Engineering topics

Browning, Katie L.

Publications and source records attributed to Browning, Katie L..

8 records

DOE OSTI2024

Percolating Interfacial Layers Enhance Conductivity in Polymer–Composite Electrolytes

Here, this study investigates the impact of the ceramic particle size on the bulk and interfacial ion transport properties of composite polymer electrolytes. The ceramic particles used for this study are micrometer-sized commercial lithium lanthanum titanate (LLTO) powders and LLTO nanorods (NR) prepared in the laboratory. The polymer matrices are vinylene carbonate (VEC) based single-ion-conducting (SIC) and dual-ion-conducting (DIC) polymer electrolytes. Our results reveal that the addition of LLTO NR results in improved ion transport, while the addition of commercial LLTO is ineffective or even detrimental. We ascribe these results to the formation of an interfacial polymer layer around the LLTO particles with enhanced Li + mobility and estimate the thickness of the interfacial layer to be ∼5 nm. The high surface-to-volume ratio of the LLTO NR leads to the percolation of the interfacial region at a relatively low ceramic loading of 30 wt %. This study highlights the importance of achieving percolation of the interface region (as opposed to the particles themselves) within the composite electrolyte when the interfacial layer is the enhancement mechanism.

Ock, Ji-young↗

DOE OSTI2023

Battery with shear thickening, impact resistant electrolytes

A battery includes an anode, a cathode, and a porous separator having a surface and percolating pores providing a porosity of from 20% to 80%. A passively impact resistant composite electrolyte includes an electrolyte and electrically non-conducting particles that enable shear thickening. The particles can have a polydispersity index of no greater than 0.1, an average particle size in a range of from 50 nm to 1 um, and an absolute zeta potential of greater than ±40 mV. The shear thickening enabling particles can be from 10 wt. % to 40 wt. % of the total weight of the separator and shear thickening particles. Between 20-40 wt. % of the shear thickening enabling particles are located in the pores of the separator.

Armstrong, Beth L.↗

DOE OSTI2023

Method of making a passively impact resistant battery

A method of making a passively impact resistant battery includes the steps of providing a porous separator material having pores and a surface, and providing a suspension composition including shear thickening enabling particles and a particle suspension solvent for suspending the shear thickening enabling particles. The shear thickening particles have a polydispersity index of no greater than 0.1, an average particle size of in a range of 50 nm to 1 um, and an absolute zeta potential of greater than ±40 mV. The suspension composition is applied to the separator material, wherein a portion of the particles and suspension solvent penetrate the pores. The suspension solvent is evaporated from the separator material. An anode layer and a cathode layer are applied. An electrolyte composition is applied between the anode layer and the cathode layer. The electrolyte composition includes an electrolyte solvent and an electrolyte salt.

Armstrong, Beth L.↗

DOE OSTI2023

Deposition and characterization of α-Fe 2 O 3 /Pd thin films for neutron reflectometry studies

Here, we report deposition of hematite/Pd thin films on silicon wafers via radio frequency (RF) magnetron sputtering and subsequent characterization for future in situ neutron reflectometry studies. Following deposition, the hematite/Pd thin films were characterized as prepared and after annealing in air for 2h at 400, 500, and 600 °C, respectively. Raman spectroscopy, grazing incidence x-ray diffraction, and neutron reflectometry (NR) were used to characterize the structure and chemical compositions of the thin films. The results indicate that pure α-Fe 2 O 3 (hematite) films were produced, free from other iron oxide phases and impurities. NR data reveal that one intermediate layer between the Pd layer and the hematite layer was formed during sputtering deposition processes. The fitted scattering length density (SLD) of the as-deposited hematite layer is 70% of the theoretical SLD value, indicating that the grains are loosely packed in the RF-deposited hematite films. After annealing at elevated temperatures, the hematite films show increased SLD values but remain comparable to that of preannealed.

