Capacity Fade in Solid-State Batteries: Interphase Formation and Chemomechanical Processes in Nickel-Rich Layered Oxide Cathodes and Lithium Thiophosphate Solid Electrolytes
All-solid-state lithium ion batteries may become long-term, stable, high-performance energy storage systems for the next generation of electric vehicles and consumer electronics, depending on the compatibility of electrode materials and suitable solid electrolytes. Nickel-rich layered oxides are now...
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| Published in | Chemistry of materials Vol. 29; no. 13; pp. 5574 - 5582 |
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| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
11.07.2017
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| Online Access | Get full text |
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| Abstract | All-solid-state lithium ion batteries may become long-term, stable, high-performance energy storage systems for the next generation of electric vehicles and consumer electronics, depending on the compatibility of electrode materials and suitable solid electrolytes. Nickel-rich layered oxides are nowadays the benchmark cathode materials for conventional lithium ion batteries because of their high storage capacity and the resulting high energy density, and their use in solid-state systems is the next necessary step. In this study, we present the successful implementation of a Li[Ni,Co,Mn]O2 material with high nickel content (LiNi0.8Co0.1Mn0.1O2, NCM-811) in a bulk-type solid-state battery with β-Li3PS4 as a sulfide-based solid electrolyte. We investigate the interface behavior at the cathode and demonstrate the important role of the interface between the active materials and the solid electrolyte for the battery performance. A passivating cathode/electrolyte interphase layer forms upon charging and leads to an irreversible first cycle capacity loss, corresponding to a decomposition of the sulfide electrolyte. In situ electrochemical impedance spectroscopy and X-ray photoemission spectroscopy are used to monitor this formation. We demonstrate that most of the interphase formation takes place in the first cycle, when charging to potentials above 3.8 V vs Li+/Li. The resulting overvoltage of the passivating layer is a detrimental factor for capacity retention. In addition to the interfacial decomposition, the chemomechanical contraction of the active material upon delithiation causes contact loss between the solid electrolyte and active material particles, further increasing the interfacial resistance and capacity loss. These results highlight the critical role of (electro-)chemo-mechanical effects in solid-state batteries. |
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| AbstractList | All-solid-state lithium ion batteries may become long-term, stable, high-performance energy storage systems for the next generation of electric vehicles and consumer electronics, depending on the compatibility of electrode materials and suitable solid electrolytes. Nickel-rich layered oxides are nowadays the benchmark cathode materials for conventional lithium ion batteries because of their high storage capacity and the resulting high energy density, and their use in solid-state systems is the next necessary step. In this study, we present the successful implementation of a Li[Ni,Co,Mn]O2 material with high nickel content (LiNi0.8Co0.1Mn0.1O2, NCM-811) in a bulk-type solid-state battery with β-Li3PS4 as a sulfide-based solid electrolyte. We investigate the interface behavior at the cathode and demonstrate the important role of the interface between the active materials and the solid electrolyte for the battery performance. A passivating cathode/electrolyte interphase layer forms upon charging and leads to an irreversible first cycle capacity loss, corresponding to a decomposition of the sulfide electrolyte. In situ electrochemical impedance spectroscopy and X-ray photoemission spectroscopy are used to monitor this formation. We demonstrate that most of the interphase formation takes place in the first cycle, when charging to potentials above 3.8 V vs Li+/Li. The resulting overvoltage of the passivating layer is a detrimental factor for capacity retention. In addition to the interfacial decomposition, the chemomechanical contraction of the active material upon delithiation causes contact loss between the solid electrolyte and active material particles, further increasing the interfacial resistance and capacity loss. These results highlight the critical role of (electro-)chemo-mechanical effects in solid-state batteries. |
| Author | Koerver, Raimund Aygün, Isabel Dietrich, Christian Zhang, Wenbo Binder, Jan O Hartmann, Pascal Janek, Jürgen Leichtweiß, Thomas Zeier, Wolfgang G |
| AuthorAffiliation | BELLA − Batteries and Electrochemistry Laboratory, Institute of Nanotechnology BASF SE Karlsruhe Institute of Technology Institute of Physical Chemistry Justus-Liebig-University Giessen Center for Materials Research (LaMa) |
| AuthorAffiliation_xml | – name: Karlsruhe Institute of Technology – name: BELLA − Batteries and Electrochemistry Laboratory, Institute of Nanotechnology – name: Justus-Liebig-University Giessen – name: Center for Materials Research (LaMa) – name: Institute of Physical Chemistry – name: BASF SE |
| Author_xml | – sequence: 1 givenname: Raimund surname: Koerver fullname: Koerver, Raimund organization: Justus-Liebig-University Giessen – sequence: 2 givenname: Isabel surname: Aygün fullname: Aygün, Isabel organization: Justus-Liebig-University Giessen – sequence: 3 givenname: Thomas surname: Leichtweiß fullname: Leichtweiß, Thomas organization: Justus-Liebig-University Giessen – sequence: 4 givenname: Christian surname: Dietrich fullname: Dietrich, Christian organization: Justus-Liebig-University Giessen – sequence: 5 givenname: Wenbo surname: Zhang fullname: Zhang, Wenbo organization: Justus-Liebig-University Giessen – sequence: 6 givenname: Jan O surname: Binder fullname: Binder, Jan O organization: Justus-Liebig-University Giessen – sequence: 7 givenname: Pascal surname: Hartmann fullname: Hartmann, Pascal organization: BASF SE – sequence: 8 givenname: Wolfgang G orcidid: 0000-0001-7749-5089 surname: Zeier fullname: Zeier, Wolfgang G email: wolfgang.g.zeier@phys.chemie.uni-giessen.de organization: Justus-Liebig-University Giessen – sequence: 9 givenname: Jürgen surname: Janek fullname: Janek, Jürgen email: juergen.janek@phys.chemie.uni-giessen.de organization: Karlsruhe Institute of Technology |
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| Title | Capacity Fade in Solid-State Batteries: Interphase Formation and Chemomechanical Processes in Nickel-Rich Layered Oxide Cathodes and Lithium Thiophosphate Solid Electrolytes |
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