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Uncommon Behavior of Li Doping Suppresses Oxygen Redox in P2-Type Manganese-Rich Sodium Cathodes.
Xiao, Biwei; Liu, Xiang; Chen, Xi; Lee, Gi-Hyeok; Song, Miao; Yang, Xin; Omenya, Fred; Reed, David M; Sprenkle, Vincent; Ren, Yang; Sun, Cheng-Jun; Yang, Wanli; Amine, Khalil; Li, Xin; Xu, Guiliang; Li, Xiaolin.
Affiliation
  • Xiao B; Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Liu X; Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA.
  • Chen X; John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, 02138, USA.
  • Lee GH; Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
  • Song M; Department of Materials Science and Engineering, Dongguk University, Seoul, 04620, Republic of Korea.
  • Yang X; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Omenya F; Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Reed DM; Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Sprenkle V; Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Ren Y; Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
  • Sun CJ; X-ray science division, Argonne National Laboratory, Lemont, IL, 60439, USA.
  • Yang W; X-ray science division, Argonne National Laboratory, Lemont, IL, 60439, USA.
  • Amine K; Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
  • Li X; Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL, 60439, USA.
  • Xu G; Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Li X; John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, 02138, USA.
Adv Mater ; 33(52): e2107141, 2021 Dec.
Article in En | MEDLINE | ID: mdl-34632654
ABSTRACT
Utilizing both cationic and anionic oxygen redox reactions is regarded as an important approach to exploit high-capacity layered cathode materials with earth abundant elements. It has been popular strategies to effectively elevate the oxygen redox activities by Li-doping to introduce unhybridized O 2p orbitals in Nax MnO2 -based chemistries or enabling high covalency transition metals in P2-Na0.66 Mnx TM1- x O2 (TM = Fe, Cu, Ni) materials. Here, the effect of Li doping on regulating the oxygen redox activities P2-structured Na0.66 Ni0.25 Mn0.75 O2 materials is investigated. Systematic X-ray characterizations and ab initio simulations have shown that the doped Li has uncommon behavior in modulating the density of states of the neighboring Ni, Mn, and O, leading to the suppression of the existing oxygen and Mn redox reactivities and the promotion of the Ni redox. The findings provide a complementary scenario to current oxygen redox mechanisms and shed lights on developing new routes for high-performance cathodes.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Adv Mater Journal subject: BIOFISICA / QUIMICA Year: 2021 Document type: Article Affiliation country:
Fulltext
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Adv Mater Journal subject: BIOFISICA / QUIMICA Year: 2021 Document type: Article Affiliation country: