Whole-Voltage-Range Oxygen Redox in P2-Layered Cathode Materials for Sodium-Ion Batteries

Li, Xun‐Lu; Wang, Tian; Yuan, Yifei; Yue, Xin‐Yang; Wang, Qin‐Chao; Wang, Jun‐Yang; Zhong, Jun; Lin, Ruo‐Qian; Yao, Yuan; Wu, Xiao‐Jing; Yu, Xi‐Qian; Fu, Zheng‐Wen; Xia, Yong‐Yao; Yang, Xiao‐Qing; Liu, Tongchao; Amine, Khalil; Shadike, Zulipiya; Zhou, Yong‐Ning; Lu, Jun

doi:10.1002/adma.202008194

Whole-Voltage-Range Oxygen Redox in P2-Layered Cathode Materials for Sodium-Ion Batteries

Journal Article · Sun Feb 28 23:00:00 EST 2021 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202008194· OSTI ID:1771140

Li, Xun‐Lu ^[1]; Wang, Tian ^[1]; Yuan, Yifei ^[2]; Yue, Xin‐Yang ^[1]; Wang, Qin‐Chao ^[3]; Wang, Jun‐Yang ^[4]; Zhong, Jun ^[5]; Lin, Ruo‐Qian ^[6]; Yao, Yuan ^[4]; Wu, Xiao‐Jing ^[1]; Yu, Xi‐Qian ^[4]; Fu, Zheng‐Wen ^[1]; Xia, Yong‐Yao ^[1]; Yang, Xiao‐Qing ^[6]; Liu, Tongchao ^[2]; Amine, Khalil ^[2]; Shadike, Zulipiya ^[6]; Zhou, Yong‐Ning ^[1]; ^[2]

Fudan Univ., Shanghai (China)
Argonne National Lab. (ANL), Lemont, IL (United States)
Fudan Univ., Shanghai (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Laboratory for Condensed Matter
Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials
Brookhaven National Lab. (BNL), Upton, NY (United States)

Oxygen-redox of layer-structured metal-oxide cathodes has drawn great attention as an effective approach to break through the bottleneck of their capacity limit. However, reversible oxygen-redox can only be obtained in the high-voltage region (usually over 3.5 V) in current metal-oxide cathodes. Here, we realize reversible oxygen-redox in a wide voltage range of 1.5-4.5 V in a P2-layered Na_0.7Mg_0.2[Fe_0.2Mn_0.6$$\square$$0.2]O₂ cathode material, where intrinsic vacancies are located in transition-metal (TM) sites and Mg-ions are located in Na sites. Mg-ions in the Na layer serve as "pillars" to stabilize the layered structure during electrochemical cycling, especially in the high-voltage region. Intrinsic vacancies in the TM layer create the local configurations of "$$\square$$-O-$$\square$$", "Na-O-$$\square$$" and "Mg-O-$$\square$$" to trigger oxygen-redox in the whole voltage range of charge-discharge. Additionally, time-resolved techniques demonstrate that the P2 phase is well maintained in a wide potential window range of 1.5-4.5 V even at 10 C. It is revealed that charge compensation from Mn- and O-ions contributes to the whole voltage range of 1.5-4.5 V, while the redox of Fe-ions only contributes to the high-voltage region of 3.0-4.5 V. The orphaned electrons in the nonbonding 2p orbitals of O that point toward TM-vacancy sites are responsible for reversible oxygen-redox, and Mg-ions in Na sites suppress oxygen release effectively.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office; National Natural Science Foundation of China (NNSFC); Science & Technology Commission of Shanghai Municipality

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 1771140

Report Number(s):: BNL--221135-2021-JAAM

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 13 Vol. 33; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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