key":"2026081410141975900_cit8","doi-asserted-by":"publisher","first-page":"652","DOI":"10.1021\/acs.macromol.3c02352","article-title":"Effect of Polyelectrolyte Charge\nDensity on the Linear Viscoelastic Behavior and Processing of Complex\nCoacervate Adhesives","volume":"57","author":"van Westerveld","year":"2024","journal-title":"Macromolecules"},{"issue":"1","key":"2026081410141975900_cit9","doi-asserted-by":"publisher","first-page":"1273","DOI":"10.1038\/s41467-017-01249-1","article-title":"Sequence and entropy-based control\nof complex coacervates","volume":"8","author":"Chang","year":"2017","journal-title":"Nat. Commun."},{"issue":"18","key":"2026081410141975900_cit10","doi-asserted-by":"publisher","first-page":"7851","DOI":"10.1021\/acs.macromol.0c00758","article-title":"Effect\nof Polymer Chemistry on the Linear Viscoelasticity of Complex Coacervates","volume":"53","author":"Liu","year":"2020","journal-title":"Macromolecules"},{"issue":"17","key":"2026081410141975900_cit11","doi-asserted-by":"publisher","first-page":"7890","DOI":"10.1021\/acs.macromol.1c01154","article-title":"Influence\nof Nonstoichiometry on the Viscoelastic Properties of a Polyelectrolyte\nComplex","volume":"54","author":"Chen","year":"2021","journal-title":"Macromolecules"},{"issue":"18","key":"2026081410141975900_cit12","doi-asserted-by":"publisher","first-page":"7835","DOI":"10.1021\/acs.macromol.0c00999","article-title":"Effects\nof Non-Electrostatic Intermolecular Interactions on the Phase Behavior\nof pH-Sensitive Polyelectrolyte Complexes","volume":"53","author":"Li","year":"2020","journal-title":"Macromolecules"},{"issue":"14","key":"2026081410141975900_cit13","doi-asserted-by":"publisher","first-page":"6878","DOI":"10.1021\/acs.macromol.1c00703","article-title":"Polyelectrolyte Complex Coacervation\nacross a Broad Range of Charge Densities","volume":"54","author":"Neitzel","year":"2021","journal-title":"Macromolecules"},{"issue":"23","key":"2026081410141975900_cit14","doi-asserted-by":"publisher","first-page":"9149","DOI":"10.1021\/acs.macromol.9b01755","article-title":"Ion Content of Polyelectrolyte\nComplex Coacervates and the Donnan Equilibrium","volume":"52","author":"Schlenoff","year":"2019","journal-title":"Macromolecules"},{"issue":"14","key":"2026081410141975900_cit15","doi-asserted-by":"publisher","first-page":"5994","DOI":"10.1021\/acs.chemmater.0c01217","article-title":"Water and\nIon Transport through the Glass Transition in Polyelectrolyte Complexes","volume":"32","author":"Shaheen","year":"2020","journal-title":"Chem. Mater."},{"key":"2026081410141975900_cit16","doi-asserted-by":"publisher","first-page":"1074597","DOI":"10.1016\/j.porgcoat.2023.107459","article-title":"Towards ductile\nsingle-step polyelectrolyte complex\nfilms by means of plasticization","volume":"177","author":"Li","year":"2023","journal-title":"Prog. Org.\nCoat"},{"issue":"8","key":"2026081410141975900_cit17","doi-asserted-by":"publisher","first-page":"684","DOI":"10.1002\/polb.24319","article-title":"Thermal\ntransitions in and structures\nof dried polyelectrolytes and polyelectrolyte complexes","volume":"55","author":"Lyu","year":"2017","journal-title":"J Polym Sci B Polym Phys."},{"issue":"42","key":"2026081410141975900_cit18","doi-asserted-by":"publisher","first-page":"14823","DOI":"10.1021\/acs.langmuir.3c00974","article-title":"A Perspective on the Glass Transition\nand the Dynamics of Polyelectrolyte Multilayers and Complexes","volume":"39","author":"Li","year":"2023","journal-title":"Langmuir"},{"issue":"19","key":"2026081410141975900_cit19","doi-asserted-by":"publisher","first-page":"7563","DOI":"10.1021\/acs.macromol.6b00742","article-title":"Effect of Water on the Thermal Transition\nObserved\nin Poly(allylamine hydrochloride)\u2013Poly(acrylic acid) Complexes","volume":"49","author":"Zhang","year":"2016","journal-title":"Macromolecules"},{"issue":"5","key":"2026081410141975900_cit20","doi-asserted-by":"publisher","first-page":"638","DOI":"10.1021\/acscentsci.8b00137","article-title":"Molecular Origin of the Glass Transition\nin Polyelectrolyte\nAssemblies","volume":"4","author":"Zhang","year":"2018","journal-title":"ACS Cent. 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Adv."},{"key":"2026081410141975900_cit24","doi-asserted-by":"publisher","first-page":"1374","DOI":"10.1038\/s41467-025-68124-2","article-title":"Ionic glass formers show an inverted\nrelation between fragility and non-exponential alpha-relaxation","volume":"17","author":"van Lange","year":"2026","journal-title":"Nat. Commun."