Papers by Jonathan Scharf
Nature Nanotechnology, Apr 12, 2022
Nature Communications, Jun 7, 2021
arXiv (Cornell University), May 7, 2021
Meeting abstracts, Oct 19, 2021
Lithium metal has been an attractive candidate as a next-generation anode material. Despite its p... more Lithium metal has been an attractive candidate as a next-generation anode material. Despite its popularity, stability issues of lithium in the liquid electrolyte and the formation of lithium whiskers have kept it from practical use. Three-dimensional (3D) current collectors have been proposed as an effective method to mitigate whisker growth. Although extensive research has been done, the effects of three key parameters of the 3D current collectors, namely, the surface area, the tortuosity factor, and the surface chemistry, on the performance of lithium metal batteries remain elusive. Herein, we quantitatively studied the role of these three parameters by synthesizing four types of porous copper networks with different sizes of well-structured microchannels. X-ray microscale computed tomography (micro-CT) allowed us to assess the surface area, the pore size, and the tortuosity factor of the porous copper materials. A metallic Zn coating was also applied to study the influence of surface chemistry on the performance of the 3D current collectors. The effects of these parameters on the performance were studied in detail through scanning electron microscopy (SEM) and titration gas chromatography (TGC). Stochastic simulations further allowed us to interpret the role of the tortuosity factor in lithiation. The optimal range of the key parameters is thereby found for the porous coppers and their performance is predicted. Using these parameters to inform the design of porous copper anodes for Li deposition, Coulombic efficiencies (CEs) of up to 99.63% are achieved, thus paving the way for the design of effective 3D current collector systems.
arXiv (Cornell University), Feb 7, 2021
Sodium ion migration has been implicated in potential induced degradation of the shunting type. T... more Sodium ion migration has been implicated in potential induced degradation of the shunting type. The kinetics of sodium migration in silicon nitride can be investigated using a simple capacitance-voltage characterization technique. However, we show that the charge trapping strongly affects the measurement and must be taken into consideration in the experimental approach. We perform a systematic analysis of charge carrier trapping in silicon nitride, allowing us to correct trapping effects that otherwise prevent sodium signal detection. We extract trapping and detrapping time constants both on the order of several hours. This shows that trapping cannot be ignored as it occurs relatively quickly and is constantly evolving in time. Accurate determination of sodium behavior in dielectric layers will facilitate robust co-optimization of these layers for optical, passivation, and barrier properties.
Nature Nanotechnology
X-ray Computed Tomography (X-ray CT) is a well-known non-destructive imaging technique where cont... more X-ray Computed Tomography (X-ray CT) is a well-known non-destructive imaging technique where contrast originates from the materials' absorption coefficients. Novel battery characterization studies on increasingly challenging samples have been enabled by the rapid development of both synchrotron and laboratory-scale imaging systems as well as innovative analysis techniques. Furthermore, the recent development of laboratory nano-scale CT (NanoCT) systems has pushed the limits of battery material imaging towards voxel sizes previously achievable only using synchrotron facilities. Such systems are now able to reach spatial resolutions down to 50 nm. Given the non-destructive nature of CT, in-situ and operando studies have emerged as powerful methods to quantify morphological parameters, such as tortuosity factor, porosity, surface area, and volume expansion during battery operation or cycling. Combined with powerful Artificial Intelligence (AI)/Machine Learning (ML) analysis techniques, extracted 3D tomograms and battery-specific morphological parameters enable the development of predictive physics-based models that can provide valuable insights for battery engineering. These models can predict the impact of the electrode microstructure on cell performances or analyze the influence of material heterogeneities on electrochemical responses. In this work, we review the increasing role of X-ray CT experimentation in the battery field, discuss the incorporation of AI/ML in analysis, and provide a perspective on how the combination of multi-scale CT imaging techniques can expand the development of predictive multiscale battery behavioral models.
physica status solidi (a), 2020
A trap‐corrected bias–temperature–stress (TraC‐BTS) method to quantify the kinetics of ion migrat... more A trap‐corrected bias–temperature–stress (TraC‐BTS) method to quantify the kinetics of ion migration in dielectrics based on capacitance–voltage measurements is presented. The method is based on the extraction of flatband potential (Vfb) shifts in metal–insulator–semiconductor test structures an enables the reliability assessment of semiconductor dielectrics and solar cells. Herein, it is shown that carrier trapping in the dielectric must be accounted for, as it strongly affects the measurement of flatband potential in silicon‐nitride‐based capacitors. This effect is corrected by isolating the contribution of trapping on Vfb using contamination‐free control devices. A specific drift‐diffusion model of the ion kinetics presented herein allows the extraction of ion diffusivity. An Arrhenius relationship is obtained for sodium diffusivity in silicon nitride in a temperature range from 30 °C to 90 °C at an electric field of 1 MV cm−1, yielding a prefactor and an activation energy , with...
