Chemo-mechanical stable cathode interphase via interface in situ catalytic-conversion integrated design for all solid-state batteries
By
Zhou, XY (Zhou, Xuanyi) [1] ; Zhang, B (Zhang, Biao) [2] ; Lyu, P (Lyu, Pengbo) [2] ; Xi, L (Xi, Lei) [1] ; Li, FK (Li, Fangkun) [1] ; Ma, ZS (Ma, Zengsheng) [2] ; Zhu, M (Zhu, Min) [1] ; Liu, J (Liu, Jun) [1]
(provided by Clarivate)
Source
ENERGY & ENVIRONMENTAL SCIENCE
DOI10.1039/d4ee02827a
Early Access
SEP 2024
Indexed
2024-10-04
Document Type
Article; Early Access
Abstract
All-solid-state lithium batteries (ASSLBs) based on LiNi1-x-yCoxMnyO2 cathodes suffer from rock-ribbed electrolyte-cathode interface issues such as oxygen evolution and side reactions with electrolytes at high operating voltages, resulting in severe structure deterioration and rapid capacity decay. Herein, a type of synergistic catalytic conversion-integrated mechanism was strategically exploited to in situ construct a steerable cathode-electrolyte interface (CEI), aiming to synchronously enhance electrochemical and structural stability upon cycling. By employing functional polypyrrole (PPy) as a coating layer on high voltage-operated LiNi0.8Co0.1Mn0.1O2 (NCM811), we revealed that the N-H bond of the polypyrrole ring can cause N-H & ctdot;O hydrogen bonding interaction to alleviate oxygen evolution. By employing functional polypyrrole (PPy) as coating layer on high voltage-operated LiNi0.8Co0.1Mn0.1O2 (NCM811), we unveils that the N-H bond of polypyrrole ring can product N-H & ctdot;O hydrogen bonding interaction to alleviate oxygen evolution. Specifically, the hydrogen bonding between the nitrogen-hydrogen (N-H) groups of polypyrrole (PPy) and lattice oxygen escaped form NCM811 facilitates the reduction of protons to generate hydroxide ions (OH-). The resulting astray OH- together with O2- further coordinated with Li+ around the aromatic skeleton interrupted by a nucleophilic pi-pi interaction, thereby promoting the in situ generation of an Li2O-LiOH-rich CEI. Finally, parasitic interfacial side reactions and oxygen evolution are considerably suppressed, endowing the NCM@PPy full cell with excellent cycling performance and a capacity retention of 81.2% after 300 cycles. This in situ-generated Li2O-LiOH-rich CEI enables the NCM811 cathode to achieve a considerable capacity of 122 mA h g(-1) at 0.5C with an operating voltage of 4.3 V and a lifetime of more than 100 cycles, demonstrating its practical application potential in the energy storage field.
Keywords
Keywords PlusHIGH-CAPACITY
Author Information
Corresponding Address
Liu, Jun
(corresponding author)
South China Univ Technol, Sch Mat Sci & Engn, Guangdong Prov Key Lab Adv Energy Storage Mat, Guangzhou 510641, Peoples R China
Affiliation
South China University of Technology
E-mail Addresses
msjliu@scut.edu.cn
Addresses
1 South China Univ Technol, Sch Mat Sci & Engn, Guangdong Prov Key Lab Adv Energy Storage Mat, Guangzhou 510641, Peoples R China
2 Xiangtan Univ, Sch Mat Sci & Engn, Key Lab Low Dimens Mat & Applicat Technol, Minist Educ, Xiangtan 411105, Peoples R China
E-mail Addresses
msjliu@scut.edu.cn
Data availability statement
The data supporting the findings of this study are available within the article and its ESI.dagger
Categories/ Classification
Research AreasChemistryEnergy & FuelsEngineeringEnvironmental Sciences & Ecology
Web of Science Categories
Chemistry, MultidisciplinaryEnergy & FuelsEngineering, ChemicalEnvironmental Sciences