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The development of bulk-type solid-state lithium-ion batteries highly requires reliable approaches to address the solid-solid interfacial issues from the viewpoints of both materials and architecture of batteries. Herein, a concept of monolithic bulk-type all-phosphate solid-state lithium-ion battery is developed and demonstrated, based on a phosphate backbone that (electro-)chemically and structurally circumvents the interphase issues. Specifically, LiTi2(PO4)3 is used as anode material, Li3V2(PO4)3 is used as cathode material and a dense Li1.3Al0.3Ti1.7(PO4)3 pellet serves as solid electrolyte. The choice of materials was primarily based on the (electro-)chemical and mechanical matching of the components instead of a solely focusing on high-performance. Thus the battery utilized a phosphate backbone in combination with tailored morphology of the electrode materials to ensure a good interfacial match for a durable mechanical stability. Moreover, the phosphate backbone leads to a high chemical stability. The operating voltage range of the electrodes matched with the intrinsic electrochemical window of the electrolyte which also resulted in a high electrochemical stability of the battery. The analysis of interfacial charge transfer kinetics confirmed the structural and electrical properties of the electrodes and their interfaces with the electrolyte, as evidenced by the excellent cycling performance of the monolithic all-phosphate solid-state battery. These interfaces have been studied via impedance analysis with subsequent distribution of relaxation times (DRT) analysis. Moreover, the prepared solid-state battery could be operated in air atmosphere owing to the low oxygen sensitivity of the phosphate materials. The analysis of electrolyte/electrode interfaces after cycling demonstrates that the interfaces remained stable during cycling. Furthermore, a prospect of potential application of the all-phosphate batteries presented in this thesis is to develop an integrated photovoltaic-battery device without any blocking diode or added electronics. The idea is proposed and confirmed by the help of a Li4Ti5O12//LiFePO4/C battery system which exhibits a similar operating potential with here presented all-phosphate batteries.

Entwicklung eines monolithischen Bulk-Typ-Festkörper-Lithium-Ionen-Akkus auf Basis von Phosphat-Materialien