Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 8, Issue 11, Pages 6982-6991Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.5b11302
Keywords
sodium-ion battery; alluaudite; Na2Fe2(SO4)(3); ionothermal synthesis; DFT
Funding
- Department of Science and Technology (DST), Govt. of India under the aegis of Solar Energy Research Initiative (SERI) programme [DST/TMC/SERI/FR/169]
- Ministry of Human Resource Development (MHRD)
- Australian Research Council
- Erasmus Mundus
- Carl Tryggers Stiftelse for Vetenskaplig Forskning (CTS)
- Swedish Research Council (VR)
- STandUP
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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.
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