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Title: Insights into the structural effects of layered cathode materials for high voltage sodium-ion batteries

Cathode materials are critical to the energy density, power density and safety of sodium-ion batteries (SIBs). Herein, we performed a comprehensive study to elucidate and exemplify the interplay mechanism between phase structures, interfacial microstrain and electrochemical properties of layered-structured Na xNi 1/3Co 1/3Mn 1/3O 2 cathode materials for high voltage SIBs. The electrochemical test results showed that Na xNi 1/3Co 1/3Mn 1/3O 2 with an intergrowth P2/O3/O1 structure demonstrates better electrochemical performance and better thermal stability than Na xNi 1/3Co 1/3Mn 1/3O 2 with P2/O3 binary-phase integration and Na xNi 1/3Co 1/3Mn 1/3O 2 where only the P phase is dominant. This result is caused by the distinct interfacial microstrain development during the synthesis and cycling of the P2/O3/O1 phase. In operando high energy X-ray diffraction further revealed that the intergrowth P2/O1/O3 cathode can inhibit the irreversible P2–O2 phase transformation and simultaneously improve the structure stability of the O3 and O1 phases during cycling. Here, we believe that interfacial microstrain can serve as an indispensable bridge to guide future design and synthesis of high performance SIB cathode materials and other high energy battery materials.
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [1] ;  [5] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [6] ; ORCiD logo [6] ;  [7] ;  [3] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Univ. of Illinois at Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Xiamen Univ., Xiamen (China)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Rochester, Rochester, NY (United States)
  6. Mohammed VI Polytechnic Univ.; Ben Guerir (Morocco)
  7. Microvast Inc., Stafford, TX (United States)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1754-5692
Royal Society of Chemistry
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NNSFC)
Country of Publication:
United States
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; layered-structured cathode; high voltage; in operando synchrotron HEXRD; interfacial microstrain; intergrowth; sodium-ion batteries; thermal stability
OSTI Identifier: