Advanced Materials for Energy Conversion and Storage 2023: Energy Storage with Battery III
Sponsored by: TMS Functional Materials Division, TMS: Energy Conversion and Storage Committee
Program Organizers: Jung Choi, Pacific Northwest National Laboratory; Amit Pandey, Lockheed Martin Space; Partha Mukherjee, Purdue University; Surojit Gupta, University of North Dakota; Soumendra Basu, Boston University; Paul Ohodnicki, University Of Pittsburgh; Eric Detsi, University of Pennsylvania
Thursday 8:30 AM
March 23, 2023
Room: 32B
Location: SDCC
Session Chair: Marm Dixit, Oak Ridge National Laboratory; Leon Shaw, Illinois Institute of Technology
8:30 AM Invited
Opportunities and Challenges for In Situ Synchrotron Characterization of All Solid State Batteries: Marm Dixit1; 1Oak Ridge National Laboratory
Next generation energy storage systems will need to leverage high energy density anodes, like Li to achieve the required performance metrics (longer vehicle range, long life, production costs, safety). Solid electrolytes (SEs) are promising materials for achieving these metrics by enabling Li metal anodes and high voltage cathodes, but SE cells suffer from poor coulombic efficiencies as well as lifetimes which impede their integration into EVs. We discuss several promising solid electrolytes and their underlying processing-structure-function relationships using in situ synchrotron techniques to elicit the mechanisms of failure within these systems. Electrolyte structure anisotropy is identified to be a key factor that initiates failures in solid electrolytes. Subsequently, I will discuss some ongoing work pertaining to development of operando cells for SSB testing. Finally, I will discuss potential research questions of fundamental interest with regards to solid|solid interfaces that can benefit tremendously from directed efforts of leveraging advanced diffraction techniques.
8:55 AM
On the Specific Capacity and Cycle Stability of Si Anodes: Effects of Charge/Discharge Protocol: Bingyu Lui1; Mei Luo1; Ziyong Wang1; Christopher Passolano1; Leon Shaw1; 1Illinois Institute of Technology
Silicon has potential to be a high-performance anode material, but its practical application is impeded by huge volume expansion during lithiation. Here we show that by introducing engineered voids into a Si/C core-shell structure to form Si@void@C structure, volume expansion of Si@void@C particles can be minimized, thereby improving the cycle stability. We further investigate the effects of charge/discharge protocol, showing that lower and upper cutoff voltages in charge/discharge have profound impact on the specific capacity and cycle stability. Importantly, cutoff voltages in formation cycles have long-lasting effects on the cycle stability, indicating the critical role of forming a robust SEI layer during formation cycles. Using constant current charge followed by potentiostatic hold charge can further improve the cycle stability. With proper choices of charge/discharge protocols, the specific capacity of Si@void@C anodes at the electrode level is 71% higher than that of graphite anodes over 300 cycles with 82% capacity retention.
9:15 AM Invited
Operando Degradation Analytics Using 3ε Toolbox: Sobana Perumaram Rangarajan1; 1General Motors
Understanding degradation and failure of lithium-ion batteries (LIB) is critical for the safe and reliable operation of electric vehicles. Tracking degradation over time is crucial to develop technologies for battery prognostics. Prognostics of LIBs is however challenging due to the interdependence of degradation mechanisms stemming from different electrodes, usage history and operating conditions. Three-electrode (3å) cells offer a convenient operando platform to examine and deconvolute the fundamental reaction mechanisms responsible for electrode degradation under a variety of operational extremes. By employing an array of recently developed data analytics techniques and parameters using the reference electrode measurements, three-electrode cells can be used as an analytics toolbox for identifying the fundamental degradation mechanisms and its observable consequences at the cell level.
9:40 AM Invited
Physics-based Understanding of Heterogeneous Nucleation during Lithium Electrodeposition: Aashutosh Mistry1; Venkat Srinivasan1; 1Argonne National Laboratory
Lithium metal anodes are required to transform the present-day Li-ion batteries for storing more energy. A key challenge is to ensure uniform electrodeposition of lithium when the cell is being charged. While most previous studies examine the efficacy of various mechanisms in regularizing an uneven interface, the formation of the uneven interface is poorly understood. Whenever lithium deposits on a surface other than pristine lithium, nucleation is observed. Physics-based understanding of this step is essential to identify the factors that govern nucleation and cause nonuniform growth. In this talk, we propose a theoretical description of lithium nucleation and growth during electrodeposition. We show that nucleation during electrodeposition differs from the metallurgical understanding of melt solidification. We correlate such theoretical understanding with experimental observations. We discuss material property targets to tune the nonuniformity associated with the nucleation and early time growth of electrodeposited lithium.
