The interplay between (electro)chemical and (chemo)mechanical effects in the cycling performance of thiophosphate-based solid-state batteries
doi: 10.1088/2752-5724/ac3897
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Abstract: Solid-state batteries (SSBs) are a promising next step in electrochemical energy storage but are plagued by a number of problems. In this study, we demonstrate the recurring issue of mechanical degradation because of volume changes in layered Ni-rich oxide cathode materials in thiophosphate-based SSBs. Specifically, we explore superionic solid electrolytes (SEs) of different crystallinity, namely glassy 1.5Li2S-0.5P2S5-LiI and argyrodite Li6PS5Cl, with emphasis on how they affect the cyclability of slurry-cast cathodes with NCM622 (60% Ni) or NCM851005 (85% Ni). The application of a combination of ex situ and in situ analytical techniques helped to reveal the benefits of using a SE with a low Young’s modulus. Through a synergistic interplay of (electro)chemical and (chemo)mechanical effects, the glassy SE employed in this work was able to achieve robust and stable interfaces, enabling intimate contact with the cathode material while at the same time mitigating volume changes. Our results emphasize the importance of considering chemical, electrochemical, and mechanical properties to realize long-term cycling performance in high-loading SSBs.
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Figure 1. Cycling performance of SSB cells with (a) glassy SE (1.5Li2S-0.5P2S5-LiI) and (b) crystalline SE (Li6PS5Cl) in both pelletized and slurry-cast cathodes and corresponding Coulombic efficiencies. Cells tested at 45 C, C/5, 2.9-4.4 V vs Li+/Li.
Figure 2. Cross-sectional SEM images of the slurry-cast cathode of SSB cells using (a), (b) glassy SE (1.5Li2S-0.5P2S5-LiI) and (c), (d) crystalline SE (Li6PS5Cl) after 200 cycles at a rate of C/5 and 45 C. The arrows denote void formation and cracking.
Figure 3. Nyquist plots of the electrochemical impedance of SSB cells (black lines: measured data; solid symbols: fitted data) using a slurry-cast cathode with (a) glassy SE (1.5Li2S-0.5P2S5-LiI) and (b) crystalline SE (Li6PS5Cl) after 200 cycles at a rate of C/5 and 45 C. Semicircles provide eye guidance for the individual resistance contributions.
Figure 4. In situ pressure monitoring of Super C65 electrodes with (a)-(c) glassy SE (1.5Li2S-0.5P2S5-LiI) and (e)-(g) crystalline SE (Li6PS5Cl). (a), (e) CV profiles, (b), (f) current response, and (c), (g) pressure response. Cells tested at 45 C, 0.05 mV s-1, OCV-4.4 V vs Li+/Li in the first cycle and 1.55-4.4 V vs Li+/Li in the following cycles. Top-view SEM images of the (d) glassy SE/Super C65 and (h) crystalline SE/Super C65 electrodes after cycling.
Figure 5. Electrochemical profile of SSB cells using a slurry-cast cathode with (a) glassy SE (1.5Li2S-0.5P2S5-LiI) and (b) crystalline SE (Li6PS5Cl) and corresponding time-resolved evolution rates (left y-axis) and cumulative amounts (right y-axis) for H2, O2, and CO2, as well as normalized ion currents for SO2. Cells tested at 45 C, C/20, 2.9-5.0 V vs Li+/Li.
Figure 6. X-ray photoelectron spectra of the (a) S 2p and (b) P 2p core levels of slurry-cast cathodes with glassy SE (1.5Li2S-0.5P2S5-LiI) and crystalline SE (Li6PS5Cl) collected before and after 200 cycles at a rate of C/5 and 45 C. Box plots of the normalized intensity of (c) PO2-, (d) PO3-, (e) SO2-, and (f) SO3- fragments for the uncycled and cycled g-SE and c-SE cells from ToF-SIMS depth-profiling analysis.
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