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Crystallographic-Site-Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathodes for Lithium-Ion Batteries

Journal Article


Abstract


  • The development of reliable and safe high-energy-density lithium-ion batteries is hindered by the structural instability of cathode materials during cycling, arising as a result of detrimental phase transformations occurring at high operating voltages alongside the loss of active materials induced by transition metal dissolution. Originating from the fundamental structure/function relation of battery materials, the authors purposefully perform crystallographic-site-specific structural engineering on electrode material structure, using the high-voltage LiNi0.5Mn1.5O4 (LNMO) cathode as a representative, which directly addresses the root source of structural instability of the Fd (Formula presented.) m structure. By employing Sb as a dopant to modify the specific issue-involved 16c and 16d sites simultaneously, the authors successfully transform the detrimental two-phase reaction occurring at high-voltage into a preferential solid-solution reaction and significantly suppress the loss of Mn from the LNMO structure. The modified LNMO material delivers an impressive 99% of its theoretical specific capacity at 1 C, and maintains 87.6% and 72.4% of initial capacity after 1500 and 3000 cycles, respectively. The issue-tracing site-specific structural tailoring demonstrated for this material will facilitate the rapid development of high-energy-density materials for lithium-ion batteries.

Publication Date


  • 2021

Citation


  • Liang, G., Peterson, V. K., Wu, Z., Zhang, S., Hao, J., Lu, C. Z., . . . Guo, Z. (2021). Crystallographic-Site-Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathodes for Lithium-Ion Batteries. Advanced Materials, 33(44). doi:10.1002/adma.202101413

Scopus Eid


  • 2-s2.0-85114169691

Volume


  • 33

Issue


  • 44

Abstract


  • The development of reliable and safe high-energy-density lithium-ion batteries is hindered by the structural instability of cathode materials during cycling, arising as a result of detrimental phase transformations occurring at high operating voltages alongside the loss of active materials induced by transition metal dissolution. Originating from the fundamental structure/function relation of battery materials, the authors purposefully perform crystallographic-site-specific structural engineering on electrode material structure, using the high-voltage LiNi0.5Mn1.5O4 (LNMO) cathode as a representative, which directly addresses the root source of structural instability of the Fd (Formula presented.) m structure. By employing Sb as a dopant to modify the specific issue-involved 16c and 16d sites simultaneously, the authors successfully transform the detrimental two-phase reaction occurring at high-voltage into a preferential solid-solution reaction and significantly suppress the loss of Mn from the LNMO structure. The modified LNMO material delivers an impressive 99% of its theoretical specific capacity at 1 C, and maintains 87.6% and 72.4% of initial capacity after 1500 and 3000 cycles, respectively. The issue-tracing site-specific structural tailoring demonstrated for this material will facilitate the rapid development of high-energy-density materials for lithium-ion batteries.

Publication Date


  • 2021

Citation


  • Liang, G., Peterson, V. K., Wu, Z., Zhang, S., Hao, J., Lu, C. Z., . . . Guo, Z. (2021). Crystallographic-Site-Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathodes for Lithium-Ion Batteries. Advanced Materials, 33(44). doi:10.1002/adma.202101413

Scopus Eid


  • 2-s2.0-85114169691

Volume


  • 33

Issue


  • 44