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Title: Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries

Abstract

Energy storage science calls for techniques to elucidate ion transport over a range of conditions and scales. We introduce a new technique, pascalammetry, in which stress is applied to a solid-state electrochemical device and induced faradaic current transients are measured and analyzed. Stress-step pascalammetry measurements are performed on operando microbattery probes (Li 2O/Li/W) and Si cathodes, revealing stress-assisted Li + diffusion. We show how non-Cottrellian lithium diffusional kinetics indicates stress, a prelude to battery degradation. An analytical solution to a diffusion/activation equation describes this stress signature, with spatiotemporal characteristics distinct from Cottrell’s classic solution for unstressed systems. These findings create an unprecedented opportunity for quantitative detection of stress in solid-state batteries through the current signature. Generally, pascalammetry offers a powerful new approach to study stress-related phenomena in any solid-state electrochemical system.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Maryland, College Park, MD (United States)
Publication Date:
Research Org.:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1499919
Grant/Contract Number:  
SC0001160
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 6; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats

Larson, Jonathan M., Gillette, Eleanor, Burson, Kristen, Wang, Yilin, Lee, Sang Bok, and Reutt-Robey, Janice E. Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries. United States: N. p., 2018. Web. doi:10.1126/sciadv.aas8927.
Larson, Jonathan M., Gillette, Eleanor, Burson, Kristen, Wang, Yilin, Lee, Sang Bok, & Reutt-Robey, Janice E. Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries. United States. doi:10.1126/sciadv.aas8927.
Larson, Jonathan M., Gillette, Eleanor, Burson, Kristen, Wang, Yilin, Lee, Sang Bok, and Reutt-Robey, Janice E. Fri . "Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries". United States. doi:10.1126/sciadv.aas8927. https://www.osti.gov/servlets/purl/1499919.
@article{osti_1499919,
title = {Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries},
author = {Larson, Jonathan M. and Gillette, Eleanor and Burson, Kristen and Wang, Yilin and Lee, Sang Bok and Reutt-Robey, Janice E.},
abstractNote = {Energy storage science calls for techniques to elucidate ion transport over a range of conditions and scales. We introduce a new technique, pascalammetry, in which stress is applied to a solid-state electrochemical device and induced faradaic current transients are measured and analyzed. Stress-step pascalammetry measurements are performed on operando microbattery probes (Li2O/Li/W) and Si cathodes, revealing stress-assisted Li+ diffusion. We show how non-Cottrellian lithium diffusional kinetics indicates stress, a prelude to battery degradation. An analytical solution to a diffusion/activation equation describes this stress signature, with spatiotemporal characteristics distinct from Cottrell’s classic solution for unstressed systems. These findings create an unprecedented opportunity for quantitative detection of stress in solid-state batteries through the current signature. Generally, pascalammetry offers a powerful new approach to study stress-related phenomena in any solid-state electrochemical system.},
doi = {10.1126/sciadv.aas8927},
journal = {Science Advances},
issn = {2375-2548},
number = 6,
volume = 4,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1. Fig. 1.: Scheme for pascalammetry with microbattery probes. (A) Cross-sectional schematic of a solid-state battery. (B) Cross-sectional schematic of the solid-state microbattery used for pascalammetry measurements. The full cell consists of a microbattery probe in contact with an oxide-free Si cathode. (C) Cross-sectional schematic of the scan-probe experimental geometry. Themore » separation distance between the Si cathode and microbattery probe is denoted as z. Negative values of z correspond to compressive forces/ stresses on the full cell. Initial approach is made with a coarse mechanical motor, while compressive forces/stresses are applied via piezo actuator. (D) Schematic of signals/ protocols used to establish a stable microbattery junction for subsequent pascalammetry measurements. The variables z, P, and I denote separation, applied pressure, and current during approach (left of vertical pink line), initial contact (vertical pink line), validation of diffusion-limited current (current decay obeys Cottrell equation to the right of vertical pink line), and establishment of a more stable junction (right of the vertical dashed gray line). (E) Schematic of the biased microbattery probe approaching and contacting the oxidefree Si counter electrode before pascalammetry measurements. Constant bias voltage (V) is applied to promote charging. Solid, dashed, and dotted outlines of the microbattery probe represent different time windows during the approach and after the initial contact with low stress. A corresponding plot of charge versus time1/2 is adjacent. The transition from a null signal (solid and dashed) to a linear signal (dotted) indicates an initial contact (pink vertical line) sufficient to establish a full-cell battery and demonstrate diffusion limited current (time right of the vertical pink line). (F) Illustration of microbattery probe/Si cathode junction and signals during two sequential stress-step pascalammetry measurements. In the junction illustration, applied compressive forces (black arrows), stress (clear to red color scale), and mechanical degradation (cracking of the electrolyte coating) are depicted. The pascalammetry signals illustration shows applied stress (pressure) in blue and induced faradaic current transients in gray. Note how this stress-step pascalammetry is analogous to potential-step voltammetry.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.