Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes
Abstract The high-voltage oxygen redox activity of Li-rich layered oxides enables additional capacity beyond conventional transition metal (TM) redox contributions and drives the development of positive electrode active materials in secondary Li-based batteries. However, Li-rich layered oxides often...
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Nature Portfolio
2024-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-54312-z |
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| author | Hao Liu Weibo Hua Sylvia Kunz Matteo Bianchini Hang Li Jiali Peng Jing Lin Oleksandr Dolotko Thomas Bergfeldt Kai Wang Christian Kübel Peter Nagel Stefan Schuppler Michael Merz Bixian Ying Karin Kleiner Stefan Mangold Deniz Wong Volodymyr Baran Michael Knapp Helmut Ehrenberg Sylvio Indris |
| author_facet | Hao Liu Weibo Hua Sylvia Kunz Matteo Bianchini Hang Li Jiali Peng Jing Lin Oleksandr Dolotko Thomas Bergfeldt Kai Wang Christian Kübel Peter Nagel Stefan Schuppler Michael Merz Bixian Ying Karin Kleiner Stefan Mangold Deniz Wong Volodymyr Baran Michael Knapp Helmut Ehrenberg Sylvio Indris |
| author_sort | Hao Liu |
| collection | DOAJ |
| description | Abstract The high-voltage oxygen redox activity of Li-rich layered oxides enables additional capacity beyond conventional transition metal (TM) redox contributions and drives the development of positive electrode active materials in secondary Li-based batteries. However, Li-rich layered oxides often face voltage decay during battery operation. In particular, although Li-rich positive electrode active materials with a high nickel content demonstrate improved voltage stability, they suffer from poor discharge capacity. Here, via physicochemical and electrochemical measurements, we investigate the correlation between oxygen redox activity and superstructure units in Li-rich layered oxides, specifically the fractions of LiMn6 and Ni4+-stabilized LiNiMn5 within the TM layer. We prove that an excess of LiNiMn5 hinders the extraction/insertion of lithium ions during Li metal coin cell charging/discharging, resulting in incomplete oxygen redox activity at a cell potential of about 3.3 V. We also demonstrate that lithium content adjustment could be a beneficial approach to tailor the superstructure units. Indeed, we report an improved oxygen redox reversibility for an optimized Li-rich layered oxide with fewer LiNiMn5 units. |
| format | Article |
| id | doaj-art-a5d51fa39c5c4b6c84662f48996f5eca |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-a5d51fa39c5c4b6c84662f48996f5eca2024-11-24T12:32:27ZengNature PortfolioNature Communications2041-17232024-11-0115111410.1038/s41467-024-54312-zTailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodesHao Liu0Weibo Hua1Sylvia Kunz2Matteo Bianchini3Hang Li4Jiali Peng5Jing Lin6Oleksandr Dolotko7Thomas Bergfeldt8Kai Wang9Christian Kübel10Peter Nagel11Stefan Schuppler12Michael Merz13Bixian Ying14Karin Kleiner15Stefan Mangold16Deniz Wong17Volodymyr Baran18Michael Knapp19Helmut Ehrenberg20Sylvio Indris21Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1University of Bayreuth, Bavarian Center for Battery Technology (BayBatt), Universitätsstraße 30University of Bayreuth, Bavarian Center for Battery Technology (BayBatt), Universitätsstraße 30Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Karlsruhe Nano Micro Facility, Karlsruhe Institute of Technology (KIT), Kaiserstraße 12Karlsruhe Nano Micro Facility, Karlsruhe Institute of Technology (KIT), Kaiserstraße 12Karlsruhe Nano Micro Facility, Karlsruhe Institute of Technology (KIT), Kaiserstraße 12Münster Electrochemical Energy Technology (MEET), University of Münster (WWU)Münster Electrochemical Energy Technology (MEET), University of Münster (WWU)Institute for Photon Science and Synchrotron Radiation (IPS), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Dynamics and Transport in Quantum Materials, Helmholtz-Zentrum Berlin für Materialen und Energie, GmbH, Albert-Einstein-Strasse 15Deutsches Elektronen-Synchrotron (DESY), Notkestrasse 85Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1Abstract The high-voltage oxygen redox activity of Li-rich layered oxides enables additional capacity beyond conventional transition metal (TM) redox contributions and drives the development of positive electrode active materials in secondary Li-based batteries. However, Li-rich layered oxides often face voltage decay during battery operation. In particular, although Li-rich positive electrode active materials with a high nickel content demonstrate improved voltage stability, they suffer from poor discharge capacity. Here, via physicochemical and electrochemical measurements, we investigate the correlation between oxygen redox activity and superstructure units in Li-rich layered oxides, specifically the fractions of LiMn6 and Ni4+-stabilized LiNiMn5 within the TM layer. We prove that an excess of LiNiMn5 hinders the extraction/insertion of lithium ions during Li metal coin cell charging/discharging, resulting in incomplete oxygen redox activity at a cell potential of about 3.3 V. We also demonstrate that lithium content adjustment could be a beneficial approach to tailor the superstructure units. Indeed, we report an improved oxygen redox reversibility for an optimized Li-rich layered oxide with fewer LiNiMn5 units.https://doi.org/10.1038/s41467-024-54312-z |
| spellingShingle | Hao Liu Weibo Hua Sylvia Kunz Matteo Bianchini Hang Li Jiali Peng Jing Lin Oleksandr Dolotko Thomas Bergfeldt Kai Wang Christian Kübel Peter Nagel Stefan Schuppler Michael Merz Bixian Ying Karin Kleiner Stefan Mangold Deniz Wong Volodymyr Baran Michael Knapp Helmut Ehrenberg Sylvio Indris Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes Nature Communications |
| title | Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes |
| title_full | Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes |
| title_fullStr | Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes |
| title_full_unstemmed | Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes |
| title_short | Tailoring superstructure units for improved oxygen redox activity in Li-rich layered oxide battery’s positive electrodes |
| title_sort | tailoring superstructure units for improved oxygen redox activity in li rich layered oxide battery s positive electrodes |
| url | https://doi.org/10.1038/s41467-024-54312-z |
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