Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

doi:10.1007/s40820-024-01358-9

Abstract

Abstract:

The pursuit of safer and high-performance lithium-ion batteries (LIBs) has triggered extensive research activities on solid-state batteries, while challenges related to the unstable electrode-electrolyte interface hinder their practical implementation. Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs (ASSLBs), while it introduces new concerns about thermal stability. In this study, we propose the incorporation of a multi-functional flame-retardant triphenyl phosphate additive into poly(ethylene oxide), acting as a thin buffer layer between LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode and garnet electrolyte. Through electrochemical stability tests, cycling performance evaluations, interfacial thermal stability analysis and flammability tests, improved thermal stability (capacity retention of 98.5% after 100 cycles at 60 °C, and 89.6% after 50 cycles at 80 °C) and safety characteristics (safe and stable cycling up to 100 °C) are demonstrated. Based on various materials characterizations, the mechanism for the improved thermal stability of the interface is proposed. The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature. Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.

Key words: Solid-state battery, Cathode electrolyte interlayer, Flame-retardant additive, Cycling stability, Interfacial stability

Leqi Zhao, Yijun Zhong, Chencheng Cao, Tony Tang, Zongping Shao. Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer[J]. Nano-Micro Letters, 2024, 16(1): 124-.

Leqi Zhao, Yijun Zhong, Chencheng Cao, Tony Tang, Zongping Shao. [J]. Nano-Micro Letters, 2024, 16(1): 124-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01358-9

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/124

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References 74

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Electrolyte	Cathode/anode	Operating potential (V)	Reversible capacity /current rate/cycle number/capacity retention	Temperature (°C)	References
Li_6.5Mg_0.05La₃Zr_1.6Ta_0.4O₁₂-PEO-TMOS-Pyr14FSI	NCM523/Li	3.0-4.3	124.0 mAh·g⁻¹/0.1 C/50/61.4%	55	[55]
PEO-Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PAN	NCM111/Li	3.0-4.3	108.6 mAh·g⁻¹/0.2 C/100/65%	30	[56]
Li_6.35Ga_0.15La₃Zr_1.8Nb_0.2O₁₂-SCN-3D	NCM523/Li (thin gold layer)	2.5-4.3	165.3 mAh·g⁻¹/0.1 C/100/95.0%	45	[57]
Li_6.75La₃Zr_1.75Ta_0.25O₁₂-PEO-PVDF-OX	Al₂O₃@NCM523/Li	2.5-4.3	150.6 mAh·g⁻¹/0.2 C/80/86.7%	55	[58]
Li₇La₃Zr₂O₁₂-PEO	NCM622/Li	3.0-4.3	176.4 mAh·g⁻¹/0.2 C/200/82.4%	60	[59]
Li₇La₃Zr₂O₁₂-LiBFSIE	NCM622 with liquid electrolyte/Li	2.5-4.2	113.0 mAh·g⁻¹/0.6 C/200/NR	40	[60]
PEO-PVDF-LiF-Li_6.4La₃Zr_1.4Ta_0.6O₁₂	NCM622 with LiBODFP layer/Li with PEO-3LiF-5LiDFOB layer	2.5-4.3	~ 105.0 mAh·g⁻¹/1 C/300/87.4%	60	[61]
Li_6.25Al_0.25La₃Zr₂O₁₂-PVDF-HFP-PAN	NCM811/Li	2.6-4.2	160.9 mAh·g⁻¹/0.1 C/100/92.5%	RT	[62]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEO-LiBOB-LiClO₄	NCM811/Li	2.8-4.3	190.0 mAh·g⁻¹/0.1 C/200/70.0%	25	[63]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEGDA-SCN	NCM811/Li	2.5-4.3	174.0 mAh·g⁻¹/0.2 C/200/85.4%	RT	[64]
Ga/F-Li₇La₃Zr₂O₁₂-PVDF-PAN	NCM811/ Li₂MoO₄/Li	2.7-4.2	103.8 mAh·g⁻¹/1 C/300/89.8%	25	[65]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEO-PVDF-LiTFSI-MgPFPAA	NCM811/Li	2.5-4.3	~ 162.0 mAh·g⁻¹/1 C/200/74.5%	60	[66]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂ with PEO-TPP-LiTFSI Interlayer	NCM811/Li-LLTO	2.8-4.3	136.0 mAh·g⁻¹/1 C/300/82.3%	60	This work
Li_6.4La₃Zr_1.4Ta_0.6O₁₂ with PEO-TPP-LiTFSI Interlayer	NCM811/Li-LLTO	2.8-4.3	162.0 mAh·g⁻¹/1 C/50/89.6%	80	This work