10:05 AM Break
10:25 AM
Rate, Size, and Temperature Effects in Alkali Metal Anodes: Matt Pharr1; 1Texas A&M University
Li, Na, and K, are ideal anode materials for rechargeable batteries, as they possess the largest theoretical capacities in their respective systems. However, when integrated with liquid electrolytes, they readily form dendrites, which leads to severe safety and cyclability issues. Even when paired with solid electrolytes, several issues still arise, including electrolyte fracture, metal penetration through the electrolyte, and/or loss of anode-electrolyte contact. This talk will discuss experimental studies of the mechanical behavior of Li, Na, and K over various strain rates, length scales, and temperatures. Temperature/size-dependent deformation mechanism maps emerge, enabling prediction of stresses that can develop in these metals under a broad range of operating conditions. I will also analyze how “size effects” may affect the stresses generated in metal protrusions at the solid electrolyte / anode interface. More broadly, this talk will outline the impact of the mechanical properties on the performance of solid-state batteries.
10:45 AM Invited
Ultra-Thick Electrodes for High Energy and Power Density Lithium-ion Batteries: Jonghyun Park1; Tazdik Plateau1; Hiep Pham1; 1Missouri University of Science and Technology
Thickening electrodes is one effective way to increase active material content in electrodes to achieve high energy density and reduce cost of batteries. However, limitation of charge transport in thick electrodes and the generation of mechanical stresses result in poor performance and eventual cell failure. In this work, a new electrode fabrication process, referred to as µ-casting, is developed, which enables ultra-thick electrodes that address the trade-off between specific capacity and areal/volumetric capacity. The process facilitates a short diffusion path structure that minimizes intercalation-induced stress, improving energy density and cell stability. We also investigated the issues with structural integrity, porosity and paste rheology, and analyzed mechanical properties due to external force. The µ-casting enables an ultra-thick electrode that effectively utilizes active materials compared to conventional thick electrodes, allowing high-mass loading, 40% higher specific capacity and 30% higher areal capacity after 200 cycles, high C-rate performance and longer cycle life.
11:10 AM Invited
Understanding Improved Alkali Metal Plating of Sodium Compared to Lithium via 2DIR characterization and MD Simulation of Weaker Solvation Behavior for High Energy Battery Systems: Rachel Carter1; Cynthia Pyles1; Michael Swift1; Matthew Lefler1; Susmita Sarkar2; Adam Dunkelberger1; Partha Mukherjee2; 1US Naval Research Laboratory; 2Purdue Universtiy
Next generation battery systems replace intercalation anodes, which store alkali ions, with the pure alkali metals. This configuration requires the alkali ions to plate and strip with high coulombic efficiency and smooth morphology. Lithium is the highest energy density alkali metal. However, sodium has much higher global abundance, making it an attractive second choice. We use in situ optical microscopy to compare Na and Li plating and stripping in 1 M MeTFSi (Me: Li or Na) FEC. We observe more desirable morphology for Na. Novel 2DIR measurements indicate weaker interaction between the FEC carbonyl and the Na+ compared to the Li+ and distinct ultrafast molecular dynamics between the two systems. MD Simulations of bond length and coordination number corroborate these observations. The inherently weaker binding of Na+ ions with the electrolyte solvent provides higher columbic efficiency plating and stripping via more desirable morphologies.
11:35 AM Keynote
Designing Electrode Architectures Across Length Scales: Sarbajit Banerjee1; 1Texas A&M University
The design and operation of rechargeable batteries is predicated on directing flows of mass, charge, and energy across multiple interfaces. Understanding such flows requires knowledge of atomistic and mesoscale diffusion pathways and the coupling of ion transport with electron conduction and stress gradients across length scales. Using multiple polymorphs of V2O5 as model systems, I will discuss our efforts to develop an Angstrom-level view of diffusion pathways using single-crystal X-ray diffraction studies of topochemical transformations. I will further discuss the accumulative results of atomic scale inhomogeneities at single-particle and particle ensemble levels based on scanning transmission X-ray microscopy and X-ray ptychography measurements of lithiation inhomogeneities and stress gradients. The mitigation of diffusion impediments will be discussed with reference to two distinct approaches: (a) utilization of Riemann manifolds as a geometric design principle for electrode architectures and (b) the atomistic design of polymorphs with well-defined diffusion pathways that provide frustrated coordination.