Energy Materials for Sustainable Development: Storage Batteries I
Sponsored by: ACerS Energy Materials and Systems Division
Program Organizers: Krista Carlson, University of Nevada, Reno; Armin Feldhoff, Leibniz University Hannover; Kyle Brinkman, Clemson University; Eva Hemmer, University of Ottawa; Nikola Kanas, BioSense Institute; Kjell Wiik, Norwegian University of Science and Technology; Lei Zuo, Virgina Tech; Joshua Tong, Clemson University ; Danielle Benetti, Institut National de la Recherche Scientifique; Katherine Develos-Bagarinao, National Institute of Advanced Industrial Science and Technology; Soumi Chatterjee, Aditya Birla Science & Technology Company, Ltd

Monday 8:00 AM
October 10, 2022
Room: 413
Location: David L. Lawrence Convention Center

Session Chair: Kyle Brinkman , Clemson University ; Krista Carlson, University of Nevada, Reno; Armin Feldhoff, Leibniz Universität Hannover


8:00 AM Introductory Comments

8:10 AM  Invited
Design, Modeling, and Direct Write Additive Manufacturing (DWAM) of Electrodes for Batteries: Amjad Almansour1; Roy Sullivan1; Mrityunjay Singh2; Michael Halbig1; Daniel Gorican3; 1NASA Glenn Research Center; 2Ohio Aerospace Institute at NASA Glenn; 3HX5, LLC at NASA Glenn
    There are critical needs for light weight and multifunctional compact energy systems which can be manufactured on-demand and can store as well as rapidly discharge the energy, and provide optimum mission performance. To meet the above needs, modeling and additive manufacturing technologies were leveraged to design and produce engineered three-dimensional (3D) electrode structures with increased interfacial area which yields increased power and energy densities. In this work, a novel engineered three-dimensional interdigitated Lithium Iron Phosphate LiFePO4 (LFP) cathode structure was designed and manufactured using direct-write additive manufacturing technology (DWAM). Ink rheology was adjusted to optimize material characteristics of the final electrodes, including the addition of carbon nanoparticles. Printed cathodes were sintered and microstructural characterization was carried out. In addition, modeling of the electrochemical performance of a 3D galvanic cell was performed and compared to that of conventional 1D planar cells and the benefits of the 3D structures were summarized.

8:40 AM  
Ceramic-based Solid-state Sodium-ion Batteries Fabricated in a Single Step via Cold Sintering: Zane Grady1; Julian Fanghanel1; Clive Randall1; 1Penn State
     One of the most prominent solid-state battery (SSB) challenges is the development of processing techniques that allows for the unification of ceramic solid electrolytes with an array of other useful battery materials, including electrode active materials and conductive carbon additives. Specifically, high ceramic sintering temperatures preclude (1) sintering of bulk composites containing dissimilar ceramics and organic materials and (2) the co-sintering of layered structures of solid-state electrodes and electrolytes with low interfacial impedance. We apply a low-temperature sintering technique, cold sintering, to densify ceramic materials below 400°C. This is applied to prototypical sodium SSB materials to produce dense composites with minimal chemical interaction between constituent phases. An array of composite compositions are cold sintered, demonstrating a systematic optimization approach to SSB design. Subsequently, we demonstrate the ability to cold sinter layers of electrodes and electrolytes with conductive interfaces allowing for cycling at practical temperatures.

9:00 AM  
Molecular Pathways to Al2S3 for Next Generation Battery Application: Chijioke Amadi1; Veronika Brune1; Michael Wilhelm1; Sanjay Mathur1; 1University of Cologne
    The increasing global population, and ever-growing energy demand calls for game-changing research strategy for electrochemical energy storage. Substantial progress in battery technology is essential if we are to succeed in an energy transition towards a more carbon-neutral society. Rechargeable aluminum batteries have recently reached great attention due to its excellent safety, natural abundance of aluminum and as well as its high theoretical capacity. The highly natural reactivity of Al2S3 with moisture and oxygen faces challenges in high quality battery applications. To control target Al2S3 material preparation we demonstrate a molecular approach by single molecular synthesis. By introducing a chelating thiol-containing ligand to suitable aluminum sources the reactivity and stability of as-prepared molecular precursors [Al2(SC2H4N(Me)C2H4S)3] and [AlH(SC2H4N(Me)C2H4S)] can be controlled. Fully characterized single molecular precursors enable a direct and sustainable material preparation by preformed Al-S bonds in thermal decomposition experiments.

