Origin of reversible oxygen redox reactions in high energy density layered oxides
Summary: Oxygen redox reactions (ORRs) are considered a new strategy in reaching a high-energy density for rechargeable batteries. Here, we propose the concept “band coherency” for identifying the origin of reversible ORRs in alkali-excess compounds, i.e., Na2RuO3 and Li2RuO3. Band coherency redox c...
| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
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Elsevier
2021-08-01
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| Series: | Cell Reports Physical Science |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2666386421002125 |
| _version_ | 1819084860713598976 |
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| author | Gwanghyeon Choi Jaewoon Lee Sojung Koo Sangeon Park Duho Kim |
| author_facet | Gwanghyeon Choi Jaewoon Lee Sojung Koo Sangeon Park Duho Kim |
| author_sort | Gwanghyeon Choi |
| collection | DOAJ |
| description | Summary: Oxygen redox reactions (ORRs) are considered a new strategy in reaching a high-energy density for rechargeable batteries. Here, we propose the concept “band coherency” for identifying the origin of reversible ORRs in alkali-excess compounds, i.e., Na2RuO3 and Li2RuO3. Band coherency redox chemistry exhibits non-discrete transition metal (TM) nd–O 2p electron activity. This can be explained by the charge variations of O and Ru, including thermodynamic-phase stability. After the cation-based redox reaction (Ru4+/Ru5+), a dominant ORR, accompanied by the partial Ru-redox reaction, takes place in the band-coherency region. Subsequently, pure anion redox through oxygen occurs. This three-step redox mechanism is consistent with the electrochemical behavior of the oxygen-redox-tuned cathodes, until the band-coherency region shows great ORR reversibility. Triggering band coherency is a rational-design principle in using ORRs, excluding pure anionic activity and maintaining their high-energy-density properties upon cycling for the next generation of alkali-ion batteries. |
| first_indexed | 2024-12-21T20:55:11Z |
| format | Article |
| id | doaj.art-7e5f25c6e1c446618863355e89020c19 |
| institution | Directory Open Access Journal |
| issn | 2666-3864 |
| language | English |
| last_indexed | 2024-12-21T20:55:11Z |
| publishDate | 2021-08-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Cell Reports Physical Science |
| spelling | doaj.art-7e5f25c6e1c446618863355e89020c192022-12-21T18:50:37ZengElsevierCell Reports Physical Science2666-38642021-08-0128100508Origin of reversible oxygen redox reactions in high energy density layered oxidesGwanghyeon Choi0Jaewoon Lee1Sojung Koo2Sangeon Park3Duho Kim4Department of Mechanical Engineering, Kyung Hee University, 1732, Deogyeong-daero, Giheung-gu, Yongin-si, Gyeonggi-do 17104, Republic of KoreaDepartment of Mechanical Engineering, Kyung Hee University, 1732, Deogyeong-daero, Giheung-gu, Yongin-si, Gyeonggi-do 17104, Republic of KoreaDepartment of Mechanical Engineering, Kyung Hee University, 1732, Deogyeong-daero, Giheung-gu, Yongin-si, Gyeonggi-do 17104, Republic of KoreaDepartment of Mechanical Engineering, Kyung Hee University, 1732, Deogyeong-daero, Giheung-gu, Yongin-si, Gyeonggi-do 17104, Republic of KoreaDepartment of Mechanical Engineering, Kyung Hee University, 1732, Deogyeong-daero, Giheung-gu, Yongin-si, Gyeonggi-do 17104, Republic of Korea; Corresponding authorSummary: Oxygen redox reactions (ORRs) are considered a new strategy in reaching a high-energy density for rechargeable batteries. Here, we propose the concept “band coherency” for identifying the origin of reversible ORRs in alkali-excess compounds, i.e., Na2RuO3 and Li2RuO3. Band coherency redox chemistry exhibits non-discrete transition metal (TM) nd–O 2p electron activity. This can be explained by the charge variations of O and Ru, including thermodynamic-phase stability. After the cation-based redox reaction (Ru4+/Ru5+), a dominant ORR, accompanied by the partial Ru-redox reaction, takes place in the band-coherency region. Subsequently, pure anion redox through oxygen occurs. This three-step redox mechanism is consistent with the electrochemical behavior of the oxygen-redox-tuned cathodes, until the band-coherency region shows great ORR reversibility. Triggering band coherency is a rational-design principle in using ORRs, excluding pure anionic activity and maintaining their high-energy-density properties upon cycling for the next generation of alkali-ion batteries.http://www.sciencedirect.com/science/article/pii/S2666386421002125anion redoxoxygen redoxlayered oxidescathodesfirst-principle calculations |
| spellingShingle | Gwanghyeon Choi Jaewoon Lee Sojung Koo Sangeon Park Duho Kim Origin of reversible oxygen redox reactions in high energy density layered oxides Cell Reports Physical Science anion redox oxygen redox layered oxides cathodes first-principle calculations |
| title | Origin of reversible oxygen redox reactions in high energy density layered oxides |
| title_full | Origin of reversible oxygen redox reactions in high energy density layered oxides |
| title_fullStr | Origin of reversible oxygen redox reactions in high energy density layered oxides |
| title_full_unstemmed | Origin of reversible oxygen redox reactions in high energy density layered oxides |
| title_short | Origin of reversible oxygen redox reactions in high energy density layered oxides |
| title_sort | origin of reversible oxygen redox reactions in high energy density layered oxides |
| topic | anion redox oxygen redox layered oxides cathodes first-principle calculations |
| url | http://www.sciencedirect.com/science/article/pii/S2666386421002125 |
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