An Ordered P2/P3 Composite Layered Oxide Cathode with Long Cycle Life in Sodium-Ion Batteries

Muhammad Mominur Rahman, Jing Mao, Wang Hay Kan, Cheng Jun Sun, Luxi Li, Yan Zhang, Maxim Avdeev, Xi Wen Du, Feng Lin

Research output: Contribution to journalArticlepeer-review

44 Scopus citations

Abstract

Developing stable cathode materials represents a crucial step toward long-life sodium-ion batteries. P2-type layered oxides are important as cathodes for their reversibility, but their long-term performance in full cells remains a key challenge. Herein, we report Na0.75Co0.125Cu0.125Fe0.125Ni0.125Mn0.5O2 with an intergrowth of ordered P2 and P3 phases, studied by neutron diffraction and Rietveld refinement. A stable electrochemical performance is achieved in Na half cells with 100% capacity retention at a rate of C/10 after 100 cycles (initial capacity of 90 mAh/g), 96% capacity retention at a rate of 1 C after 500 cycles (initial capacity of 70 mAh/g), and 85% capacity retention at a rate of 5 C after 1000 cycles (initial capacity of 55 mAh/g). Stable full cell performance is achieved with 84.2% capacity retention after 1000 cycles at a rate of 1 C. Synchrotron X-ray diffraction, spectroscopy, and imaging are applied to elucidate the relationship between chemical/structural evolution and battery performance. A reversible local and global structural evolution is observed during initial cycles. Meanwhile, the challenges with enabling prolonged cycling (beyond 1000 cycles) may be associated with Fe dissolution and formation of a copper oxide phase. This study implies that cathodes with complex chemical and structural formations may stabilize electrochemical performance and highlights the importance of decoupling the contribution of each transition metal to performance degradation.

Original languageEnglish
Pages (from-to)573-581
Number of pages9
JournalACS Materials Letters
Volume1
Issue number5
DOIs
StatePublished - Nov 4 2019
Externally publishedYes

Funding

The work was supported by the Virginia Tech Department of Chemistry Startup Funds, 4-VA Collaborative Research, and National Science Foundation (No. CBET-1912885). Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-76SF00515. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory, under Contract No. DE-AC02-06CH11357. W.H.K. appreciates the beamtime in ECHIDNA granted from Australian Centre for Neutron Scattering (CSNS) in ANSTO. W.H.K. also is thankful for the support from the National Natural Science Foundation of China (Nos. 11805034 and 21704105), and Natural Science Foundation of Guangdong Province (No. 2017A030313021). The authors would like to acknowledge Dr. Linqin Mu and Zhengrui Xu for the fruitful discussions.

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