{"title":"Multiple enhancement effects of dipoles within polyimide cathode promoting highly efficient energy storage of lithium-ion batteries","authors":"","doi":"10.1016/j.ensm.2024.103779","DOIUrl":null,"url":null,"abstract":"<div><p>Polyimide (PI) has been recognized as a potential organic cathode for Li-ion batteries (LIBs) due to its programmable structural design, high theoretical capacity, and resource availability. However, the poor intrinsic electrical conductivity of PI means that PI-based cathodes of LIBs have inefficient energy storage performance, especially at high current densities. In this work, the molecular structure of PI is optimized to obtain a layer-stacked crystalline PI with significantly enhanced dipoles, denoted NT-B for the first time. The dipoles in this PI are induced by the electronegative carbonyl groups from the monomer biuret and further enhanced via a π-π layer stacking effect. This work is the first to verify that the co-directional dipole enhancement effect of biuret is surprisingly different from that of monomer urea. A series of ex-situ/in-situ and theoretical DFT simulations are carried out to understand the functional mechanism of such effects. The multiple enhancement effects of the dipoles synergistically promoting the generation of a strong built-in electric field (BIEF) within NT-B are proposed based on the results obtained. It is confirmed that this BIEF plays a significant role in accelerating electron transport, which enhances the electrochemical activity of LIB cathodes. This work provides a new idea for the structural design of high-performance PI cathodes for LIBs.</p></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":null,"pages":null},"PeriodicalIF":18.9000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy Storage Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2405829724006056","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Polyimide (PI) has been recognized as a potential organic cathode for Li-ion batteries (LIBs) due to its programmable structural design, high theoretical capacity, and resource availability. However, the poor intrinsic electrical conductivity of PI means that PI-based cathodes of LIBs have inefficient energy storage performance, especially at high current densities. In this work, the molecular structure of PI is optimized to obtain a layer-stacked crystalline PI with significantly enhanced dipoles, denoted NT-B for the first time. The dipoles in this PI are induced by the electronegative carbonyl groups from the monomer biuret and further enhanced via a π-π layer stacking effect. This work is the first to verify that the co-directional dipole enhancement effect of biuret is surprisingly different from that of monomer urea. A series of ex-situ/in-situ and theoretical DFT simulations are carried out to understand the functional mechanism of such effects. The multiple enhancement effects of the dipoles synergistically promoting the generation of a strong built-in electric field (BIEF) within NT-B are proposed based on the results obtained. It is confirmed that this BIEF plays a significant role in accelerating electron transport, which enhances the electrochemical activity of LIB cathodes. This work provides a new idea for the structural design of high-performance PI cathodes for LIBs.
期刊介绍:
Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field.
Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy.
Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.