},{"issue":"5","key":"2026081410141975900_cit25","doi-asserted-by":"publisher","first-page":"1195","DOI":"10.1039\/D5SM01081K","article-title":"A molecular dynamics study of the structure and dynamics of screened\npolyelectrolyte complex materials","volume":"22","author":"van Lange","year":"2026","journal-title":"Soft Matter."},{"issue":"116","key":"2026081410141975900_cit26","doi-asserted-by":"publisher","first-page":"116","DOI":"10.1002\/ad.1710","article-title":"4D Printing\nMulti-Material Shape Change","volume":"84","author":"Tibbits","year":"2014","journal-title":"Archit. Des."},{"issue":"1","key":"2026081410141975900_cit27","doi-asserted-by":"publisher","first-page":"78","DOI":"10.1080\/21680396.2018.1530155","article-title":"Liquid crystal elastomers:\nan introduction and review\nof emerging technologies","volume":"6","author":"Ula","year":"2018","journal-title":"Liq. Cryst. Rev."},{"issue":"7660","key":"2026081410141975900_cit28","doi-asserted-by":"publisher","first-page":"632","DOI":"10.1038\/nature22987","article-title":"Making waves in\na photoactive polymer film","volume":"546","author":"Gelebart","year":"2017","journal-title":"Nature"},{"issue":"2","key":"2026081410141975900_cit29","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201805985","article-title":"An Artificial\nNocturnal Flower via Humidity-Gated Photoactuation in Liquid Crystal\nNetworks","volume":"31","author":"Wani","year":"2019","journal-title":"Adv. Mater."},{"issue":"36","key":"2026081410141975900_cit30","doi-asserted-by":"publisher","first-page":"14364","DOI":"10.1021\/jacs.9b06757","article-title":"Interpenetrating\nLiquid-Crystal Polyurethane\/Polyacrylate Elastomer with Ultrastrong\nMechanical Property","volume":"141","author":"Lu","year":"2019","journal-title":"J. Am. Chem. Soc."},{"issue":"5","key":"2026081410141975900_cit31","doi-asserted-by":"publisher","first-page":"870","DOI":"10.1039\/C8SM02174K","article-title":"Direct shape programming of liquid crystal elastomers","volume":"15","author":"Barnes","year":"2019","journal-title":"Soft Matter."},{"issue":"6","key":"2026081410141975900_cit32","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202115166","article-title":"One-Pot Synthesis of Melt-Processable\nSupramolecular Soft Actuators","volume":"61","author":"Lugger","year":"2022","journal-title":"Angew. Chem.,\nInt. Ed. Engl."},{"issue":"1","key":"2026081410141975900_cit33","doi-asserted-by":"publisher","first-page":"36","DOI":"10.1038\/nmat3812","article-title":"Mouldable liquid-crystalline elastomer actuators with\nexchangeable covalent bonds","volume":"13","author":"Pei","year":"2014","journal-title":"Nat. Mater."},{"issue":"5","key":"2026081410141975900_cit34","doi-asserted-by":"publisher","first-page":"4927","DOI":"10.1021\/acs.chemrev.0c01057","article-title":"Exchangeable\nLiquid Crystalline Elastomers\nand Their Applications","volume":"122","author":"Saed","year":"2022","journal-title":"Chem. Rev."},{"key":"2026081410141975900_cit35","doi-asserted-by":"publisher","first-page":"101112","DOI":"10.1016\/j.mtbio.2024.101112","article-title":"Melt electrowritten poly-lactic acid\/nanodiamond scaffolds\ntowards wound-healing patches","volume":"26","author":"Wu","year":"2024","journal-title":"Mater. Today\nBio"},{"issue":"1","key":"2026081410141975900_cit36","doi-asserted-by":"publisher","first-page":"38","DOI":"10.1038\/s43246-025-01048-y","article-title":"Multi-functional liquid\ncrystal oligomer networks for human-interactive self-regulation","volume":"7","author":"Lyu","year":"2025","journal-title":"Commun. Mater."},{"issue":"5","key":"2026081410141975900_cit37","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202516769","article-title":"Universal Water Transfer Printing\nEnables Scalable Structural Coloration of Responsive Textile Fibers\nfor Wearable Electronics","volume":"38","author":"Chen","year":"2026","journal-title":"Adv. Mater."