Unravelling the Nature of the Intrinsic Complex Structure of Binary‐Phase Na‐Layered Oxides
[6]
- Beamline Division PLS‐II Pohang Accelerator Laboratory (PAL) Pohang 37673 Republic of Korea
- Department of Printed Electronics Engineering Sunchon National University Chonnam 57922 Republic of Korea
- Division of Physics and Semiconductor Science Dongguk University 30, Pildong‐ro 1gil, Jung‐gu Seoul 04620 Republic of Korea
- Graduate School of Semiconductor Materials and Devices Engineering &, UNIST Central Research Facilities Ulsan 44919 Republic of Korea
- Faculty of Nanotechnology and Advanced Materials Engineering Sejong University Seoul 05006 Republic of Korea
- Electrochemical Energy Storage Department Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA
- Australian Nuclear Science and Technology Organization (ANSTO) New Illawarra Road Lucas Heights New South Wales 2234 Australia
Abstract The layered sodium transition metal oxide, NaTMO 2 (TM = transition metal), with a binary or ternary phases has displayed outstanding electrochemical performance as a new class of strategy cathode materials for sodium‐ion batteries (SIBs). Herein, an in‐depth phase analysis of developed Na 1− x TMO 2 cathode materials, Na 0.76 Ni 0.20 Fe 0.40 Mn 0.40 O 2 with P2‐ and O3‐type phases (NFMO‐P2/O3) is offered. Structural visualization on an atomic scale is also provided and the following findings are unveiled: i) the existence of a mixed‐phase intergrowth layer distribution and unequal distribution of P2 and O3 phases along two different crystal plane indices and ii) a complete reversible charge/discharge process for the initial two cycles that displays a simple phase transformation, which is unprecedented. Moreover, first‐principles calculations support the evidence of the formation of a binary NFMO‐P2/O3 compound, over the proposed hypothetical monophasic structures (O3, P3, O′3, and P2 phases). As a result, the synergetic effect of the simultaneous existence of P‐ and O‐type phases with their unique structures allows an extraordinary level of capacity retention in a wide range of voltage (1.5–4.5 V). It is believed that the insightful understanding of the proposed materials can introduce new perspectives for the development of high‐voltage cathode materials for SIBs.
- Sponsoring Organization:
- USDOE
- Grant/Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1871239
- Journal Information:
- Advanced Materials, Journal Name: Advanced Materials Journal Issue: 29 Vol. 34; ISSN 0935-9648
- Publisher:
- Wiley Blackwell (John Wiley & Sons)Copyright Statement
- Country of Publication:
- Germany
- Language:
- English
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