Tale of Three Phosphate Additives for Stabilizing NCM811/Graphite Pouch Cells: Significance of Molecular Structure-Reactivity in Dictating Interphases and Cell Performance

被引：17

作者：

Zhao, Huajun ^{[1
,2
]}

Qian, Yunxian ^{[3
]}

Hu, Shiguang ^{[3
]}

Luo, Guangfu ^{[1
,4
]}

Nie, Chenxi ^{[1
]}

Qiu, Peiqi ^{[1
]}

Kang, Yuanyuan ^{[3
]}

Wang, Han ^{[3
]}

Chu, Yanli ^{[3
]}

Wang, Qingrong ^{[1
]}

Wang, Jun ^{[1
]}

Shao, Huaiyu ^{[2
]}

Xu, Kang ^{[5
]}

Deng, Yonghong ^{[1
]}

机构：

[1] Southern Univ Sci & Technol, Acad Adv Interdisciplinary Studies, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

[2] Univ Macau, Inst Appl Phys & Mat Engn, Guangdong Hong Kong Macau Joint Lab Photon Therma, Taipa 999078, Macao, Peoples R China

[3] Shenzhen CAPCHEM Technol Co Ltd, Shenzhen 518118, Peoples R China

[4] Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Peoples R China

[5] US Army Res Lab, Energy Storage Branch, Adelphi, MD 20783 USA

来源：

ACS APPLIED MATERIALS & INTERFACES | 2021年 / 13卷 / 25期

基金：

中国国家自然科学基金;

关键词：

electrolyte additive; high energy density; lithium-ion batteries; molecular structure; solid electrolyte interphase; LITHIUM-ION BATTERIES; IONIZATION MASS-SPECTROMETRY; RICH CATHODE MATERIALS; HIGH-ENERGY-DENSITY; ELECTROLYTE ADDITIVES; DEGRADATION-PRODUCTS; FORMATION MECHANISM; CYCLING STABILITY; METAL BATTERIES; NI-RICH;

D O I：

10.1021/acsami.1c06890

中图分类号：

TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

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 degrees 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.

引用

页码：29676 / 29690

页数：15