Local structure adaptability through multi cations for oxygen redox accommodation in Li-Rich layered oxides

Enyue Zhao, Minghao Zhang, Xuelong Wang, Enyuan Hu, Jue Liu, Xiqian Yu, Marco Olguin, Thomas A. Wynn, Ying Shirley Meng, Katharine Page, Fangwei Wang, Hong Li, Xiao Qing Yang, Xuejie Huang, Liquan Chen

Research output: Contribution to journalArticlepeer-review

126 Scopus citations

Abstract

Stable lattice oxygen redox (l-OR) is the key enabler for achieving attainable high energy density in Li-rich layered oxide cathode materials for Li-ion batteries. However, the unique local structure response to oxygen redox in these materials, resulting in energy inefficiency and hysteresis, still remains elusive, preventing their potential applications. By combining the state-of-the-art neutron pair distribution function with crystal orbital overlap analysis, we directly observe the distinct local structure adaption originated from the potential O–O chemical bonds. The structure adaptability is optimized based on the nature of multi transition metals in our model compound Li1.2Ni0.13Mn0.54Co0.13O2, which accommodates the oxygen redox and at the same time preserves the global layered structure. These findings not only advance the understanding of l-OR, but also provide new perspectives in the rational design of high-energy-density cathode materials with reversible and stable l-OR.

Original languageEnglish
Pages (from-to)384-393
Number of pages10
JournalEnergy Storage Materials
Volume24
DOIs
StatePublished - Jan 2020

Funding

The work done at Institute of Physics , Chinese Academy of Sciences was supported by funding from National Key R&D Program of China ( 2016YFB0100100 ), National Materials Genome Project ( 2016YFB0100106 ), NSFC (Grant No. 11675255 , 51502334 , 51822211 ) and “Thousand Talents Program for Young Scientists”. The work done at UCSD was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract DE-AC02-05CH11231 , Subcontract 7073923, under the Advanced Battery Materials Research (BMR) Program. Research conducted at the NOMAD beamline at ORNL’s SNS was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, USDOE . J.L. and K.P are partially supported by U.S. DOE , Office of Science , Office of Basic Energy Sciences , Early Career Research Program award KC040602 , under contract number DE-AC05-00OR22725 . The work at BNL were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the BMR Program, including Battery 500 Consortium under contract DE-SC0012704. The authors are very indebted to Prof. Yonggao Xia (Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences ) for the insightful discussion on this paper. sXAS data were collected at beamline 8.0.1 of the ALS, which is supported by the Director, Office of Science , Office of Basic Energy Sciences , of the U.S. DOE under Contract No. DE-AC02-05CH11231 . We thank the help from beamline BL14W1 at SSRL, China. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. DOE. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. The work done at Institute of Physics, Chinese Academy of Sciences was supported by funding from National Key R&D Program of China (2016YFB0100100), National Materials Genome Project (2016YFB0100106), NSFC (Grant No. 11675255, 51502334, 51822211) and ?Thousand Talents Program for Young Scientists?. The work done at UCSD was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract DE-AC02-05CH11231, Subcontract 7073923, under the Advanced Battery Materials Research (BMR) Program. Research conducted at the NOMAD beamline at ORNL's SNS was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, USDOE. J.L. and K.P are partially supported by U.S. DOE, Office of Science, Office of Basic Energy Sciences, Early Career Research Program award KC040602, under contract number DE-AC05-00OR22725. The work at BNL were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the BMR Program, including Battery 500 Consortium under contract DE-SC0012704. The authors are very indebted to Prof. Yonggao Xia (Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences) for the insightful discussion on this paper. sXAS data were collected at beamline 8.0.1 of the ALS, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. DOE under Contract No. DE-AC02-05CH11231. We thank the help from beamline BL14W1 at SSRL, China. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. DOE. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan.

Keywords

  • Lattice oxygen redox
  • Lithium-ion battery
  • Lithium-rich cathode
  • Local structure
  • Pair distribution function

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