1Shenzhen Key Laboratory of Advanced Energy Storage, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
2Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
3SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
4Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology, Kowloon, 997077 Hong Kong Special Administrative Region of China, People’s Republic of China
5HKUST Shenzhen-Hong Kong Collaborative Innovation Research Institute, Futian, Shenzhen, People’s Republic of China
【AIGC One Sentence Reading】:3D printed composite solid electrolytes enhance ASSLMBs' stability, energy density, and cycle life at room temperature.
【AIGC Short Abstract】:This study develops 3D-printed composite solid electrolytes with vertical-aligned and spiral structures for all-solid-state lithium metal batteries, enhancing Li+ transport and interfacial adhesion. The design achieves robust cycle life, high current density, and superior areal capacity, addressing interfacial degradation and contact loss issues at room temperature.
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Abstract
Improving the long-term cycling stability and energy density of all-solid-state lithium (Li)-metal batteries (ASSLMBs) at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport. Solid electrolytes are generally studied as two-dimensional (2D) structures with planar interfaces, showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces. Herein, three-dimensional (3D) architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment. Multiple-type electrolyte films with vertical-aligned micro-pillar (p-3DSE) and spiral (s-3DSE) structures are rationally designed and developed, which can be employed for both Li metal anode and cathode in terms of accelerating the Li+ transport within electrodes and reinforcing the interfacial adhesion. The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm-2. The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm-2 (LFP) and 3.92 mAh cm-2 (NCM811). This unique design provides enhancements for both anode and cathode electrodes, thereby alleviating interfacial degradation induced by dendrite growth and contact loss. The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.