TY - JOUR
T1 - Crystallographic-Site-Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High-Voltage LiNi0.5Mn1.5O4 Spinel Cathodes for Lithium-Ion Batteries
AU - Liang, Gemeng
AU - Peterson, Vanessa K.
AU - Wu, Zhibin
AU - Zhang, Shilin
AU - Hao, Junnan
AU - Lu, Cheng-Zhang
AU - Chuang, Cheng-Hao
AU - Lee, Jyh-Fu
AU - Liu, Jue
AU - Leniec, Grzegorz
AU - Kaczmarek, Sławomir Maksymilian
AU - D'Angelo, Anita M.
AU - Johannessen, Bernt
AU - Thomsen, Lars
AU - Pang, Wei Kong
AU - Guo, Zaiping
PY - 2021/11/2
Y1 - 2021/11/2
N2 - 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. © 2021 Wiley-VCH GmbH
AB - 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. © 2021 Wiley-VCH GmbH
KW - crystallographic-site-specific
KW - high-voltage spinel cathodes
KW - lithium-ion batteries
KW - structural engineering
KW - structure/function relation of materials
UR - https://www.scopus.com/pages/publications/85114169691
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85114169691&origin=recordpage
U2 - 10.1002/adma.202101413
DO - 10.1002/adma.202101413
M3 - RGC 21 - Publication in refereed journal
C2 - 34480499
SN - 0935-9648
VL - 33
JO - Advanced Materials
JF - Advanced Materials
IS - 44
M1 - 2101413
ER -
SDG 7 Affordable and Clean Energy