Continuous novelty as the basis for creative advance in rapidly developing different form-factor microelectronic devices requires seamless integrability of batteries. Thus, in the past decade, along with developments in battery materials, the focus has been shifting more and more towards innovative fabrication processes, unconventional configurations, and designs with multi-functional components.We present here, for the first time, a novel concept and feasibility study of a 3D-microbattery printed by fused-filament fabrication (FFF). The reversible electrochemical cycling of 3D printed lithium iron phosphate (LFP) and lithium titanate (LTO) composite polymer electrodes vs. the lithium metal anode has been demonstrated in cells containing conventional non-aqueous and ionic-liquid electrolytes. We believe that by using comprehensively structured interlaced electrode networks it would be possible not only to fabricate free form-factor batteries but also to alleviate the continuous volume changes occurring during charge and discharge.

The high areal-energy and power requirements of advanced microelectronic devices favor the choice of a lithium-ion system, since it provides the highest energy density of available battery technologies suitable for a variety of applications. Several attempts have been made to produce primary and secondary thin-film batteries utilizing printing techniques. These technologies are still at an early stage, and most currently-printed batteries exploit printed electrodes sandwiching self-standing commercial polymer membranes, produced by conventional extrusion or papermaking techniques, followed by soaking in non-aqueous liquid electrolytes. In this work, we suggest a novel flexible-battery design and report the initial results of development and characterization of novel 3D printed allsolid-state electrolytes prepared by fused-filament fabrication (FFF). The electrolytes are composed of LiTFSI, polyethylene oxide (PEO), which is a known lithium-ion conductor, and polylactic acid (PLA) for enhanced mechanical properties and high-temperature durability. The 3D printed electrolytes were characterized by means of ESEM imaging, mass spectroscopy, differential scanning calorimetry (DSC) and electrochemical impedance spectroscopy (EIS). TOFSIMS analysis reveals formation of lithium complexes with both polymers. The flexible all-solid LiTFSI-based electrolyte exhibited bulk ionic conductivity of 3 × 10 −5 S/cm at 90°C and 156ohmxcm 2 resistance of the solid electrolyte interphase (SEI). We believe that the coordination mechanism of the lithium cation by the oxygen of the PLA chain is similar to that of PEO and local relaxation motions of PLA chain segments could promote Li-ion hopping between oxygens of adjacent CH-O groups. What is meant by this is that PLA not only improves the mechanical properties of PEO, but also serves as a Li-ion-conducting medium. These results pave the way for a fully printed solid battery, which enables free-form-factor flexible geometries.

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