Quantification of Charge Transport and Mass Deprivation in Solid Electrolyte Interphase for Kinetically-Stable Low-Temperature Lithium-Ion Batteries

被引：9

作者：

Dong, Liwei ^{[1
]}

Yan, Hui-Juan ^{[2
,4
]}

Liu, Qing-Xiang ^{[2
,4
]}

Liang, Jia-Yan ^{[1
,2
]}

Yue, Junpei ^{[2
]}

Niu, Min ^{[1
]}

Chen, Xingyu ^{[1
]}

Wang, Enhui ^{[2
]}

Xin, Sen ^{[2
,4
]}

Zhang, Xinghong ^{[3
]}

Yang, Chunhui ^{[1
]}

Guo, Yu-Guo ^{[2
,4
]}

机构：

[1] Harbin Inst Technol HIT, MOE Engn Res Ctr Electrochem Energy Storage & Carb, Sch Chem & Chem Engn, Harbin 150001, Peoples R China

[2] Chinese Acad Sci, CAS Key Lab Mol Nanostruct & Nanotechnol, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci BNLMS,Inst Chem, Beijing 100190, Peoples R China

[3] Harbin Inst Technol HIT, Ctr Composite Mat & Struct, Natl Key Lab Sci & Technol Adv Composites Special, Harbin 150001, Peoples R China

[4] Univ Chinese Acad Sci UCAS, Sch Chem Sci, Beijing 100049, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2024年 / 63卷 / 43期

基金：

北京市自然科学基金; 中国博士后科学基金; 国家重点研发计划; 中国国家自然科学基金;

关键词：

Lithium-ion battery; Low temperature; Solid electrolyte interphase; Transport kinetic; Interfacial stability; LI+; INTERFACE;

D O I：

10.1002/anie.202411029

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Graphite (Gr)-based lithium-ion batteries with admirable electrochemical performance below -20 degrees C are desired but are hindered by sluggish interfacial charge transport and desolvation process. Li salt dissociation via Li+-solvent interaction enables mobile Li+ liberation and contributes to bulk ion transport, while is contradictory to fast interfacial desolvation. Designing kinetically-stable solid electrolyte interphase (SEI) without compromising strong Li+-solvent interaction is expected to compatibly improve interfacial charge transport and desolvation kinetics. However, the relationship between physicochemical features and temperature-dependent kinetics properties of SEI remains vague. Herein, we propose four key thermodynamics parameters of SEI potentially influencing low-temperature electrochemistry, including electron work function, Li+ transfer barrier, surface energy, and desolvation energy. Based on the above parameters, we further define a novel descriptor, separation factor of SEI (SSEI), to quantitatively depict charge (Li+/e-) transport and solvent deprivation processes at Gr/electrolyte interface. A Li3PO4-based, inorganics-enriched SEI derived by Li difluorophosphate (LiDFP) additive exhibits the highest SSEI (4.89x103) to enable efficient Li+ conduction, e- blocking and rapid desolvation, and as a result, much suppressed Li-metal precipitation, electrolyte decomposition and Gr sheets exfoliation, thus improving low-temperature battery performances. Overall, our work originally provides visualized guides to improve low-temperature reaction kinetics/thermodynamics by constructing desirable SEI chemistry. A novel thermodynamics descriptor, separation factor of solid electrolyte interphase (SSEI) for designing desirable SEI chemistry, is established on the energy of Li+ diffusion (Delta VLi), electron tunneling (Phi e), solvent adsorption (Es), and desolvation processes (Delta Ed), and thus the kinetic stability of charge (Li+/e-) transport and mass (solvent) deprivation through SEI layer at low temperatures could be quantitatively evaluated. image

引用

页数：9

共 35 条

[11] Mitigating Swelling of the Solid Electrolyte Interphase using an Inorganic Anion Switch for Low-temperature Lithium-ion Batteries [J].