Tailoring Electrolyte Distributions to Enable High-performance Li3PS4-based All-solid-state Batteries under Different Operating Temperatures

Wei，Chaochao1,2; Yu，Dian2; Xu，Xiangling2; Wang，Ru2; Li，Jiayang2; Lin，Jinyan2; Chen，Shaoqing3; Zhang，Long4; Yu，Chuang1,2

2023

10.1002/asia.202300304

Chemistry - An Asian Journal   Impact Factor & Quartile

1861-4728

1861-471X

LiPS shows great potential as solid electrolyte for all-solid-state lithium batteries (ASSLBs) due to its high Li-ion conductivity and excellent mechanical properties. However, its poor interfacial stability with bare high-nickel active materials in the cathode mixture inhibits the energy density and electrochemical performances of the corresponding LiNiMnCoO/LiPS/Li−In battery. The LiInCl electrolyte with good electrochemical/chemical stability with bare LiNiMnCoO(NCM622), which acts both as a Li-ion additive in the cathode mixture and as an isolation layer to isolate the direct contact between the sulfide electrolytes and active materials, providing superior solid/solid interface stabilities in the assembled battery. XPS and TEM results confirm that this strategy can mitigate the side reactions between the bare NCM622 and LiPS electrolytes. In-situ EIS and DRT results prove that this grading utilization of different solid electrolytes can greatly alleviate the poor electrochemical stability between those two materials, yielding smaller interfacial resistances. The corresponding battery delivers high discharge capacities at various C-rates under different operating temperatures. It delivers a much higher initial discharge capacity of 187.7 mAh g (vs. 92.5 mAh g) at 0.1 C with a coulombic efficiency of 87.6% (vs. 71.1%) at room temperature. Moreover, this battery can even show highly reversible capacity with excellent cyclability when the operating temperature lowers to 0 and −20 °C. This work provides a hierarchical utilization strategy to fabricate sulfide electrolytes-based ASSLBs with high energy density and superior cycling performance combined with highly-oxidation cathode materials.

ASSLBs bare NCM622 cathode interfacial instability Li3InCl6 Li3PS4 electrolyte

SCI

English

Others

National Key Research and Development Program[2021YFB2500200] ; National Natural Science Foundation of China[52177214] ; China Fujian Energy Devices Science and Technology Innovation Laboratory Open Fund[21C-OP202211]

Chemistry

Chemistry, Multidisciplinary

WOS:000980425100001

WILEY-V C H VERLAG GMBH

2-s2.0-85156098182

Scopus

1.School of Chemistry and Chemical Engineering,Huazhong University of Science and Technology,Wuhan,430074,China
2.State Key Laboratory of Advanced Electromagnetic Engineering and Technology,School of Electrical and Electronic Engineering,Huazhong University of Science and Technology,Wuhan,430074,China
3.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
4.College of Physics and Energy,Fujian Normal University,Fuzhou,350117,China

Wei，Chaochao,Yu，Dian,Xu，Xiangling,et al. Tailoring Electrolyte Distributions to Enable High-performance Li3PS4-based All-solid-state Batteries under Different Operating Temperatures[J]. Chemistry - An Asian Journal,2023,18(12).

Wei，Chaochao.,Yu，Dian.,Xu，Xiangling.,Wang，Ru.,Li，Jiayang.,...&Yu，Chuang.(2023).Tailoring Electrolyte Distributions to Enable High-performance Li3PS4-based All-solid-state Batteries under Different Operating Temperatures.Chemistry - An Asian Journal,18(12).

Wei，Chaochao,et al."Tailoring Electrolyte Distributions to Enable High-performance Li3PS4-based All-solid-state Batteries under Different Operating Temperatures".Chemistry - An Asian Journal 18.12(2023).