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Tale of Three Phosphate Additives for Stabilizing NCM811/Graphite Pouch Cells: Significance of Molecular Structure-Reactivity in Dictating Interphases and Cell Performance
Zhao, Huajun1,3; Qian, Yunxian2; Hu, Shiguang2; Luo, Guangfu1,5; Nie, Chenxi1; Qiu, Peiqi1; Kang, Yuanyuan2; Wang, Han2; Chu, Yanli2; Wang, Qingrong1; Wang, Jun1; Shao, Huaiyu3; Xu, Kang4; Deng, Yonghong1
2021-06-30
Source PublicationACS Applied Materials and Interfaces
ISSN1944-8244
Volume13Issue:25Pages:29676-29690
Abstract

Electrolyte additives have been extensively used as an economical approach to improve Li-ion battery (LIB) performances; however, their selection has been conducted on an Edisonian trial-and-error basis, with little knowledge about the relationship between their molecular structure and reactivity as well as the electrochemical performance. In this work, a series of phosphate additives with systematic structural variation were introduced with the purpose of revealing the significance of additive structure in building a robust interphase and electrochemical property in LIBs. By comparing the interphases formed by tripropyl phosphate (TPPC1), triallyl phosphate (TPPC2), and tripropargyl phosphate (TPPC3) containing alkane, alkene, and alkyne functionalities, respectively, theoretical calculations and comprehensive characterizations reveal that TPPC3 and TPPC2 exhibit more reactivity than TPPC1, and both can preferentially decompose both reductively and oxidatively, forming dense and protective interphases on both the cathode and anode, but they lead to different long-term cycling behaviors at 55 °C. We herein correlate the electrochemical performance of the high energy Li-ion cells to the molecular structure of these additives, and it is found that the effectiveness of TPPC1, TPPC2, and TPPC3 in preventing gas generation, suppressing interfacial resistance growth, and improving cycling stability can be described as TPPC3 > TPPC2 > TPPC1, i.e., the most unsaturated additive TPPC3 is the most effective additive among them. The established correlation between structure-reactivity and interphase-performance will doubtlessly construct the principle foundation for the rational design of new electrolyte components for future battery chemistry.

KeywordElectrolyte Additive High Energy Density Lithium-ion Batteries Molecular Structure Solid Electrolyte Interphase
DOI10.1021/acsami.1c06890
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaMaterials Science ; Science & Technology - Other Topics
WOS SubjectNanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000670430100041
Scopus ID2-s2.0-85110246189
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Cited Times [WOS]:2   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionUniversity of Macau
Corresponding AuthorShao, Huaiyu; Xu, Kang; Deng, Yonghong
Affiliation1.Department of Materials Science and Engineering, Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology, Shenzhen, 518055, China
2.Shenzhen CAPCHEM Technology Co. Ltd., Shenzhen, 518118, China
3.Guangdong-Hong Kong-Macau Jt. Lab. for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Taipa, Avenida da Universidade, 999078, Macao
4.Energy Storage Branch, US Army Research Laboratory, Adelphi, 20783, United States
5.Guangdong Provincial Key Laboratory of Computational Science and Material Design, Southern University of Science and Technology, Shenzhen, 518055, China
First Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Recommended Citation
GB/T 7714
Zhao, Huajun,Qian, Yunxian,Hu, Shiguang,et al. Tale of Three Phosphate Additives for Stabilizing NCM811/Graphite Pouch Cells: Significance of Molecular Structure-Reactivity in Dictating Interphases and Cell Performance[J]. ACS Applied Materials and Interfaces,2021,13(25):29676-29690.
APA Zhao, Huajun,Qian, Yunxian,Hu, Shiguang,Luo, Guangfu,Nie, Chenxi,Qiu, Peiqi,Kang, Yuanyuan,Wang, Han,Chu, Yanli,Wang, Qingrong,Wang, Jun,Shao, Huaiyu,Xu, Kang,&Deng, Yonghong.(2021).Tale of Three Phosphate Additives for Stabilizing NCM811/Graphite Pouch Cells: Significance of Molecular Structure-Reactivity in Dictating Interphases and Cell Performance.ACS Applied Materials and Interfaces,13(25),29676-29690.
MLA Zhao, Huajun,et al."Tale of Three Phosphate Additives for Stabilizing NCM811/Graphite Pouch Cells: Significance of Molecular Structure-Reactivity in Dictating Interphases and Cell Performance".ACS Applied Materials and Interfaces 13.25(2021):29676-29690.
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