D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries
Abstract Charge overpotential for oxygen evolution reaction is a crucial parameter for the energy conversion efficiency of lithium-oxygen (Li-O2) batteries. So far, the realization of low charge overpotential via catalyst design is a grand challenge in this field, which usually exceeds 0.25 V. Herei...
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58640-6 |
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| author | Yin Zhou Kun Yin Yingying Huang Jiapei Li Anquan Zhu Dewu Lin Guoqiang Gan Jianfang Zhang Kai Liu Tian Zhang Kunlun Liu Chuhao Luan Huawei Yang Hou Chen Shaojun Guo Wenjun Zhang Guo Hong |
| author_facet | Yin Zhou Kun Yin Yingying Huang Jiapei Li Anquan Zhu Dewu Lin Guoqiang Gan Jianfang Zhang Kai Liu Tian Zhang Kunlun Liu Chuhao Luan Huawei Yang Hou Chen Shaojun Guo Wenjun Zhang Guo Hong |
| author_sort | Yin Zhou |
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| description | Abstract Charge overpotential for oxygen evolution reaction is a crucial parameter for the energy conversion efficiency of lithium-oxygen (Li-O2) batteries. So far, the realization of low charge overpotential via catalyst design is a grand challenge in this field, which usually exceeds 0.25 V. Herein, we report an orbital reconstruction strategy to significantly decrease the charge overpotential to the low 0.11 V by employing PdCo nanosheet catalyst under a low-loading mass (0.3 mg/cm2) and capacity (0.3 mAh/cm2). Experimental and theoretical calculations demonstrate that the precise d-d orbital coupling (d xz-d xz, d yz-d yz and d z 2-d z 2) between the low-electronegativity Co and Pd leads to the reconstruction of Pd 4 d orbitals in PdCo nanosheets, thereby resulting in a downward shift of all the three active Pd 4 d orbitals (d z 2, d xz and d yz) relative to that of Pd nanosheets. Furthermore, the highest energy level of the Pd 4d z 2 orbital in PdCo is lower than the lowest energy levels of the Pd 4d xz and 4d yz orbitals in pure Pd, significantly decreasing the charge activation energy and achieving a highest energy conversion efficiency of 91%. This finding provides the orbital-level tuning into rational design of highly efficient electrocatalysts for Li-O2 batteries. |
| format | Article |
| id | doaj-art-14b65a0834cc42bf9e1d4d4b1318ae22 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-14b65a0834cc42bf9e1d4d4b1318ae222025-08-20T02:17:01ZengNature PortfolioNature Communications2041-17232025-04-011611910.1038/s41467-025-58640-6D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen BatteriesYin Zhou0Kun Yin1Yingying Huang2Jiapei Li3Anquan Zhu4Dewu Lin5Guoqiang Gan6Jianfang Zhang7Kai Liu8Tian Zhang9Kunlun Liu10Chuhao Luan11Huawei Yang12Hou Chen13Shaojun Guo14Wenjun Zhang15Guo Hong16Department of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueSchool of Chemistry and Materials Science, Shandong Key University Laboratory of High Performance and Functional Polymer, Ludong UniversityDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueSchool of Chemistry and Materials Science, Shandong Key University Laboratory of High Performance and Functional Polymer, Ludong UniversitySchool of Chemistry and Materials Science, Shandong Key University Laboratory of High Performance and Functional Polymer, Ludong UniversitySchool of Materials Science and Engineering, Peking UniversityDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueDepartment of Materials Science and Engineering & Center of Super-Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee AvenueAbstract Charge overpotential for oxygen evolution reaction is a crucial parameter for the energy conversion efficiency of lithium-oxygen (Li-O2) batteries. So far, the realization of low charge overpotential via catalyst design is a grand challenge in this field, which usually exceeds 0.25 V. Herein, we report an orbital reconstruction strategy to significantly decrease the charge overpotential to the low 0.11 V by employing PdCo nanosheet catalyst under a low-loading mass (0.3 mg/cm2) and capacity (0.3 mAh/cm2). Experimental and theoretical calculations demonstrate that the precise d-d orbital coupling (d xz-d xz, d yz-d yz and d z 2-d z 2) between the low-electronegativity Co and Pd leads to the reconstruction of Pd 4 d orbitals in PdCo nanosheets, thereby resulting in a downward shift of all the three active Pd 4 d orbitals (d z 2, d xz and d yz) relative to that of Pd nanosheets. Furthermore, the highest energy level of the Pd 4d z 2 orbital in PdCo is lower than the lowest energy levels of the Pd 4d xz and 4d yz orbitals in pure Pd, significantly decreasing the charge activation energy and achieving a highest energy conversion efficiency of 91%. This finding provides the orbital-level tuning into rational design of highly efficient electrocatalysts for Li-O2 batteries.https://doi.org/10.1038/s41467-025-58640-6 |
| spellingShingle | Yin Zhou Kun Yin Yingying Huang Jiapei Li Anquan Zhu Dewu Lin Guoqiang Gan Jianfang Zhang Kai Liu Tian Zhang Kunlun Liu Chuhao Luan Huawei Yang Hou Chen Shaojun Guo Wenjun Zhang Guo Hong D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries Nature Communications |
| title | D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries |
| title_full | D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries |
| title_fullStr | D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries |
| title_full_unstemmed | D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries |
| title_short | D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries |
| title_sort | d orbital reconstruction achieves low charge overpotential in li oxygen batteries |
| url | https://doi.org/10.1038/s41467-025-58640-6 |
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