{"title":"Reversible Multielectron Transfer Chemistry of I-Activated Voltage-Enhanced Ferrocene-Based Organic Cathodes.","authors":"Pei Li,Yichao Yan,Jiaxiong Zhu,Yiqiao Wang,Leyu Bi,Hu Hong,Xinru Yang,Yuwei Zhao,Qing Li,Shengnan Wang,Yue Hou,Alex K-Y Jen,Chunyi Zhi","doi":"10.1021/jacs.4c12173","DOIUrl":null,"url":null,"abstract":"Organic molecule engineering has the potential to design materials with multiple electroactive centers, affording high energy storage capabilities and low-cost chemistry. The discovery of ferrocenes contributes significantly to the broad applications of organometallic compounds. Even though their reversible redox reactions can be used in batteries, their low potential and limited electron density per unit mass pose some challenges. Here, we report an I-activated voltage-enhanced ferrocene-based molecule, (ferrocenylmethyl) trimethylammonium iodide (FcNI), featuring a dual redox center by decorating the ferrocene backbone with designed functional groups to regulate the electron energy of Fe3+/2+ redox couples. It enables multielectron transfer of I0/- and Fe3+/2+, a sharply increased potential of Fe3+/2+ redox couples, and high-power energy storage with cycling stability. An organic cathode based on FcNI molecules displays a discharge capacity of over 400 mAh g-1 at 2 A g-1 with high-voltage plateaus up to 1.7 and 3.5 V when coupled with a zinc or lithium anode, respectively, and an excellent rate capability. Our results show that organic molecules can be programmed with multiple redox sites to develop high-voltage, fast-charging, and high-capacity organic rechargeable batteries.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"90 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c12173","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Organic molecule engineering has the potential to design materials with multiple electroactive centers, affording high energy storage capabilities and low-cost chemistry. The discovery of ferrocenes contributes significantly to the broad applications of organometallic compounds. Even though their reversible redox reactions can be used in batteries, their low potential and limited electron density per unit mass pose some challenges. Here, we report an I-activated voltage-enhanced ferrocene-based molecule, (ferrocenylmethyl) trimethylammonium iodide (FcNI), featuring a dual redox center by decorating the ferrocene backbone with designed functional groups to regulate the electron energy of Fe3+/2+ redox couples. It enables multielectron transfer of I0/- and Fe3+/2+, a sharply increased potential of Fe3+/2+ redox couples, and high-power energy storage with cycling stability. An organic cathode based on FcNI molecules displays a discharge capacity of over 400 mAh g-1 at 2 A g-1 with high-voltage plateaus up to 1.7 and 3.5 V when coupled with a zinc or lithium anode, respectively, and an excellent rate capability. Our results show that organic molecules can be programmed with multiple redox sites to develop high-voltage, fast-charging, and high-capacity organic rechargeable batteries.
有机分子工程有潜力设计具有多个电活性中心的材料,提供高能量存储能力和低成本的化学。二茂铁的发现为有机金属化合物的广泛应用做出了重要贡献。尽管它们的可逆氧化还原反应可以用于电池,但它们的低电位和单位质量有限的电子密度带来了一些挑战。在这里,我们报道了一种i激活电压增强的二茂铁分子(二茂铁基甲基)三甲基碘化铵(FcNI),它通过用设计的官能团修饰二茂铁骨架来调节Fe3+/2+氧化还原对的电子能量,从而具有双氧化还原中心。它实现了I0/-和Fe3+/2+的多电子转移,Fe3+/2+氧化还原对电位的急剧增加,以及具有循环稳定性的高功率储能。基于FcNI分子的有机阴极在2 a g-1下具有超过400 mAh g-1的放电容量,当与锌或锂阳极耦合时,分别具有高达1.7 V和3.5 V的高压平台,并且具有出色的倍率能力。我们的研究结果表明,有机分子可以被编程为多个氧化还原位点,从而开发出高压、快速充电和高容量的有机可充电电池。
期刊介绍:
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