Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes
Abstract High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging...
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Nature Portfolio
2025-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-62518-y |
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| author | Tongtai Ji Yuxuan Zhang James Torres Aleksandar S. Mijailovic Ya Tang Xianhui Zhao Jean-Christophe Bilheux Jiwei Wang Brian W. Sheldon Oluwafemi Oyedeji Hongli Zhu |
| author_facet | Tongtai Ji Yuxuan Zhang James Torres Aleksandar S. Mijailovic Ya Tang Xianhui Zhao Jean-Christophe Bilheux Jiwei Wang Brian W. Sheldon Oluwafemi Oyedeji Hongli Zhu |
| author_sort | Tongtai Ji |
| collection | DOAJ |
| description | Abstract High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm2 (5.0 mAh/cm2) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li+ flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li+ flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO2 composite cathode with 100 mg/cm2 high-mass-loading exhibits an areal capacity of 10.4 mAh/cm2 at a current density of 2.25 mA/cm2. This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance. |
| format | Article |
| id | doaj-art-16336b2f2bc8426fa52f2ebdc14d36d0 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-16336b2f2bc8426fa52f2ebdc14d36d02025-08-24T11:38:37ZengNature PortfolioNature Communications2041-17232025-08-0116111210.1038/s41467-025-62518-yOperando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodesTongtai Ji0Yuxuan Zhang1James Torres2Aleksandar S. Mijailovic3Ya Tang4Xianhui Zhao5Jean-Christophe Bilheux6Jiwei Wang7Brian W. Sheldon8Oluwafemi Oyedeji9Hongli Zhu10Department of Mechanical and Industrial Engineering, Northeastern UniversityNeutron Scattering Division, Oak Ridge National LaboratoryNeutron Scattering Division, Oak Ridge National LaboratorySchool of Engineering, Brown UniversityOak Ridge National LaboratoryOak Ridge National LaboratoryNeutron Scattering Division, Oak Ridge National LaboratoryDepartment of Mechanical and Industrial Engineering, Northeastern UniversitySchool of Engineering, Brown UniversityOak Ridge National LaboratoryDepartment of Mechanical and Industrial Engineering, Northeastern UniversityAbstract High-mass-loading cathodes are crucial for achieving high energy density in all-solid-state batteries from the lab scale to industry. However, as mass-loading increases, electrochemical performance is significantly compromised due to sluggish kinetics. In this work, operando neutron imaging is deployed on a high-mass-loading NMC 811 cathode of 33 mg/cm2 (5.0 mAh/cm2) and directly visualizes the lithiation prioritization of the cathode active material (CAM) from the solid electrolyte membrane side to the current collector side. In addition to the tortuosity, another key limitation on ion transfer in the cathode arises from the mismatch between the uniform distribution of the solid electrolyte (catholyte) in the conventional composite cathode and the non-uniform Li+ flux generated by the faradaic reaction of CAMs. Therefore, we engineer a gradient in the catholyte concentration to match the Li+ flux distribution as a means of eliminating the ion transfer obstacle. This approach demonstrates enhanced rate performance, even with high-mass-loading cathodes. A LiCoO2 composite cathode with 100 mg/cm2 high-mass-loading exhibits an areal capacity of 10.4 mAh/cm2 at a current density of 2.25 mA/cm2. This work provides insight into the ion-transport limitation in thick cathodes and demonstrates an effective gradient design to overcome the kinetic barrier and achieve high battery performance.https://doi.org/10.1038/s41467-025-62518-y |
| spellingShingle | Tongtai Ji Yuxuan Zhang James Torres Aleksandar S. Mijailovic Ya Tang Xianhui Zhao Jean-Christophe Bilheux Jiwei Wang Brian W. Sheldon Oluwafemi Oyedeji Hongli Zhu Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes Nature Communications |
| title | Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes |
| title_full | Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes |
| title_fullStr | Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes |
| title_full_unstemmed | Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes |
| title_short | Operando neutron imaging-guided gradient design of Li-ion solid conductor for high-mass-loading cathodes |
| title_sort | operando neutron imaging guided gradient design of li ion solid conductor for high mass loading cathodes |
| url | https://doi.org/10.1038/s41467-025-62518-y |
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