Robust polymer electrolytes with fast ion-transport nanochannels constructed by carbon dots for long lifespan Li metal batteries

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 500; p. 157379
• Main Authors: Ni, Jia-Wen, Zhang, Xi-Rong, Song, Tian-Bing, Huang, Zun-Hui, Ma, Qian-Li, He, Tian-Le, Xiong, Huan-Ming
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 15.11.2024
• Subjects: Carbon dot; Ion-transport channel; Lithium metal battery; Phase inversion; Polymer electrolyte; Ion-transport channel; Phase inversion; Carbon dot; Polymer electrolyte; Lithium metal battery
• DOI: 10.1016/j.cej.2024.157379
• ISSN: 1385-8947

[Display omitted] •Novel PVDF-HFP/CDs based GPEs with vertical nanochannels for lithium transport.•High ionic conductivities and Li ion transference numbers at room temperature.•Excellent electrochemical performance of the Li||Li symmetric cells, Li||Cu semi cells, Li||LFP and Li||LCO full cells. As an anode material in energy storage systems, Li metal has exceptional merits, including high specific capacity, low density, and low redox potential. However, challenges such as lithium dendrites and unstable solid electrolyte interphase (SEI) hinder the practical application of lithium metal batteries (LMBs). Solid polymer electrolytes (SPEs), notably PVDF-HFP, are expected to overcome the above problems because of their mechanical merits and safe features, but their limited ion transportation behaviors result in insufficient ionic conductivity at room temperature. Herein, we invent an approach to prepare high performance electrolytes composed by porous PVDF-HFP and functionalized carbon dots (CDs). Such porous PVDF-HFP polymer membranes are created by a subtle phase inversion process, possessing a sponge-like structure, vertical lithium-ion transport channels and CDs decorated surfaces, thus able to uptake the liquid electrolyte (LE) to form gel polymer electrolytes (GPEs). The CDs fillers are produced in large scale with adjustable surface states, which can enhance Li salts disassociation to release free Li ions. As a result, the optimal conductivity of the as-prepared GPEs at room temperature is up to 8.7 mS cm−1 and the lithium transference number reaches 0.64. Our GPEs endow Li symmetric batteries with very stable SEI and long cycling life over 2200 h, and help realize high capacities and retention rates of the LMBs using LiFePO4(LFP) or LiCoO2(LCO) cathodes.