{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,17]],"date-time":"2026-09-17T15:02:17Z","timestamp":1789657337750,"version":"4.0.1"},"reference-count":30,"publisher":"American Chemical Society (ACS)","issue":"37","license":[{"start":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T00:00:00Z","timestamp":1788739200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T00:00:00Z","timestamp":1788739200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T00:00:00Z","timestamp":1788739200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100021171","name":"Basic and Applied Basic Research Foundation of Guangdong Province","doi-asserted-by":"publisher","award":["2026A1515010159"],"award-info":[{"award-number":["2026A1515010159"]}],"id":[{"id":"10.13039\/501100021171","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100011436","name":"State Key Laboratory of Electrical Insulation and Power Equipment","doi-asserted-by":"publisher","id":[{"id":"10.13039\/501100011436","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100012226","name":"Fundamental Research Funds for the Central Universities","doi-asserted-by":"publisher","award":["xzy012024004"],"award-info":[{"award-number":["xzy012024004"]}],"id":[{"id":"10.13039\/501100012226","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["52573086"],"award-info":[{"award-number":["52573086"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100017610","name":"Shenzhen Science and Technology Innovation Program","doi-asserted-by":"publisher","award":["JCYJ20240813143309013"],"award-info":[{"award-number":["JCYJ20240813143309013"]}],"id":[{"id":"10.13039\/501100017610","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100017610","name":"Shenzhen Science and Technology Innovation Program","doi-asserted-by":"publisher","award":["QNXMB20250701094319027"],"award-info":[{"award-number":["QNXMB20250701094319027"]}],"id":[{"id":"10.13039\/501100017610","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Guangdong Provincial Young Science and Technology Talent Cultivation Program","award":["SKXRC2025236"],"award-info":[{"award-number":["SKXRC2025236"]}]},{"name":"Specialized Innovation Projects in General Universities of Guangdong Province","award":["2025KTSCX112"],"award-info":[{"award-number":["2025KTSCX112"]}]},{"name":"Shenzhen Strategic Emerging Industry Support Plan","award":["F-2023-Z99-509043"],"award-info":[{"award-number":["F-2023-Z99-509043"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,17]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Poly(ether imide) (PEI) is a promising high-temperature dielectric material, yet its application is limited by severe intrachain and interchain charge transfer (CT) effects, which give rise to high leakage currents at elevated temperatures. Tuning interchain spacing has been recognized as an effective strategy to suppress CT effects, but it entails an intrinsic tradeoff: excessively large spacing facilitates free charge transport, whereas overly compact chain packing exacerbates CT interactions. Herein, we report a series of spiral-twisted PEI copolymers synthesized by incorporating the bulky, twisted BAFL diamine and the planar PPDA diamine with BPADA dianhydride. By systematically varying the BAFL\/PPDA molar ratio, we identified that the cPEI-5 composition (50 mol % BAFL and 50 mol % PPDA) as possessing the most favorable interchain spacing, which effectively suppresses CT without unduly weakening interchain coupling, thereby yielding the widest bandgap (3.37\u202feV) and the deepest trap level (2.19\u202feV). This optimal spacing, enabled by the spiral-twisted backbone, concurrently shortens the hopping distance and lowers the carrier mobility, leading to a substantial reduction in leakage current. Consequently, cPEI-5 achieves a breakdown strength of 610\u202fMV\u202fm\u20131 at 150\u202f\u00b0C, which is 36.2% higher than cPEI-0 and 9.5% higher than cPEI-10, and delivers a discharged energy density of 5.5\u202fJ\u202fcm\u20133 at &amp;gt; 90% efficiency, surpassing the room-temperature performance of biaxially oriented polypropylene (BOPP, 4.0\u202fJ\u202fcm\u20133). Moreover, cPEI-5 demonstrates excellent cycling stability (over 50\u202f000 cycles, 0.8% loss) and fast discharge capability (t95\u202f=\u202f2.47\u202f\u03bcs, power density = 0.28\u202fMW\u202fcm\u20133). This work underscores that rational engineering of spiral-twisted structures enables a synergistic balance between CT suppression and charge transport, offering a new paradigm for high-performance polymer dielectrics under harsh operating conditions.