Abstract
We report a (Ni)MnO2 layered birnessite material with a framwork doping of Ni ions as the cathode for much enhanced aqueous Na-ion storage. Characterized by neutron total scattering and pair distribution function (PDF) analysis, in situ XRD, in situ X-ray PDF, XANES, and XPS, the synergistic interaction between disordered [NiO6] and ordered [MnO6] octahedra contribute to the enhanced specific capacity and cycle life (63 mAh g-1 at 0.2 A g-1 after 2000 full-cell cycles). Electro-kinetic analysis and structural characterizations show that stable local structure is maintained by [MO6] octahedra during charge-discharge processes, while disordered [NiO6] octahedra significantly improve pseudocapacitive redox charge storage. This finding may pave a new way for designing a new type of low-cost and high performance layered electrode materials.
Original language | English |
---|---|
Pages (from-to) | 8774-8786 |
Number of pages | 13 |
Journal | Chemistry of Materials |
DOIs | |
State | Published - 2019 |
Funding
This work was supported by the US Department of Energy (DOE), Office of Science Basic Energy Sciences, under Award DE-SC0018922 (X.S., F.G., X.T.). Research conducted at ORNL's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy, under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory. Electron microscopy work was performed at the Center for Functional Nanomaterials, Brookhaven National Laboratory supported by U.S. Department of Energy, Office of Basic Energy Sciences under Contract DE-SC-00112704. This research used 6-BM-B and 28-ID-1 beamlines of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. X.S. contributed to the material synthesis, characterizations, electrochemical experimental measurements and analysis, and neutron and X-ray PDF analysis. F.G. contributed to half-cell measurements. K.P. and J.C.N. contributed to neutron measurements. D.S. contributed to the HRTEM and EDXS mapping measurements. X.S., A.M.M.A., G.K., and D.O. contributed to X-ray measurements. X.S., X.T., and B.R. contributed to XANES measurements. X.T. contributed to XANES analysis. X.S. and X.T. contributed to the research design and manuscript preparation. X.T. supervised the project. All authors discussed the results and commented on the manuscript. This work was supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences, under Award DE-SC0018922 (X.S., F.G., X.T.). Research conducted at ORNL’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy, under Contract No. DE-AC05-00OR22725 with Oak Ridge National Laboratory. Electron microscopy work was performed at the Center for Functional Nanomaterials, Brookhaven National Laboratory, supported by U.S. Department of Energy, Office of Basic Energy Sciences, under Contract DE-SC-00112704. This research used 6-BM-B and 28-ID-1 beamlines of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. The authors declare no competing financial interest.