Lithiation-induced conductivity modulation in Prussian blue interlayer for stable Li/garnet solid-state batteries

Author:

Zhang Bo12ORCID,Zhang Yang23,Hu Jiulin24ORCID,Lei Meng24ORCID,Shen Zong-Yang1ORCID,Li Chilin234ORCID

Affiliation:

1. School of Materials Science and Engineering, Jingdezhen Ceramic University 1 , Jingdezhen 333403, China

2. CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences 2 , Shanghai 201899, China

3. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences 3 , Beijing 100049, China

4. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences 4 , Shanghai 201899, China

Abstract

The garnet-based solid-state batteries have the potential advantages of high energy density and safety. However, the poor solid–solid contact and Li dendrite growth at the anode interface lead to uneven Li deposition or short circuit, which hinders their practical application. Here, we propose a Prussian blue (PB) interlayer to improve the interface contact and charge transfer between Li anode and garnet electrolyte by lithiation-induced conductivity modulation. This mixed-conducting interlayer with unique 3D open framework enables a well welded interface with enhanced lithiophilicity and uniform Li diffusion. The Li/garnet interface resistance is significantly reduced. This lithiated PB interlayer is highly durable with invariable thickness during cycling, leading to a highly stable cycling of Li plating/stripping and corresponding LiFePO4 full cells without dendrite growth. The dual modulation of ion and electron transports in an integrated structure without phase segregation through thermal or electrochemical lithiation provides a solution to the challenge of solid–solid interfaces and the development of practical solid-state batteries.

Funder

National Natural Science Foundation of China

Publisher

AIP Publishing

Subject

Physics and Astronomy (miscellaneous)

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