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02606","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T10:02:03Z","timestamp":1788775323000},"page":"10657-10664","source":"Crossref","is-referenced-by-count":0,"title":["Spiral-Twisted Poly(ether imide) Copolymer Dielectrics\nwith Synergistically Modulated Interchain Spacing and Charge Transfer\nfor High-Temperature Capacitive Energy Storage"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-5759-6800","authenticated-orcid":true,"given":"Li","family":"Tan","sequence":"first","affiliation":[{"name":"Shenzhen University , , ,","place":["Shenzhen, China, 518060"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ding","family":"Ai","sequence":"additional","affiliation":[{"name":"Xi\u2019an Jiaotong University , , ,","place":["Xian, China, 710049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1461-2222","authenticated-orcid":true,"given":"Wugang","family":"Liao","sequence":"additional","affiliation":[{"name":"Shenzhen University , , ,","place":["Shenzhen, China, 518060"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuangwu","family":"Huang","sequence":"additional","affiliation":[{"name":"Shenzhen University , , ,","place":["Shenzhen, China, 518060"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0516-6208","authenticated-orcid":true,"given":"Qiyan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shenzhen University , , ,","place":["Shenzhen, China, 518060"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,7]]},"reference":[{"key":"2026091709085958200_cit1","doi-asserted-by":"publisher","first-page":"576","DOI":"10.1038\/nature14647","article-title":"Flexible high-temperature dielectric materials from polymer nanocomposites","volume":"523","author":"Li","year":"2015","journal-title":"Nature"},{"key":"2026091709085958200_cit2","doi-asserted-by":"publisher","first-page":"62","DOI":"10.1038\/s41586-022-05671-4","article-title":"Ladderphane copolymers for high-temperature\ncapacitive energy storage","volume":"615","author":"Chen","year":"2023","journal-title":"Nature"},{"key":"2026091709085958200_cit3","doi-asserted-by":"publisher","first-page":"143","DOI":"10.1038\/s41560-023-01416-3","article-title":"Roll-to-roll fabricated polymer composites\nfilled with subnanosheets exhibiting high energy density and cyclic\nstability at 200 \u00b0C","volume":"9","author":"Yang","year":"2024","journal-title":"Nat. Energy"},{"key":"2026091709085958200_cit4","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202311739","article-title":"Dilute Nanocomposites:\nTuning Polymer Chain Local Nanostructures to Enhance Dielectric Responses","volume":"36","author":"Rui","year":"2024","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit5","doi-asserted-by":"publisher","DOI":"10.1002\/sus2.228","article-title":"Flexible mica films coated by magnetron\nsputtered insulating layers for high-temperature capacitive energy\nstorage","volume":"4","author":"Yin","year":"2024","journal-title":"SusMat"},{"key":"2026091709085958200_cit6","doi-asserted-by":"publisher","first-page":"7793","DOI":"10.1021\/acs.nanolett.5c00788","article-title":"Nanostructure Engineering Significantly Enhances Capacitive Energy\nStorage Performance in All-Polymer Dielectrics at Elevated Temperatures","volume":"25","author":"Xie","year":"2025","journal-title":"Nano Lett."},{"key":"2026091709085958200_cit7","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2026.176261","article-title":"Nanostructured interfaces\nin thermoplastic\/thermosetting polymer blends for enhanced high-temperature\ncapacitive energy storage","volume":"537","author":"Fu","year":"2026","journal-title":"Chem. Eng. J."},{"key":"2026091709085958200_cit8","doi-asserted-by":"publisher","first-page":"9351","DOI":"10.1038\/s41467-024-53674-8","article-title":"Scalable all polymer\ndielectrics with self-assembled nanoscale multiboundary exhibiting\nsuperior high temperature capacitive performance","volume":"15","author":"Zhang","year":"2024","journal-title":"Nat. Commun."},{"key":"2026091709085958200_cit9","doi-asserted-by":"publisher","first-page":"1074","DOI":"10.1038\/s41563-025-02130-z","article-title":"Dielectric\npolymers with mechanical bonds for high-temperature\ncapacitive energy storage","volume":"24","author":"Wang","year":"2025","journal-title":"Nat. Mater."},{"key":"2026091709085958200_cit10","doi-asserted-by":"publisher","first-page":"8119","DOI":"10.1039\/D4EE02455A","article-title":"Low-entropy amorphous\ndielectric polymers for high-temperature capacitive\nenergy storage","volume":"17","author":"Zhang","year":"2024","journal-title":"Energy Environ. Sci."},{"key":"2026091709085958200_cit11","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202211487","article-title":"Scalable Polyimide-Organosilicate\nHybrid Films for High-Temperature Capacitive Energy Storage","volume":"35","author":"Dong","year":"2023","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit12","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202521682","article-title":"Scalable Polymer\nComposites Enhanced by Trace-Amount Polymer Semiconductor for High-Performance\nCapacitive Energy Storage at 250 \u00b0C","volume":"38","author":"Pan","year":"2026","journal-title":"Adv.\nMater."},{"key":"2026091709085958200_cit13","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202303732","article-title":"Scalable High-Permittivity\nPolyimide Copolymer with Ultrahigh High-Temperature\nCapacitive Performance Enabled by Molecular Engineering","volume":"14","author":"Dong","year":"2024","journal-title":"Adv. Energy Mater."},{"key":"2026091709085958200_cit14","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202207451","article-title":"Dynamic Sustainable\nPolyimide Film Combining Hardness with Softness via a \u2033Mimosa-Like\u2033\nBionic Strategy","volume":"35","author":"Wan","year":"2023","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit15","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202307804","article-title":"Dual-Effect Coupling for Superior\nDielectric and Thermal Conductivity of Polyimide Composite Films Featuring\n\u2033Crystal-Like Phase\u2033 Structure","volume":"36","author":"Dong","year":"2024","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit16","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.170158","article-title":"Molecularly\nconstrained conformation engineering suppresses charge hopping in\npolyetherimide for superior capacitive storage at elevated temperatures","volume":"525","author":"Dong","year":"2025","journal-title":"Chem. Eng. J."