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Synergistic halide-sulfide hybrid solid electrolytes for Ni-rich cathodes design guided by digital twin for all-solid-State Li batteries

Title
Synergistic halide-sulfide hybrid solid electrolytes for Ni-rich cathodes design guided by digital twin for all-solid-State Li batteries
Author(s)
Kim, Jong SeokJung, SeungwonKwak, HiramHan, YoonjaeKim, SuhwanLim, JongwooLee, Yong MinJung, Yoon Seok
Issued Date
2023-01
Citation
Energy Storage Materials, v.55, pp.193 - 204
Type
Article
Author Keywords
All-solid-state lithium batteriesHalide solid electrolytesSulfide solid electrolytesDigital twinsElectrochemical stabilities
Keywords
LITHIUM-IONCOMPOSITE CATHODESSTABILITYINTERFACELICOO2LINI0.5MN1.5O4
ISSN
2405-8297
Abstract
Halide solid electrolytes are a promising candidate for all-solid-state Li batteries (ASLBs) owing to their mechanical sintering ability and excellent (electro)chemical oxidation stability. However, these advantages are counteracted by the lower Li+ conductivities and higher specific densities compared with those of sulfides. Herein, a novel halide-sulfide hybrid catholyte design for Ni-rich layered oxide cathodes for ASLBs is reported. In a hybrid catholyte, Li3YCl6 (0.40 mS cm−1) coatings protect the surface of Li[Ni0.88Co0.11Al0.01]O2 while Li6PS5Cl (1.80 mS cm−1) serves as a Li+ highway. Li[Ni0.88Co0.11Al0.01]O2 cathodes with an optimal fraction of Li3YCl6, 10 wt% with respect to Li [Ni0.88Co0.11Al0.01]O2, substantially outperform electrodes using either Li6PS5Cl or Li3YCl6 in terms of capacity (202 vs. 171 or 191 mA h g−1 at 0.1C, respectively), initial Coulombic efficiency, rate capability, and cycling performance. The superiority of Li3YCl6 for interfacial stability in the Li3YCl6-coated electrode to the electrode without Li3YCl6 is confirmed by complementary analysis. Moreover, the digital twin model is successfully established and reveals electrically isolated Li[Ni0.88Co0.11Al0.01]O2 particles when 14 wt% Li3YCl6 is used. This insight leads to the development of a mixed conductor coating consisting of Li3YCl6 and carbon, further enhancing the performance: e.g., 134 vs. 53 mA h g−1 at 2C. © 2022 Elsevier B.V.
URI
http://hdl.handle.net/20.500.11750/17371
DOI
10.1016/j.ensm.2022.11.038
Publisher
Elsevier BV
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Department of Energy Science and Engineering Battery Materials & Systems LAB 1. Journal Articles

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