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However, their practical application is often limited by low output voltage and poor thermal stability. Herein, we use a heteroatomic substitution strategy to develop 4,4\u2032\u2010azopyridine. This modification results in a 350\u2005mV increase in reduction potential compared to traditional azobenzene, increasing the energy density at the material level from 187 to 291\u2005Wh\u2009kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    . The introduced heteroatoms not only raise the melting point of azo compounds from 68\u2009\u00b0C to 112\u2009\u00b0C by forming an intermolecular hydrogen\u2010bond network but also improves electrode kinetics by reducing energy band gaps. Moreover, 4,4\u2032\u2010azopyridine forms metal\u2010ligand complexes with Zn\n                    <jats:sup>2+<\/jats:sup>\n                    ions, which further self\u2010assemble into a robust superstructure, acting as a molecular conductor to facilitate charge transfer. Consequently, the batteries display a good rate performance (192\u2005mAh\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 20\u2005C) and an ultra\u2010long lifespan of 60,000\u2005cycles. Notably, we disclose that the depleted batteries spontaneously self\u2010charge when exposed to air, marking a significant advancement in the development of self\u2010powered aqueous systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202408292","type":"journal-article","created":{"date-parts":[[2024,5,31]],"date-time":"2024-05-31T04:11:16Z","timestamp":1717128676000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":52,"title":["High\u2010Performance Azo Cathodes Enabled by N\u2010Heteroatomic Substitution for Zinc Batteries with a Self\u2010Charging Capability"],"prefix":"10.1002","volume":"63","author":[{"given":"Dawei","family":"Du","sequence":"first","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuqi","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiapeng","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lanyu","family":"Jin","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weixiao","family":"Ji","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-2831-2236","authenticated-orcid":false,"given":"He","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Siping","family":"Pang","sequence":"additional","affiliation":[{"name":"School of Materials Science &amp; Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,7,15]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2023.06.007"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.coelec.2021.100801"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202008960"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1002\/batt.202200237"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1039\/D3EE00211J"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1039\/C9EE02526J"},{"key":"e_1_2_7_8_2","first-page":"1","volume":"14","author":"Deng R.","year":"2023","journal-title":"Nat. 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