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Ionothermal Synthesis of High-Voltage Alluaudite Na2+2xFe2-x(SO4)(3) Sodium Insertion Compound: Structural, Electronic, and Magnetic Insights
Indian Inst Sci, Mat Res Ctr, Faraday Mat Lab, CV Raman Ave, Bangalore 560012, Karnataka, India..
Univ Sydney, Sch Chem, Bldg F11, Sydney, NSW 2006, Australia..
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
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2016 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 8, no 11, 6982-6991 p.Article in journal (Refereed) PublishedText
Abstract [en]

Exploring future cathode materials for sodium-ion batteries, alluaudite class of Na2Fe2II(SO4)(3) has been recently unveiled as a 3.8 V positive insertion candidate (Barpanda et al. Nat. Commun. 2014, 5, 4358). It forms an Fe-based polyanionic compound delivering the highest Fe-redox potential along with excellent rate kinetics and reversibility. However, like all known SO4-based insertion materials, its synthesis is cumbersome that warrants careful processing avoiding any aqueous exposure. Here, an alternate low temperature ionothermal synthesis has been described to produce the alluaudite Na2+2xFe2-xII(SO4)(3). It marks the first demonstration of solvothermal synthesis of alluaudite Na2+2xM2-xII(SO4)(3) (M = 3d metals) family of cathodes. Unlike classical solid-state route, this solvothermal route favors sustainable synthesis of homogeneous nanostructured alluaudite products at only 300 degrees C, the lowest temperature value until date. The current work reports the synthetic aspects of pristine and modified ionothermal synthesis of Na2+2xFe2-xII(SO4)(3) having tunable size (300 nm similar to 5 mu m) and morphology. It shows antiferromagnetic ordering below 12 K. A reversible capacity in excess of 80 mAh/g was obtained with good rate kinetics and cycling stability over 50 cycles. Using a synergistic approach combining experimental and ab initio DFT analysis, the structural, magnetic, electronic, and electrochemical properties and the structural limitation to extract full capacity have been described.

Place, publisher, year, edition, pages
2016. Vol. 8, no 11, 6982-6991 p.
Keyword [en]
sodium-ion battery, alluaudite, Na2Fe2(SO4)(3), ionothermal synthesis, DFT
National Category
Materials Engineering
URN: urn:nbn:se:uu:diva-294306DOI: 10.1021/acsami.5b11302ISI: 000372946600024PubMedID: 26931644OAI: oai:DiVA.org:uu-294306DiVA: diva2:929458
Carl Tryggers foundation Swedish Research CouncilStandUp
Available from: 2016-05-18 Created: 2016-05-18 Last updated: 2016-05-18Bibliographically approved

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Araujo, Rafael B.Chakraborty, SudipAhuja, Rajeev
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