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Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries.
Small. 2020 Jun; 16(25):e2001524.S

Abstract

Developing high-voltage cathode materials is critical for sodium-ion batteries to boost energy density. NASICON (Na super-ionic conductor)-structured Nax MnM(PO4)3 materials (M represents transition metal) have drawn increasing attention due to their features of robust crystal framework, low cost, as well as high voltage based on Mn4+ /Mn3+ and Mn3+ /Mn2+ redox couples. However, full activation of Mn4+ /Mn3+ redox couple within NASICON framework is still a great challenge. Herein, a novel NASICON-type Na4 MnCr(PO4)3 material with highly reversible Mn4+ /Mn3+ redox reaction is discovered. It proceeds a two-step reaction with voltage platforms centered at 4.15 and 3.52 V versus Na+ /Na, delivering a capacity of 108.4 mA h g-1 . The Na4 MnCr(PO4)3 cathode also exhibits long durability over 500 cycles and impressive rate capability up to 10 C. The galvanostatic intermittent titration technique (GITT) test shows fast Na diffusivity which is further verified by density functional theory calculations. The high electrochemical activity derives from the 3D robust framework structure, fast kinetics, and pseudocapacitive contribution. The sodium storage mechanism of the Na4 MnCr(PO4)3 cathode is deeply studied by ex situ X-ray diffraction (XRD) and ex situ X-ray photoelectron spectroscopy (XPS), revealing that both solid-solution and two-phase reactions are involved in the Na+ ions extraction/insertion process.

Authors+Show Affiliations

School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong, P. R. China.School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.Department of Applied Physics, Hong Kong Polytechnic University, Kowloon, Hong Kong, P. R. China.School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong Innovation Campus, Squires Way, North Wollongong, NSW, 2522, Australia.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

32452618

Citation

Zhang, Wei, et al. "Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries." Small (Weinheim an Der Bergstrasse, Germany), vol. 16, no. 25, 2020, pp. e2001524.
Zhang W, Li H, Zhang Z, et al. Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries. Small. 2020;16(25):e2001524.
Zhang, W., Li, H., Zhang, Z., Xu, M., Lai, Y., & Chou, S. L. (2020). Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries. Small (Weinheim an Der Bergstrasse, Germany), 16(25), e2001524. https://doi.org/10.1002/smll.202001524
Zhang W, et al. Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries. Small. 2020;16(25):e2001524. PubMed PMID: 32452618.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Full Activation of Mn4+ /Mn3+ Redox in Na4 MnCr(PO4)3 as a High-Voltage and High-Rate Cathode Material for Sodium-Ion Batteries. AU - Zhang,Wei, AU - Li,Huangxu, AU - Zhang,Zhian, AU - Xu,Ming, AU - Lai,Yanqing, AU - Chou,Shu-Lei, Y1 - 2020/05/26/ PY - 2020/03/08/received PY - 2020/04/05/revised PY - 2020/5/27/pubmed PY - 2020/5/27/medline PY - 2020/5/27/entrez KW - Mn 4+/Mn 3+ redox couple KW - NASICON structure KW - Na 4MnCr(PO 4) 3 KW - cathode materials KW - sodium-ion batteries SP - e2001524 EP - e2001524 JF - Small (Weinheim an der Bergstrasse, Germany) JO - Small VL - 16 IS - 25 N2 - Developing high-voltage cathode materials is critical for sodium-ion batteries to boost energy density. NASICON (Na super-ionic conductor)-structured Nax MnM(PO4)3 materials (M represents transition metal) have drawn increasing attention due to their features of robust crystal framework, low cost, as well as high voltage based on Mn4+ /Mn3+ and Mn3+ /Mn2+ redox couples. However, full activation of Mn4+ /Mn3+ redox couple within NASICON framework is still a great challenge. Herein, a novel NASICON-type Na4 MnCr(PO4)3 material with highly reversible Mn4+ /Mn3+ redox reaction is discovered. It proceeds a two-step reaction with voltage platforms centered at 4.15 and 3.52 V versus Na+ /Na, delivering a capacity of 108.4 mA h g-1 . The Na4 MnCr(PO4)3 cathode also exhibits long durability over 500 cycles and impressive rate capability up to 10 C. The galvanostatic intermittent titration technique (GITT) test shows fast Na diffusivity which is further verified by density functional theory calculations. The high electrochemical activity derives from the 3D robust framework structure, fast kinetics, and pseudocapacitive contribution. The sodium storage mechanism of the Na4 MnCr(PO4)3 cathode is deeply studied by ex situ X-ray diffraction (XRD) and ex situ X-ray photoelectron spectroscopy (XPS), revealing that both solid-solution and two-phase reactions are involved in the Na+ ions extraction/insertion process. SN - 1613-6829 UR - https://www.unboundmedicine.com/medline/citation/32452618/Full_Activation_of_Mn4+_/Mn3+_Redox_in_Na4_MnCr_PO4_3_as_a_High_Voltage_and_High_Rate_Cathode_Material_for_Sodium_Ion_Batteries_ L2 - https://doi.org/10.1002/smll.202001524 DB - PRIME DP - Unbound Medicine ER -
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