LiNi0.8Co0.1Mn0.1O2 (NCM) can
achieve a high capacity of more than 200 mAh g–1 at charging voltages above 4.5 V, but it suffers from severe capacity
fading at a high voltage during cycling associated with the lattice
oxygen evolution-induced phase and surface structure modifications.
Therefore, the big challenge for improving electrochemical performance
is suppressing the lattice oxygen loss at a high voltage. Here, a
facile strategy to inhibit the lattice oxygen loss of a Ni-rich material
at a high charging voltage by a simple Sr treatment method is reported.
The Sr treatment leads to the formation of a Sr-based sub/surface
integrated layer and induces the atomic rearrangement on the subsurface
to form Sr-based perovskite-like Li
x
Sr1–x
TMO3 (TM = Ni, Co and
Mn) during the heat treatment process. The perovskite-like structure
can adsorb the oxidized Oα– to oxygen vacancies,
transplant the pumped charges from the oxidized Oα–, and reduce them back to O2–
to inhibit
the movement of oxidized oxygen anions at the charged NCM surface.
Furthermore, the formed Sr1–x
HPO4 outer layer can prevent NCM from corroding by HF in organic
electrolytes. Meanwhile, bulk doping stabilizes the metal–oxygen
bond by suppressing the Ni migration at a high charging voltage. The
modified NCM thus exhibited a significantly enhanced high-voltage
cycle stability with 82.3 and 80.1% of capacity retentions at 1C achieved
after 250 cycles at 25 °C and 100 cycles at 60 °C, respectively.
This work opened a new avenue to suppress the lattice oxygen loss
via surface structure regulations in high-energy-density rechargeable
batteries during high-voltage cycling.