AVS 66th International Symposium & Exhibition
    Thin Films Division Monday Sessions
       Session TF-MoM

Paper TF-MoM4
Organic/Inorganic Solid Electrolytes and Electrode Coatings for 3D Lithium-ion Microbatteries

Monday, October 21, 2019, 9:20 am, Room A124-125

Session: Thin Films for Electrochemistry and Energy Storage
Presenter: Ryan Sheil, University of California, Los Angeles
Authors: R. Sheil, University of California, Los Angeles
J. Lau, University of California, Los Angeles
K. Jungjohann, Sandia National Laboratories
J. Yoo, Los Alamos National Laboratory
B. Dunn, University of California, Los Angeles
J.P. Chang, University of California, Los Angeles
Correspondent: Click to Email

Lithium-ion batteries have been an enabling factor in the success of consumer electronics and have the potential to offer energy storage solutions for microelectromechanical systems (MEMS), such as sensors for IoT and biomedical applications. Three-dimensional battery architectures allow for an effective decoupling of the areal energy and power density resulting in improved areal footprint utilization required of these small devices. In 3D battery designs, the short distances between the anode and cathode improve the transport properties allowing for high areal power densities and the high aspect-ratio nature of the electrodes promotes high areal energy densities. One requirement in the utilization of 3D based electrodes is the incorporation of a solid electrolyte that can be coated pinhole free and conformally on high aspect ratio structures. The solid electrolyte material must be ionically conductive, electronically insulating, and be flexible to withstand the volume expansion and contraction of the electrode during charge and discharge.

The self-limiting nature of atomic layer deposition allows for precise thickness control across high aspect ratio structures. ALD LixAlySizO was synthesized utilizing lithium tert-butoxide (LTB), trimethyl aluminum (TMA), and tris(tert-butoxy) silanol (TTBS). ALD LixAlySizO was integrated with high aspect ratio SiGe nanowires for in-situ TEM characterization, where the chemical, structural, and morphological changes of the electrode/electrolyte system were characterized in-situ during lithiation and delithiation. An ALD LixAlySizO-coated Si0.4Ge0.6 nanowire demonstrates lithiation and delithiation with an intact solid state electrolyte layer with ~39% radial expansion observed upon lithiation. To further improve the mechanical properties for integration on high capacity/large volume expansion anodes, an MLD process was explored to synthesize lithium alkoxide and aluminum alkoxide utilizing trimethyl aluminum and lithium tert-butoxide coupled with glycerol. Incorporation of the MLD, ALD, and MLD/ALD coatings were integrated with Si and Co3O4 elecrodes, where improvements to cycling stability and coulombic efficiency were observed. LixAlySizO coated Co3O4 thin films exhibited improved coulombic efficiency (99.5% (coated), 90.5% (uncoated) and capacity retention (2458 mAh/cm3 (coated), 2038 mAh/cm3 (uncoated)) after 100 cycles at 2C.