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However, the lack of rational materials design results in unsatisfactory self\u2010charging performance. Here, a covalent organic framework containing pyrene\u20104,5,9,10\u2010tetraone groups (COF\u2010PTO) is reported as a cathode material for aqueous self\u2010charging zinc batteries. The ordered channel structure of the COF\u2010PTO provides excellent capacity retention of 98% after 18 000 cycles at 10 A g\u22121<\/jats:sup> and ultra\u2010fast ion transfer. To visually assess the self\u2010charging performance, two parameters, namely self\u2010charging efficiency (self\u2010charging discharge capacity\/galvanostatic discharge capacity, \u03b7<\/jats:italic>) and average self\u2010charging rate (total discharge capacity after cyclic self\u2010charging\/total cyclic self\u2010charging time, \u03bd<\/jats:italic>), are proposed for performance evaluation. COF\u2010PTO achieves an impressive \u03b7<\/jats:italic> of 96.9% and an \u03bd of 30\u00a0mAh\u00a0g\u22121<\/jats:sup> self\u2010charge capacity per hour in 100 self\u2010charging cycles, surpassing the previous reports. Mechanism studies reveal the co\u2010insertion of Zn2+<\/jats:sup> and H+<\/jats:sup> double ions in COF\u2010PTO of self\u2010charging zinc batteries. In addition, the C\u2550N and C\u2550O (on the benzene) in COF\u2010PTO are ortho structures to each other, which can easily form metal heterocycles with Zn ions, thereby driving the forward progress of the self\u2010charging reaction and enhancing the self\u2010charging performance.<\/jats:p>","DOI":"10.1002\/adma.202314050","type":"journal-article","created":{"date-parts":[[2024,2,21]],"date-time":"2024-02-21T06:30:10Z","timestamp":1708497010000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":74,"title":["Self\u2010Charging Aqueous Zn\/\/COF Battery with UltraHigh Self\u2010Charging Efficiency and Rate"],"prefix":"10.1002","volume":"36","author":[{"given":"Leheng","family":"Zhong","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 51006 P. R. 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