},{"key":"2026081410141975900_cit38","doi-asserted-by":"crossref","DOI":"10.1002\/047147875X","volume-title":"Principles of Polymerization.","author":"Odian","year":"2004"},{"issue":"6","key":"2026081410141975900_cit39","doi-asserted-by":"publisher","first-page":"2484","DOI":"10.1021\/acs.macromol.2c02230","article-title":"Facile Assembly of C\u2013N Bond-Containing Polymer\nElectrolytes Enabled by Lithium Salt-Catalyzed Aza-Michael Addition","volume":"56","author":"Wang","year":"2023","journal-title":"Macromolecules"},{"issue":"14","key":"2026081410141975900_cit40","doi-asserted-by":"publisher","first-page":"2095","DOI":"10.1002\/1521-3935(200210)203:14&lt;2095::AID-MACP2095&gt;3.0.CO;2-9","article-title":"Effect of charge density\non the formation and salt\nstability of polyelectrolyte complexes","volume":"203","author":"Dautzenberg","year":"2002","journal-title":"Macromol.\nChem. Phys."},{"issue":"17","key":"2026081410141975900_cit41","doi-asserted-by":"publisher","first-page":"7765","DOI":"10.1021\/acs.macromol.1c00940","article-title":"Relaxation\nTimes of Solid-like Polyelectrolyte Complexes of Varying pH and Water\nContent","volume":"54","author":"Lalwani","year":"2021","journal-title":"Macromolecules"},{"issue":"10","key":"2026081410141975900_cit42","doi-asserted-by":"publisher","first-page":"4680","DOI":"10.1021\/acs.macromol.4c00247","article-title":"Decoupling\nthe Effects of Charge Density and Hydrophobicity on the Phase Behavior\nand Viscoelasticity of Complex Coacervates","volume":"57","author":"Rami\u0301rez Marrero","year":"2024","journal-title":"Macromolecules"},{"issue":"29","key":"2026081410141975900_cit43","doi-asserted-by":"publisher","first-page":"5219","DOI":"10.1021\/acs.macromol.6c00278","article-title":"Effect of Copolymer\nChemistry on the Humidity- and Temperature-Dependent Mechanical Properties\nand Structure of Polyelectrolyte Complexes","volume":"59","author":"Rami\u0301rez Marrero","year":"2026","journal-title":"Macromolecules"},{"issue":"25","key":"2026081410141975900_cit44","doi-asserted-by":"publisher","first-page":"18997","DOI":"10.1039\/C5RA01039J","article-title":"Tailorable and programmable\nliquid-crystalline elastomers\nusing a two-stage thiol\u2013acrylate reaction","volume":"5","author":"Yakacki","year":"2015","journal-title":"RSC Adv."},{"issue":"5","key":"2026081410141975900_cit45","doi-asserted-by":"publisher","first-page":"567","DOI":"10.1107\/S002188988201259X","article-title":"Interpretation\nof small-angle scattering curves proportional to a negative power\nof the scattering vector","volume":"15","author":"Schmidt","year":"1982","journal-title":"J. Appl. Crystallogr."},{"issue":"6","key":"2026081410141975900_cit46","doi-asserted-by":"publisher","first-page":"781","DOI":"10.1107\/S0021889888000263","article-title":"Small-angle\nscattering by fractal systems","volume":"21","author":"Teixeira","year":"1988","journal-title":"J. Appl. Crystallogr."},{"issue":"18","key":"2026081410141975900_cit47","doi-asserted-by":"publisher","first-page":"7944","DOI":"10.1021\/acs.macromol.0c00930","article-title":"Solid-to-Liquid\nPhase Transition in Polyelectrolyte Complexes","volume":"53","author":"Meng","year":"2020","journal-title":"Macromolecules"},{"issue":"13","key":"2026081410141975900_cit48","doi-asserted-by":"publisher","first-page":"2454","DOI":"10.1039\/C7SM02041D","article-title":"Structure and rheology of polyelectrolyte\ncomplex coacervates","volume":"14","author":"Marciel","year":"2018","journal-title":"Soft Matter."},{"issue":"37","key":"2026081410141975900_cit49","doi-asserted-by":"publisher","first-page":"6594","DOI":"10.1039\/C7SM01215B","article-title":"Highly stretchable\nhydrogels from complex coacervation of natural polyelectrolytes","volume":"13","author":"Laleve\u0301e","year":"2017","journal-title":"Soft Matter."}],"container-title":["ACS Applied Polymer Materials"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acsapm.6c01534","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/aapmcd\/article-pdf\/8\/15\/12440\/66392242\/acsapm.6c01534.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/aapmcd\/article-pdf\/8\/15\/12440\/66392242\/acsapm.6c01534.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T14:25:56Z","timestamp":1786717556000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/aapmcd\/article\/8\/15\/12440\/5243570\/Stretchable-Water-Free-Liquid-Crystalline"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,4]]},"references-count":49,"journal-issue":{"issue":"15","published-online":{"date-parts":[[2026,8,4]]},"published-print":{"date-parts":[[2026,8,14]]}},"URL":"https:\/\/doi.org\/10.1021\/acsapm.6c01534","relation":{},"ISSN":["2637-6105"],"issn-type":[{"value":"2637-6105","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,4]]}}}