36 MATERIALS SCIENCE↗

DOE OSTI2023

In Situ Measurement of Buried Electrolyte–Electrode Interfaces for Solid State Batteries with Nanometer Level Precision

Many technologies including high-energy solid-state batteries rely on high quality solid–solid interfaces. Solid–solid interfaces are particularly difficult to study as their nature requires the interface to be buried. Here, in this work, we demonstrate the use of a combination of neutron reflectometry and in situ electrochemistry to measure the interface between Li metal and the solid electrolyte LiPON across an 8 cm 2 area. Neutron reflectometry measurements confirm the interphase to be less than 7 nm thick. The neutron reflectometry data further emphasize that the interphase that forms is a chemical gradient consisting of a Li-rich layer that gradually decreases in Li content until it blends into pure LiPON. Experimental confirmation that we can make ideal solid–solid interphases less than 10 nm thick will help facilitate the adoption of high efficiency next generation solid state batteries. Further this combination of complementary techniques provides a more general methodology for studying buried solid–solid interfaces across applications.

25 ENERGY STORAGE↗

DOE OSTI2023

Functionalized Silicon Particles for Enhanced Half- and Full-Cell Cycling of Si-Based Li-Ion Batteries

Vinylene carbonate (VC) and polyethylene oxide (PEO) have been investigated as functional agents that mimic the solid electrolyte interphase (SEI) chemistry of silicon (Si). VC and PEO are known to contribute to the stability of Si-based lithium-ion batteries as an electrolyte additive and as a SEI component, respectively. In this work, covalent surface functionalization was achieved via a facile route, which involves ball-milling the Si particles with sacrificial VC and PEO. Thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS), and magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy indicate that the additives are strongly bound to Si. In particular, MAS NMR shows Si–R or Si–O–R groups, which confirm functionalization of the Si after milling in VC or PEO. Particle size analysis by dynamic light scattering reveals that the additives facilitate particle size reduction and that the functionalized particles result in more stable dispersions based on zeta potential measurements. Raman mapping of the electrodes fabricated from the VC and PEO-coated active material with a polyacrylic acid (PAA) binder reveals a more homogenous distribution of Si and the carbon conductive additive compared to the electrodes prepared from the neat Si. Furthermore, the VC-milled Si strikingly exhibited the highest capacity in both half- and full-cell configurations, with more than 200 mAh g –1 measured capacity compared to the neat Si in the half-cell format. This is linked to an improved electrode processing based on the Raman and zeta potential measurements as well as a thinner SEI (with more organic components for the functionalized Si relative to the neat Si) based on XPS analysis of the cycled electrodes. In conclusion, the effect of binder was also investigated by comparing PAA with P84 (polyimide type), where an increased capacity is observed in the latter case.

25 ENERGY STORAGE↗

DOE OSTI2022

Thin-Film Paradigm to Probe Interfacial Diffusion during Solid-State Metathesis Reactions

We highlight a paradigm for studying complex reaction mechanisms that guide the synthesis of materials. Thin films of FeCl 2 and Na 2 S 2 were deposited to study the metathesis reaction to form FeS 2 and NaCl. In situ X-ray reflectivity was used to monitor the interface between materials, which revealed a slow, impeded reaction at high temperatures as compared to previous studies using powder samples. AC impedance and X-ray photoelectron spectroscopy provided insight into distribution of elements and conductivity of the phases present during the reaction, and phase-field modeling was used to elucidate the diffusion of ions throughout the thin-film bilayers. Here, the use of thin-film bilayers provides a simplified system to study solid-state metathesis reactions and highlights the complexity of diffusion at solid-state interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Fabrication of films and coatings used to activate shear thickening, impact resistant electrolytes

A method of making a passively impact resistant composite electrolyte and separator layer includes providing a suspension composition including electrically non-conducting particles that enable shear thickening. The particles can have a polydispersity index of no greater than 0.1, an average particle size in a range of from 50 nm to 1 um, and an absolute zeta potential of greater than ±40 mV. A particle suspension solvent is provided for suspending the particles. The suspension composition is applied to a porous separator material. A portion of the particles and suspension solvent penetrate the pores and the remainder of the particles in the suspension composition are distributed across the surface of the separator material. The suspension solvent is evaporated from the separator material to provide a shear thickening particle loaded separator. A separator assembly and a passivated battery are also disclosed.

Armstrong, Beth L.↗