TY - JOUR
T1 - Utilizing Oxygen Redox in Layered Cathode Materials from Multiscale Perspective
AU - Lee, Gi Hyeok
AU - Lau, Vincent Wing hei
AU - Yang, Wanli
AU - Kang, Yong Mook
N1 - Funding Information:
G.‐H.L. and V.W.L. contributed equally to this work. Y.‐M.K. acknowledges the financial support from National Research Foundation of Korea (NRF) grants funded by the Korean government (MSIP; NRF‐2017R1A2B3004383) and Future Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF‐2017M3D1A1039553 and NRF‐2020M3D1A1068764). G.‐H.L. acknowledges the financial support of the ALS fellowship program. V.W.L. is funded by the “First Research in Lifetime” grant from the National Research Foundation of Korea (NRF) under grant number NRF‐2018R1C1B5047313. Soft X‐ray analysis used resources of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE‐AC02‐05CH11231.
Publisher Copyright:
© 2021 Wiley-VCH GmbH
PY - 2021/7/22
Y1 - 2021/7/22
N2 - In high-capacity layered oxide cathode materials, utilization of lattice oxygen as a redox center is considered to be one of the most promising approaches to overcome the capacity limitation set by conventional transition metal redox centers. However, rapid material degradation is often associated with oxygen oxidation, leading to formidable challenges in utilizing oxygen redox. Further mechanistic understanding of the oxygen activities thus becomes critical to better control oxygen redox reactions. This review summarizes recent advances for investigating oxygen redox reactions in cathode materials from a multiscale perspective, i.e., from the atomistic level to the microstructure regime. First the mechanistic aspects of oxygen redox and the consequences of this reaction on various electrode degradation pathways during battery operation (e.g., oxygen loss, transition metal migration, irreversible phase transition), relating structural changes at the crystallographic scale to those at the macro scale, are discussed. Then recent developments based on atomic and microstructure modifications that are promising for improving the reversibility of oxygen redox reaction or mitigating the harmful processes arising from oxidation of the oxygen centers under high operating voltage are recounted. The analysis is concluded with a commentary on further research directions toward optimizing the oxygen activity for high-capacity charge storage.
AB - In high-capacity layered oxide cathode materials, utilization of lattice oxygen as a redox center is considered to be one of the most promising approaches to overcome the capacity limitation set by conventional transition metal redox centers. However, rapid material degradation is often associated with oxygen oxidation, leading to formidable challenges in utilizing oxygen redox. Further mechanistic understanding of the oxygen activities thus becomes critical to better control oxygen redox reactions. This review summarizes recent advances for investigating oxygen redox reactions in cathode materials from a multiscale perspective, i.e., from the atomistic level to the microstructure regime. First the mechanistic aspects of oxygen redox and the consequences of this reaction on various electrode degradation pathways during battery operation (e.g., oxygen loss, transition metal migration, irreversible phase transition), relating structural changes at the crystallographic scale to those at the macro scale, are discussed. Then recent developments based on atomic and microstructure modifications that are promising for improving the reversibility of oxygen redox reaction or mitigating the harmful processes arising from oxidation of the oxygen centers under high operating voltage are recounted. The analysis is concluded with a commentary on further research directions toward optimizing the oxygen activity for high-capacity charge storage.
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U2 - 10.1002/aenm.202003227
DO - 10.1002/aenm.202003227
M3 - Review article
AN - SCOPUS:85102268436
SN - 1614-6832
VL - 11
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 27
M1 - 2003227
ER -