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Valence Change Ability and Geometrical Occupation of Substitution Cations Determine the Pseudocapacitance of Spinel Ferrite XFe₂O₄ (X = Mn, Co, Ni, Fe) Public Deposited

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  • In recent years, spinel ferrites have attracted much attention as a merging material for oxygen reduction reaction (ORR),(1) advanced battery electrodes,(2, 3) and supercapacitors.(4, 5) Generally, the spinel structure can be described by a formula [X₁−λ²⁺Bλ³⁺]ᵀ[Xλ²⁺B₂−λ³⁺]ᴼ O₄, where λ is the inversion degree in-between 0 and 1, and superscripts T and O denote the tetrahedral and octahedral sites, respectively. Depending on the cation distribution, a spinel can be normal (λ = 0, 100% X in tetrahedral sites), inverse (λ = 1, 100% X in octahedral sites), or partially inverse (0 < λ < 1). Previous studies on spinel ferrites focused intensively on their magnetic properties,(6, 7) as the substitution of Fe cations by transition metals can affect the cation distribution, thus resulting in significantly different magnetic properties due to the regulation of the unpaired electron spins of Fe²⁺ in octahedral sites.(8, 9) Recent studies also showed that this substitution affects their electrochemical performance. For example, Mn substituted ferrites show nearly the same ORR activity as Pt/C in alkaline and Mn substitution also influences the capacitance more than other metal ion substituted ferrites.(1, 10) Such difference on electrochemical performance could be ascribed to the type of substituent cations and their influence. However, no systematic mechanistic investigation has been carried out. This lack of knowledge hinders the understanding of the substitution effects on the performance and, thus, the development of spinel ferrites as energy materials.
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  • Wei, C., Feng, Z., Baisariyev, M., Yu, L., Zeng, L., Wu, T., ... & Xu, Z. J. (2016). Valence Change Ability and Geometrical Occupation of Substitution Cations Determine the Pseudocapacitance of Spinel Ferrite XFe₂O₄ (X= Mn, Co, Ni, Fe). Chemistry of Materials, 28(12), 4129-4133. doi:10.1021/acs.chemmater.6b00713
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  • 28
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  • 12
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  • This work was supported by the Singapore Ministry of Education Tier 1 Grants (RGT13/13 and RG131/14) and the Singapore National Research Foundation under its Campus for Research Excellence And Technological Enterprise (CREATE) programme. LZ and MJB were supported by the MRSEC funded by NSF under DMR-1121262. The Advanced Photon Source (APS) at Argonne National Laboratory is supported by DOE under DE-AC02-06CH11357.
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  • description.provenance : Approved for entry into archive by Patricia Black(patricia.black@oregonstate.edu) on 2016-08-05T20:20:26Z (GMT) No. of bitstreams: 3 krauserp1418436277.zip: 6111795 bytes, checksum: a1698f53273d51ca8875d347eeb988ae (MD5) WeiValenceChangeAbility.pdf: 1506652 bytes, checksum: 8c177e67b7001fd9a5524c587b21a33f (MD5) WeiValenceChangeAbilitySupportingInfo.pdf: 5099047 bytes, checksum: 33e7dc44bc241925ee525b02f166d36c (MD5)
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