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Rescaling of metal oxide nanocrystals for energy storage having high capacitance and energy density with robust cycle life

Jeong, Hyung Mo and Choi, Kyung Min and Cheng, Tao and Lee, Dong Ki and Zhou, Renjia and Ock, Il Woo and Milliron, Delia J. and Goddard, William A., III and Kang, Jeung Ku (2015) Rescaling of metal oxide nanocrystals for energy storage having high capacitance and energy density with robust cycle life. Proceedings of the National Academy of Sciences of the United States of America, 112 (26). pp. 7914-7919. ISSN 0027-8424. PMCID PMC4491738. https://resolver.caltech.edu/CaltechAUTHORS:20150615-151220941

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Abstract

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:Li_2O), whereas subsequent delithiation causes Ni:Li_2O to form atomic clusters of NiO-a. This is consistent with in situ X-ray photoelectron and optical spectroscopy results showing that Ni^(2+) of the nanocrystal changes during lithiation–delithiation through Ni^0 and back to Ni^(2+). 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.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1073/pnas.1503546112DOIArticle
http://www.pnas.org/content/112/26/7914PublisherArticle
http://www.pnas.org/lookup/suppl/doi:10.1073/pnas.1503546112/-/DCSupplementalPublisherSupporting Information
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4491738/PubMed CentralArticle
ORCID:
AuthorORCID
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Kang, Jeung Ku0000-0003-3409-7544
Additional Information:© 2015 National Academy of Sciences. Contributed by William A. Goddard III, May 20, 2015 (sent for review December 9, 2014) Published online before print June 15, 2015, doi: 10.1073/pnas.1503546112. This research was supported by the Global Frontier R&D Program (2013M3A6B1078865) on Center for Hybrid Interface Materials funded by the Ministry of Science, Information and Communication Technology and Future Planning, and the National Research Foundation of Korea (2011-0028737, 2012M1A2A2671813). The work at the Molecular Foundry was supported by the US Department of Energy (DOE) under Contract DE-AC02-05CH11231. D.J.M. was supported by DOE Advanced Research Projects Agency-Energy under the same contract. Support for T.C. and W.A.G. was provided by National Science Foundation (CBET-1067848). Author contributions: H.M.J. and J.K.K. designed research; H.M.J., K.M.C., R.Z., I.W.O., and J.K.K. performed research; D.K.L. and I.W.O. contributed new reagents/analytic tools; T.C. and W.A.G. analyzed data; and H.M.J., K.M.C., T.C., D.J.M., W.A.G., and J.K.K. wrote the paper. The authors declare no conflict of interest. This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1503546112/-/DCSupplemental.
Funders:
Funding AgencyGrant Number
Ministry of Science, Information and Communication Technology and Future Planning (Korea)2013M3A6B1078865
National Research Foundation of Korea2011-0028737
National Research Foundation of Korea2012M1A2A2671813
Department of Energy (DOE)DE-AC02-05CH11231
NSFCBET-1067848
Subject Keywords:rescaled atomic clusters; metal oxide nanocrystals; energy storage; molecular dynamic simulation; in situ electrochemical spectroscopy
Issue or Number:26
PubMed Central ID:PMC4491738
Record Number:CaltechAUTHORS:20150615-151220941
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150615-151220941
Official Citation:Hyung Mo Jeong, Kyung Min Choi, Tao Cheng, Dong Ki Lee, Renjia Zhou, Il Woo Ock, Delia J. Milliron, William A. Goddard III, and Jeung Ku Kang Rescaling of metal oxide nanocrystals for energy storage having high capacitance and energy density with robust cycle life PNAS 2015 112 (26) 7914-7919; published ahead of print June 15, 2015, doi:10.1073/pnas.1503546112
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:58263
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:15 Jun 2015 22:55
Last Modified:09 Mar 2020 13:18

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