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For a long time, the dominant approach to optimizing the thermoelectric performance of most organic materials is chemical doping, which, however, is not always ideal for practical applications due to its tendency to involve intricate processing procedure and trigger material and device instability. Currently, the pursuit of single\u2010component neutral thermoelectric materials without exogenous doping presents a compelling alternative. In this work, we designed and synthesized a high\u2010spin polymer material, PBBT\u2010TT, by simultaneously employing thieno[3,4\u2010\n                    <jats:italic>b<\/jats:italic>\n                    ]thiophene (T\n                    <jats:italic>b<\/jats:italic>\n                    T) and benzo[1,2\u2010\n                    <jats:italic>c<\/jats:italic>\n                    \u2009:\u20094,5\u2010\n                    <jats:italic>c<\/jats:italic>\n                    \u2032]bis[1,2,5]thiadiazole (BBT) units with pronounced proquinoidal characteristics, its analogue, PBBT\u2010T to demonstrate the effect of the T\n                    <jats:italic>b<\/jats:italic>\n                    T unit was also synthesized. The results indicate that because of the enhanced quinoidal resonance, increased spin density and strong intermolecular antiferromagnetic coupling, PBBT\u2010TT exhibits high intrinsic electrical conductivity and Seebeck coefficient, which showcases an outstanding power factor of 26.1\u2005\u03bcW\u2009m\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2009K\n                    <jats:sup>\u22122<\/jats:sup>\n                    without doping. This achievement surpasses other neutral organic conjugated polymer and radical conductors, and is even comparable to some typical early\u2010stage doped polymers. Notably, PBBT\u2010TT exhibits remarkable ambient stability, retaining its initial thermoelectric performance over a 120\u2010day period. Our finding demonstrates that modulating the intermolecular spin interactions in open\u2010shell polymers through the introduction of strong proquinoidal units is an effective strategy for the development of doping\u2010free, intrinsically high\u2010performance polymer thermoelectric materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.202413061","type":"journal-article","created":{"date-parts":[[2024,8,14]],"date-time":"2024-08-14T07:38:25Z","timestamp":1723621105000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Thermoelectric Performance in Triplet\u2010Ground\u2010State Polymer Intrinsically Boosted by Enhanced Proquinoidal Characteristic"],"prefix":"10.1002","volume":"64","author":[{"given":"Runshi","family":"Wu","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory for Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Wei","sequence":"additional","affiliation":[{"name":"College of Chemistry, Key Laboratory of Theoretical &amp; Computational Photochemistry of Ministry of Education Beijing Normal University  Beijing 100190 China"},{"name":"Laboratory of Theoretical and Computational Nanoscience, CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaojuan","family":"Dai","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory for Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liqin","family":"Yan","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"School of Physical Sciences University of Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wuyue","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory for Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dafei","family":"Yuan","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha, Hunan 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia","family":"Zhu","sequence":"additional","affiliation":[{"name":"Laboratory of Theoretical and Computational Nanoscience, CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6812-0856","authenticated-orcid":false,"given":"Xiaozhang","family":"Zhu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory for Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,10,16]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2016.50"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00204F"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.2c00696"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.26599\/NRE.2023.9120097"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00581"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.2c00696"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-020-17063-1"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6CS00149A"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.6b00329"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1TC06175E"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/aelm.201800825"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nww040"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/256394a0"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja0502728"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aao7287"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202206161"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201909805"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aav2336"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.xcrp.2021.100467"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.985"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.10.001"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201908015"},{"key":"e_1_2_7_23_1","author":"Tahir H.","year":"2023","journal-title":"Adv. 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