Advanced Energy Materials, 2021
To meet growing energy demands, degradation mechanisms of energy storage devices must be better u... more To meet growing energy demands, degradation mechanisms of energy storage devices must be better understood. As a non‐destructive tool, X‐ray Computed Tomography (CT) has been increasingly used by the battery community to perform in situ experiments that can investigate dynamic phenomena. However, few have used X‐ray CT to study representative battery systems over long cycle lifetimes (>100 cycles). Here, the in situ CT study of Zn–Ag batteries is reported and the effects of current collector parasitic gassing over long‐term storage and cycling are demonstrated. Performance representative in situ CT cells are designed that can achieve >250 cycles at a high areal capacity of 12.5 mAh cm−2. Combined with electrochemical experiments, the effects of current collector parasitic gassing are revealed with micro‐scale CT. The volume expansion and evolution of ZnO and Zn depletion are quantified with cycling and elevated temperature testing. The experimental insights are utilized to dev...
Science, 2021
Silicon anode solid-state batteries Research on solid-state batteries has focused on lithium meta... more Silicon anode solid-state batteries Research on solid-state batteries has focused on lithium metal anodes. Alloy-based anodes have received less attention in part due to their lower specific capacity even though they should be safer. Tan et al . developed a slurry-based approach to create films from micrometer-scale silicon particles that can be used in anodes with carbon binders. When incorporated into solid-state batteries, they showed good performance across a range of temperatures and excellent cycle life in full cells. —MSL
ACS Applied Energy Materials, 2021
Joule, 2021
The rise of flexible electronics calls for cost-effective and scalable batteries with good mechan... more The rise of flexible electronics calls for cost-effective and scalable batteries with good mechanical and electrochemical performance. In this work, we developed printable, polymerbased AgO-Zn batteries that feature flexibility, rechargeability, high areal capacity, and low impedance. Using elastomeric substrate and binders, the current collectors, electrodes, and separators can be easily screen-printed layer-by-layer and vacuum-sealed in a stacked configuration. The batteries are customizable in sizes and capacities, with the highest obtained areal capacity of 54 mAh/cm 2 for primary applications. Advanced micro-CT and EIS were used to characterize the battery, whose mechanical stability was tested with repeated twisting and bending. The batteries were used to power a flexible E-ink display system that requires a high-current drain and exhibited superior performance than commercial coin-cell batteries. The developed battery presents a practical solution for powering a wide range of electronics and holds major implications for the future development of practical and high-performance flexible batteries.
Nature Communications, 2021
Confining molecules in the nanoscale environment can lead to dramatic changes of their physical a... more Confining molecules in the nanoscale environment can lead to dramatic changes of their physical and chemical properties, which opens possibilities for new applications. There is a growing interest in liquefied gas electrolytes for electrochemical devices operating at low temperatures due to their low melting point. However, their high vapor pressure still poses potential safety concerns for practical usages. Herein, we report facile capillary condensation of gas electrolyte by strong confinement in sub-nanometer pores of metal-organic framework (MOF). By designing MOF-polymer membranes (MPMs) that present dense and continuous micropore (~0.8 nm) networks, we show significant uptake of hydrofluorocarbon molecules in MOF pores at pressure lower than the bulk counterpart. This unique property enables lithium/fluorinated graphite batteries with MPM-based electrolytes to deliver a significantly higher capacity than those with commercial separator membranes (~500 mAh g−1 vs. <0.03 mAh ...
2019 IEEE 46th Photovoltaic Specialists Conference (PVSC), 2019
Sodium ion migration has been implicated in potential induced degradation of the shunting type. T... more Sodium ion migration has been implicated in potential induced degradation of the shunting type. The kinetics of sodium migration in silicon nitride can be investigated using a simple capacitance-voltage characterization technique. However, we show that the charge trapping strongly affects the measurement and must be taken into consideration in the experimental approach. We perform a systematic analysis of charge carrier trapping in silicon nitride, allowing us to correct trapping effects that otherwise prevent sodium signal detection. We extract trapping and detrapping time constants both on the order of several hours. This shows that trapping cannot be ignored as it occurs relatively quickly and is constantly evolving in time. Accurate determination of sodium behavior in dielectric layers will facilitate robust co-optimization of these layers for optical, passivation, and barrier properties.
Uploads
Papers by Jonathan Scharf