Rescaling of metal oxide nanocrystals for energy storage having high capacitance and energy density with robust cycle life
- Rescaling of metal oxide nanocrystals for energy storage having high capacitance and energy density with robust cycle life
- 이동기; 정형모; 최경민; Tao Cheng; Renjia Zhou; 옥일우; Delia J. Milliron; William A. Goddard III; 강정구
- Issue Date
- Proceedings of the National Academy of Sciences of the United States of America
- VOL 112, NO 26-7919
- Nanocrystals are promising structures, but they are too large for achieving maximum energy storage performance. We show that rescaling 3-nm particles through lithiation followed by delithiation leads to high-performance energy storage by realizing high capacitance close to the theoretical capacitance available via ion-to-atom redox reactions. Reactive force-field (ReaxFF) molecular dynamics simulations support the conclusion that Li atoms react with nickel oxide nanocrystals (NiO-n) to form lithiated core-shell structures (Ni:Li2O), whereas subsequent delithiation causes Ni:Li2O to form atomic clusters of NiO-a. This is consistent with in situ X-ray photoelectron and optical spectroscopy results showing that Ni2+ of the nanocrystal changes during lithiation-delithiation through Ni-0 and back to Ni2+. These processes are also demonstrated to provide a generic route to rescale another metal oxide. Furthermore, assembling NiO-a into the positive electrode of an asymmetric device enables extraction of full capacitance for a counter negative electrode, giving high energy density in addition to robust capacitance retention over 100,000 cycles.
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