Electrolyte	Cathode/anode	Operating potential (V)	Reversible capacity /current rate/cycle number/capacity retention	Temperature (°C)	References
Li_6.5Mg_0.05La₃Zr_1.6Ta_0.4O₁₂-PEO-TMOS-Pyr14FSI	NCM523/Li	3.0-4.3	124.0 mAh·g⁻¹/0.1 C/50/61.4%	55	[55]
PEO-Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PAN	NCM111/Li	3.0-4.3	108.6 mAh·g⁻¹/0.2 C/100/65%	30	[56]
Li_6.35Ga_0.15La₃Zr_1.8Nb_0.2O₁₂-SCN-3D	NCM523/Li (thin gold layer)	2.5-4.3	165.3 mAh·g⁻¹/0.1 C/100/95.0%	45	[57]
Li_6.75La₃Zr_1.75Ta_0.25O₁₂-PEO-PVDF-OX	Al₂O₃@NCM523/Li	2.5-4.3	150.6 mAh·g⁻¹/0.2 C/80/86.7%	55	[58]
Li₇La₃Zr₂O₁₂-PEO	NCM622/Li	3.0-4.3	176.4 mAh·g⁻¹/0.2 C/200/82.4%	60	[59]
Li₇La₃Zr₂O₁₂-LiBFSIE	NCM622 with liquid electrolyte/Li	2.5-4.2	113.0 mAh·g⁻¹/0.6 C/200/NR	40	[60]
PEO-PVDF-LiF-Li_6.4La₃Zr_1.4Ta_0.6O₁₂	NCM622 with LiBODFP layer/Li with PEO-3LiF-5LiDFOB layer	2.5-4.3	~ 105.0 mAh·g⁻¹/1 C/300/87.4%	60	[61]
Li_6.25Al_0.25La₃Zr₂O₁₂-PVDF-HFP-PAN	NCM811/Li	2.6-4.2	160.9 mAh·g⁻¹/0.1 C/100/92.5%	RT	[62]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEO-LiBOB-LiClO₄	NCM811/Li	2.8-4.3	190.0 mAh·g⁻¹/0.1 C/200/70.0%	25	[63]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEGDA-SCN	NCM811/Li	2.5-4.3	174.0 mAh·g⁻¹/0.2 C/200/85.4%	RT	[64]
Ga/F-Li₇La₃Zr₂O₁₂-PVDF-PAN	NCM811/ Li₂MoO₄/Li	2.7-4.2	103.8 mAh·g⁻¹/1 C/300/89.8%	25	[65]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂-PEO-PVDF-LiTFSI-MgPFPAA	NCM811/Li	2.5-4.3	~ 162.0 mAh·g⁻¹/1 C/200/74.5%	60	[66]
Li_6.4La₃Zr_1.4Ta_0.6O₁₂ with PEO-TPP-LiTFSI Interlayer	NCM811/Li-LLTO	2.8-4.3	136.0 mAh·g⁻¹/1 C/300/82.3%	60	This work
Li_6.4La₃Zr_1.4Ta_0.6O₁₂ with PEO-TPP-LiTFSI Interlayer	NCM811/Li-LLTO	2.8-4.3	162.0 mAh·g⁻¹/1 C/50/89.6%	80	This work

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