Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 13, Issue 6, Pages 1500-1505Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c04085
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Funding
- National Nature Science Foundation of China [21905314, 21825202, 21733012, 92045302, 21603231]
- Newton Advanced Fellowships [NAF/R2/180603]
- Scientist Studio Funding from Tianmu Lake Institute of Advanced Energy Storage Technologies Co., Ltd
- Science and Technology Service Network Initiative from Chinese Academy of Science [STS 2020T3022]
- National Science Foundation [DMR-1644779]
- State of Florida
- Fundamental Research Funds for the Central Universities , JLU
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A fundamental understanding of lithium-ion transport in polymer-inorganic composite electrolytes is crucial for the design and optimization of solid-state batteries. This study investigates the Li+ ion transport pathway in a model composite electrolyte and finds that the interface between LLZO and PEO affects the Li+ flux, especially at high current densities. The results provide an intuitive picture of Li+ ion transport in polymer-inorganic composite electrolytes, which can be helpful for optimizing and designing better composite electrolytes.
Fundamental understanding of the lithium-ion transport mechanism in polymer-inorganic composite electrolyte is crucially important for the rational design of composite electrolytes for solid-state batteries. In this work, the Li+ ion transport pathway in a model composite electrolyte of PEO containing sparsely dispersed LLZO (PEO-LLZO) was studied by an advanced characterization technique, i.e., 6Li-tracer NMR spectroscopy. By analyzing the 6Li distribution within the PEO-LLZO composite at the end of the discharge of an electrochemical cell of 6Li | PEO-LLZO | stainless steel with a fixed capacity (less than the total amount of the Li+ in the composite) at various current densities, it is found that the interfacial barrier between LLZO and PEO could cause a reduced Li+ flux through LLZO, particularly at high current densities, and therefore plays a critical role in determining the Li+ transport pathway in the composite electrolyte. This work provides an intuitive picture of Li+ ion transport in a polymer-inorganic composite electrolyte that is helpful to optimize and design better composite electrolytes.
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