{"title":"多电子基聚苯基苯胺有机阴极的分子设计策略及其电化学性能","authors":"Lihuan Xu, Guangzhen Wang, Lin Yao, Chang Su","doi":"10.1021/acsaem.4c01344","DOIUrl":null,"url":null,"abstract":"The growing demands for electronic devices and electric vehicles require the exploration of more efficient and high-power battery systems, in which the organic cathode materials are becoming a research hot issue in energy storage batteries. In the work, a polytriphenylamine derivative of polyphenylaniline (P(PhAn)) with a polyaniline-like molecular backbone structure was prepared by Buchwald-Hartwig C–N coupling reaction, and its electrochemical performances were evaluated in detail as the lithium organic cathode material. P(PhAn) as cathode displayed the multielectron redox characteristic, in which two pairs of redox characteristic peaks occurred in the measured voltage range. Density functional theory (DFT) calculation and simulations further proved that the formed push–pull electron effect and the conjugated polyaniline-like skeleton change the redox potentials and electron transfer of the cathode material. The electrode material also exhibited stable cycling performances and superior rate performances. It has a decent initial discharge specific capacity of 133 mAh·g<sup>–1</sup>, and after the 100 cycles, it kept at 111.2 mAh·g<sup>–1</sup>, remaining the 86% of capacity retention compared to the second cycle. Under the current densities of 20, 50, 100, 200, and 500 mA·g<sup>–1</sup>, it displayed the discharge specific capacities of 124, 122.1, 119.5, 115.3, and 112.4 mAh·g<sup>–1</sup>, respectively, and a 90.6% of capacity was even remained at the rate of 500 mA·g<sup>–1</sup>. Furthermore, it was proved that the energy storage process for P(PhAn) was mainly controlled by a capacitive-diffusion hybrid kinetics process.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Molecular Design Strategy toward Multielectron-Based Polyphenylaniline Organic Cathode and Its Electrochemical Performance\",\"authors\":\"Lihuan Xu, Guangzhen Wang, Lin Yao, Chang Su\",\"doi\":\"10.1021/acsaem.4c01344\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The growing demands for electronic devices and electric vehicles require the exploration of more efficient and high-power battery systems, in which the organic cathode materials are becoming a research hot issue in energy storage batteries. In the work, a polytriphenylamine derivative of polyphenylaniline (P(PhAn)) with a polyaniline-like molecular backbone structure was prepared by Buchwald-Hartwig C–N coupling reaction, and its electrochemical performances were evaluated in detail as the lithium organic cathode material. P(PhAn) as cathode displayed the multielectron redox characteristic, in which two pairs of redox characteristic peaks occurred in the measured voltage range. Density functional theory (DFT) calculation and simulations further proved that the formed push–pull electron effect and the conjugated polyaniline-like skeleton change the redox potentials and electron transfer of the cathode material. The electrode material also exhibited stable cycling performances and superior rate performances. It has a decent initial discharge specific capacity of 133 mAh·g<sup>–1</sup>, and after the 100 cycles, it kept at 111.2 mAh·g<sup>–1</sup>, remaining the 86% of capacity retention compared to the second cycle. Under the current densities of 20, 50, 100, 200, and 500 mA·g<sup>–1</sup>, it displayed the discharge specific capacities of 124, 122.1, 119.5, 115.3, and 112.4 mAh·g<sup>–1</sup>, respectively, and a 90.6% of capacity was even remained at the rate of 500 mA·g<sup>–1</sup>. Furthermore, it was proved that the energy storage process for P(PhAn) was mainly controlled by a capacitive-diffusion hybrid kinetics process.\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-09-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsaem.4c01344\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsaem.4c01344","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Molecular Design Strategy toward Multielectron-Based Polyphenylaniline Organic Cathode and Its Electrochemical Performance
The growing demands for electronic devices and electric vehicles require the exploration of more efficient and high-power battery systems, in which the organic cathode materials are becoming a research hot issue in energy storage batteries. In the work, a polytriphenylamine derivative of polyphenylaniline (P(PhAn)) with a polyaniline-like molecular backbone structure was prepared by Buchwald-Hartwig C–N coupling reaction, and its electrochemical performances were evaluated in detail as the lithium organic cathode material. P(PhAn) as cathode displayed the multielectron redox characteristic, in which two pairs of redox characteristic peaks occurred in the measured voltage range. Density functional theory (DFT) calculation and simulations further proved that the formed push–pull electron effect and the conjugated polyaniline-like skeleton change the redox potentials and electron transfer of the cathode material. The electrode material also exhibited stable cycling performances and superior rate performances. It has a decent initial discharge specific capacity of 133 mAh·g–1, and after the 100 cycles, it kept at 111.2 mAh·g–1, remaining the 86% of capacity retention compared to the second cycle. Under the current densities of 20, 50, 100, 200, and 500 mA·g–1, it displayed the discharge specific capacities of 124, 122.1, 119.5, 115.3, and 112.4 mAh·g–1, respectively, and a 90.6% of capacity was even remained at the rate of 500 mA·g–1. Furthermore, it was proved that the energy storage process for P(PhAn) was mainly controlled by a capacitive-diffusion hybrid kinetics process.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.