},{"key":"2026091709085958200_cit17","doi-asserted-by":"publisher","first-page":"2730","DOI":"10.1016\/0032-3861(94)90300-X","article-title":"Charge-transfer\ninteraction and chain association in\npoly(ether imide) solutions: a fluorescence spectroscopic study","volume":"35","author":"Viallat","year":"1994","journal-title":"Polymer"},{"key":"2026091709085958200_cit18","doi-asserted-by":"publisher","first-page":"6369","DOI":"10.1039\/D0CS00765J","article-title":"Dielectric polymers for high-temperature capacitive energy storage","volume":"50","author":"Li","year":"2021","journal-title":"Chem. Soc. 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Interfaces"},{"key":"2026091709085958200_cit21","doi-asserted-by":"publisher","first-page":"56","DOI":"10.1039\/D1EE03186D","article-title":"High-temperature\npolyimide dielectric materials for energy storage: theory, design,\npreparation and properties","volume":"15","author":"Liu","year":"2022","journal-title":"Energy Environ.\nSci."},{"key":"2026091709085958200_cit22","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202303849","article-title":"Spiral-Structured Dielectric Polymers\nExhibiting Ultrahigh Energy Density and Charge\u2013Discharge Efficiency\nat High Temperatures","volume":"35","author":"Ran","year":"2023","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit23","doi-asserted-by":"publisher","first-page":"2448","DOI":"10.1016\/j.matt.2021.04.026","article-title":"High-temperature\npolymers with record-high breakdown strength enabled by rationally\ndesigned chain-packing behavior in blends","volume":"4","author":"Zhang","year":"2021","journal-title":"Matter"},{"key":"2026091709085958200_cit24","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202511464","article-title":"Confined Dynamic and\nStatic Disorder Realized by Entropy Engineering,\na New Path to Excellent High Temperature Energy Storage Performance","volume":"38","author":"Yang","year":"2026","journal-title":"Adv. Mater."},{"key":"2026091709085958200_cit25","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.155398","article-title":"Enhanced High-Temperature\nperformance of PEI dielectrics via deep trap energy levels and physically\ncrosslinked effects","volume":"498","author":"Hu","year":"2024","journal-title":"Chem. Eng. J."},{"key":"2026091709085958200_cit26","doi-asserted-by":"publisher","first-page":"46573","DOI":"10.1002\/app.46573","article-title":"Synthesis,\noptical, and thermal properties of polyimides\ncontaining flexible ether linkage","volume":"135","author":"Kaya","year":"2018","journal-title":"J. Appl.\nPolym. Sci."},{"key":"2026091709085958200_cit27","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202313258","article-title":"Significant\nEnhancement in Dielectric\nProperties of Polyimide Alloys Through a Two-Phase Interlocking Structure","volume":"34","author":"Liu","year":"2024","journal-title":"Adv. Funct. Mater."},{"key":"2026091709085958200_cit28","doi-asserted-by":"publisher","first-page":"1223","DOI":"10.1039\/D4MH01407C","article-title":"Outstanding\nhigh-temperature capacitive performance in all-organic dielectrics\nenabled by synergistic optimization of molecular traps and aggregation\nstructures","volume":"12","author":"Peng","year":"2025","journal-title":"Mater. Horiz."},{"key":"2026091709085958200_cit29","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202202421","article-title":"Excellent\nStability in Polyetherimide\/SiO2 Nanocomposites with Ultrahigh\nEnergy Density and Discharge Efficiency\nat High Temperature","volume":"18","author":"Sun","year":"2022","journal-title":"Small"},{"key":"2026091709085958200_cit30","doi-asserted-by":"publisher","first-page":"3919","DOI":"10.1038\/s41467-020-17760-x","article-title":"Polymer\/molecular\nsemiconductor all-organic composites for high-temperature dielectric\nenergy storage","volume":"11","author":"Yuan","year":"2020","journal-title":"Nat. Commun."}],"container-title":["The Journal of Physical Chemistry Letters"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acs.jpclett.6c02606","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/37\/10657\/68401446\/acs.jpclett.6c02606.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/37\/10657\/68401446\/acs.jpclett.6c02606.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,17]],"date-time":"2026-09-17T14:04:19Z","timestamp":1789653859000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article\/17\/37\/10657\/5422244\/Spiral-Twisted-Poly-ether-imide-Copolymer"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,9,7]]},"references-count":30,"journal-issue":{"issue":"37","published-online":{"date-parts":[[2026,9,7]]},"published-print":{"date-parts":[[2026,9,17]]}},"URL":"https:\/\/doi.org\/10.1021\/acs.jpclett.6c02606","relation":{},"ISSN":["1948-7185"],"issn-type":[{"value":"1948-7185","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,9,7]]}}}