9:20 AM  
Self-propagating High Temperature Synthesis of Chevrel Phase Sulfides from Elemental Precursors: Tessa Gilmore1; Pelagia-Irene Gouma1; 1The Ohio State University
    Self-propagating high temperature synthesis (SHS) is a spontaneous, irreversible, combustion process that requires close to no energy to produce complex materials at high temperature through self-sustained reactions. Little is known about the mechanistic nature of this versatile process, which limits its controllability and applicability. Chevrel Phase (CP) compounds (MxMo6S8-CPs) constitute a class of multifunctional, ceramic, designer materials targeted for catalysis, battery electrodes, quantum computing, and other applications. In this research, the successful and rapid processing of the sulfide Chevrel compound Cu4Mo6S8 via SHS is demonstrated, and a mechanism is provided. Thermochemical measurements identify an atypical behavior for this SHS process where the overall reaction temperature does not surpass that of the materials with the lowest melting point. This result is attributed to intercalation assisted massive phase transformation facilitated by the use of a MoS2 precursor. Further work to synthesize the Chevrel phase using other cations is continuing.

9:40 AM  Invited
Processing and Characterization of Li7La3Zr0.5Nb0.5Ta0.5Hf0.5O12 High-entropy Li-garnet Electrolyte: Zhezhen Fu1; 1University of Wisconsin-Platteville
    We demonstrated the processing of Li7La3Zr0.5Nb0.5Ta0.5Hf0.5O12 high-entropy Li-garnet with promising properties for lithium batteries. We first synthesized the LLZNTH Li-garnet powders which have a single cubic garnet phase without any secondary phases as well as uniform elements distributions. The prepared powders were further densified to a relative density of ~94% with well-crystallized grains and a good contact area with the neighboring grains. Minimal grain growth can be observed in the sintering time range from 8 hours to 20 hours, likely due to high-entropy compounds' sluggish effects. The sample also maintains the cubic garnet phase and uniform elements distribution after sintering. Electrochemical characterizations indicate that the densified sample has an adequate ionic conductivity of 4.67×10-4 S cm-1 at room temperature, a low activation energy of 0.25eV, and a low electronic conductivity in the order of 10-8 S cm-1. Mechanical properties are also studied.

10:00 AM Break

10:20 AM  
Cycling Demonstration of Sequential Deposition Synthesis-synthesized Lithium Garnet Films in Full Batteries: Jesse Hinricher1; Chae-Ah Kim2; Heung Chan Lee3; Lincoln Miara2; Won Seok Chang3; Andrea Maurano2; Jeong-Ju Cho2; Zachary Hood1; Jennifer Rupp1; 1Massachusetts Institute of Technology; 2Samsung Research America; 3Samsung Advanced Institute of Technology
    Sequential deposition synthesis (SDS) is a recently-discovered technique that allows a solid-state electrolyte layer to be fabricated directly from a liquid precursor which is then atomized onto a heated substrate where the solvent evaporates and the precursor salts decompose to form a conformal layer. Li7La3Zr2O12 (LLZO) is a promising material that has seen much interest in the battery field but has challenges to synthesize this layer between 5-15 µm thick which SDS is capable of fabricating. LLZO films were fabricated directly onto a porous substrate that was infiltrated with a polymer gel electrolyte and the cycling performance was demonstrated in a full cell using Li metal anode and lithium cobalt oxide (LCO) cathode. The cycling performance is discussed in reference to state-of-the-art performance in the battery field and post-mortem analysis on the cells is performed to elucidate failure mechanisms.

10:40 AM  
Electrospun Vanadium Pentoxide Nanofibers as a Photocathode in a Light Rechargeable LIB: Michael Wilhelm1; Ruth Adam1; Aman Bhardwaj1; Veronika Brune1; Sanjay Mathur1; 1University of Cologne
     Sunlight is the most sustainable energy source on earth, which can be harvested and converted into electricity. This harvested energy must be immediately used or stored electrochemically. Lithium-ion batteries (LIB) are currently one of the most promising techniques to do so. The innovative way of a so-called “photo battery” using a shared electrode, as both, energy harvester and storage, could be an innovative way to play a big role in terms of renewable energy. Vanadium pentoxide (V2O5) has a suitable band gap (2.35 eV) and good theoretical capacity value (294 mAh g-1 for 2 Li+) to work as both. Within here, we report electrospun vanadium pentoxide nanofibers (VNF) and carbon-coated VNF by plasma-enhanced chemical vapor deposition. Under light illumination, the discharge capacity could be increased. Further, the materials could be charged only by light to power a LED and achieve promising overall conversion efficiencies.

11:00 AM  
Synthesis of Ce-Doped NaSICON Using Mechanical-Activation-Enhanced-Process: Brian Johnston1; 1North Central College
    Natrium Super Ionic Conductor (NaSICON) is one of the most promising solid electrolytes due to high ionic conductivity at room temperature, thermal stability, and good mechanical strength. In addition, the demand for long-lasting, cost-effective, and safer solid-state batteries has increased drastically which makes it even more attractive. However, the state-of-art developments have been impeded due to the lack of sustainable solid-electrolyte materials. Furthermore, no manufacturing method is available today to fabricate ultra-high purity yet fully dense NaSICON at low cost. In this study, we demonstrate, for the very first time that cerium-doped NaSICON (Na3Zr1.9Ce0.1Si2PO12) with relative density higher than 97% can be manufactured through one mechanical-activation-enhanced-process and one high temperature reaction. The powder processing, sintering condition as well as the ionic conductivity will be discussed.