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 (LiO/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.
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http://dx.doi.org/10.1126/sciadv.aas8927 | DOI Listing |
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October 2024
Department of Chemistry, Humboldt-University Berlin, Brook-Taylor-Strasse 2, 12489, Berlin, Germany.
Upcoming energy-autonomous mm-scale Internet-of-things devices require high-energy and high-power microbatteries. On-chip 3D thin-film batteries (TFBs) are the most promising option but lack high-rate anode materials. Here, LiTiO thin films fabricated by atomic layer deposition (ALD) are electrochemically evaluated on 3D substrates for the first time.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2022
Catalonia Institute for Energy Research (IREC), Jardins de les Dones de Negre 1, Planta 2, Sant Adrià del Besòs, Barcelona 08930, Spain.
Extending the potential window toward the 3 V plateau below the typically used range could boost the effective capacity of LiMnO spinel cathodes. This usually leads to an "overdischarge" of the cathode, which can cause severe material damage due to manganese dissolution into the electrolyte and a critical volume expansion (induced by Jahn-Teller distortions). As those factors determine the stability and cycling lifetime for all-solid-state batteries, the operational window of LiMnO is usually limited to 3.
View Article and Find Full Text PDFSci Adv
June 2018
Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA.
Sci Rep
February 2018
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200030, P.R. China.
Rechargeable non-aqueous lithium-oxygen batteries with a large theoretical capacity are emerging as a high-energy electrochemical device for sustainable energy strategy. Despite many efforts made to understand the fundamental Li-O electrochemistry, the kinetic process of cathodic reactions, associated with the formation and decomposition of a solid LiO phase during charging and discharging, remains debate. Here we report direct visualization of the charge/discharge reactions on a gold cathode in a non-aqueous lithium-oxygen micro-battery using liquid-cell aberration-corrected scanning transmission electron microscopy (STEM) combining with synchronized electrochemical measurements.
View Article and Find Full Text PDFNano Lett
February 2018
Collège de France , 11 Place Marcelin Berthelot, 75231 Paris, France.
Although in sodium-oxygen (Na-O) batteries show promise as high-energy storage systems, this technology is still the subject of intense fundamental research, owing to the complex reaction by which it operates. To understand the formation mechanism of the discharge product, sodium superoxide (NaO), advanced experimental tools must be developed. Here we present for the first time the use of a Na-O microbattery using a liquid aprotic electrolyte coupled with fast imaging transmission electron microscopy to visualize, in real time, the mechanism of NaO nucleation/growth.
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