2-Dimensional g-C3N4 nanosheets modified LATP-based “Polymer-in-Ceramic” electrolyte for solid-state lithium batteries

Composite polymer electrolytes (CPEs) are gaining increasing interest due to their combined advantages of polymer and inorganic ceramic. "Polymer-in-Ceramic" (PIC) system containing a large portion of ceramic fillers (higher than 50 wt%), possesses superior safety, electrochemical and mechanical properties, which render it a promising strategy for mass production of inorganic ceramic electrolytes. However, the poor organic-inorganic interface compatibility between polymer and ceramic leads to severe agglomeration of ceramic fillers within the polymer electrolyte, resulting in cracks in the membrane that impedes the transportation of lithium ions. Thus, two-dimensional (2D) g-C3N4 nanosheets are introduced into the PIC-type electrolyte as a bridge between the organic and inorganic components to improve the homogeneity of the electrolyte membrane and build an effective transportation network. In this work, a PIC type g-C3N4/ Li1.3Al0.3Ti1.7(PO4)3(LATP)/Poly(vinylidene fluoride) (PVDF) electrolyte membrane with a thickness of 35.2 µm is prepared via a simple solution-casing method and delivers satisfactory all-around properties (a high conductivity of 5.9 × 10−4 S cm−1 at 25 ℃, a high lithium-ion transference number of 0.63 and superior thermal stability). To further evaluate its practicability, a solid-state lithium battery of LiNi0.8Mn0.1Co0.1O2|CPEs|Li is assembled and provides good cycling and rate performance at room temperature. This work proves the effectiveness of the 2D g-C3N4 nanosheets in resolving the agglomeration issue and optimizing the electrochemical properties of LATP-based polymer-in-ceramic electrolyte, which provides a universal strategy to modify the PIC-type solid-state electrolytes.