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Structural and electrochemical stabilization enabling high-energy P3-type Cr-based layered oxide cathode for K-ion batteries

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Carbon Energy 2024年第5期6卷 81-93页

作者： Wonseok Ko seokjin lee Hyunyoung Park Jungmin Kang Jinho Ahn Yongseok lee Gwangeon Oh Jung-Keun Yoo Jang-Yeon Hwang Jongsoon Kim Department of Energy Science Sungkyunkwan UniversitySuwonRepublic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwonRepublic of Korea Department of Energy Engineering Hanyang UniversitySeoulRepublic of Korea Carbon Composites Department Korea Institute of Materials Science(KIMS)ChangwonRepublic of Korea Department of Battery Engineering Hanyang UniversitySeoulRepublic of Korea

Layered-type transition metal(TM)oxides are considered as one of the most promising cathodes for K-ion batteries because of the large theoretical gravimetric capacity by low molar ***,they suffer from severe structural change by de/intercalation and diffusion of K^(+)ions with large ionic size,which results in not only much lower reversible capacity than the theoretical capacity but also poor power ***,it is important to enhance the structural stability of the layered-type TM oxides for outstanding electrochemical behaviors under the K-ion battery ***,it is investigated that the substitution of the appropriate Ti^(4+)contents enables a highly enlarged reversible capacity of P3-type KxCrO_(2) using combined studies of first-principles calculation and various *** the pristine P3-type KxCrO_(2) just exhibits the reversible capacity of∼120 mAh g^(−1) in the voltage range of 1.5-4.0 V(vs.K^(+)/K),the∼0.61 mol K^(+)corresponding to∼150 mAh g^(−1) can be reversible de/intercalated at the structure of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) under the same ***,even at the high current density of 788 mA g^(−1),the specific capacity of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) is∼120 mAh g^(−1),which is∼81 times larger than that of the pristine P3-type KxCrO_(2).It is believed that this research can provide an effective strategy to improve the electrochemical performances of the cathode materials suffered by severe structural change that occurred during charge/discharge under not only K-ion battery system but also other rechargeable battery systems.

关键词： cathodes first-principles calculations layered-type oxide materials potassium-ion batteries structural stabilization

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Occurrence of anionic redox with absence of full oxidation to Ru^(5+) in high-energy P2-type layered oxide cathode

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Journal of Energy Chemistry 2023年第9期84卷 153-161页

作者： Jinho Ahn Hyunyoung Park Wonseok Ko Yongseok lee Jungmin Kang seokjin lee Sangyeop lee Eunji Sim Kyuwook Ihm Jihyun Hong Jung-Keun Yoo Kyojin Ku Jongsoon Kim Department of Energy Science Sungkyunkwan UniversitySuwon 16419Republic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwon 16419Republic of Korea Nano&Interface Research Team Pohang Accelerator LaboratoryPohang 37673Republic of Korea Department of Smart Fabrication Technology Sungkyunkwan UniversitySuwon 16419Republic of Korea Energy Materials Research Center Korea Institute of Science and Technology(KIST)14 Gil 5 Hwarang-roSeongbuk-guSeoul 02792Republic of Korea Carbon Composites Department Composites Research DivisionKorea Institute of Materials Science(KIMS)797 ChangwondaeroChangwon 51508Republic of Korea Department of Materials Science and Engineering Hanbat National UniversityDaejeon 34158Republic of Korea

The anionic redox has been widely studied in layered-oxide-cathodes in attempts to achieve highenergy-density for Na-ion batteries(NIBs).It is known that an oxidation state of Mn^(4+) or Ru^(5+) is essential for the anionic reaction of O^(2-)/O~-to occur during Na^(+) de/***,here,we report that the anionic redox can occur in Ru-based layered-oxide-cathodes before full oxidation of Ru^(4+)/Ru^(5+).Combining studies using first-principles calculation and experimental techniques reveals that further Na^(+) deintercalation from P2-Na_(0.33)[Mg_(0.33)Ru_(0.67)]O_(2) is based on anionic oxidation after 0.33 mol Na^(+) deintercalation from P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) with cationic oxidation of Ru^(4+)/Ru^(4.5+).Especially,it is revealed that the only oxygen neighboring 2Mg/1 Ru can participate in the anionic redox during Na^(+) de/intercalation,which implies that the Na-O-Mg arrangement in the P2-Na_(0.33)[M9_(0.33)Ru_(0.67)]O_(2) structure can dramatically lower the thermodynamic stability of the anionic redox than that of cationic *** the O anionic and Ru cationic reaction,P2-Na_(0.67)[Mg_(0.33)Ru_(0.67)]O_(2) exhibits not only a large specific capacity of~172 mA h g^(-1) but also excellent power-capability via facile Na^(+) diffusion and reversible structural change during charge/*** findings suggest a novel strategy that can increase the activity of anionic redox by modulating the local environment around oxygen to develop high-energy-density cathode materials for NIBs.

关键词： Na-ion batteries P2-type cathode Anionic redox Local environment First-principles calculation

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