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Issue 47, 2013
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Understanding the origin of high-rate intercalation pseudocapacitance in Nb2O5 crystals

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Pseudocapacitors aim to maintain the high power density of supercapacitors while increasing the energy density towards those of energy dense storage systems such as lithium ion batteries. Recently discovered intercalation pseudocapacitors (e.g. Nb2O5) are particularly interesting because their performance is seemingly not limited by surface reactions or structures, but instead determined by the bulk crystalline structure of the material. We study ordered polymorphs of Nb2O5 and detail the mechanism for the intrinsic high rates and energy density observed for this class of materials. We find that the intercalating atom (lithium) forms a solid solution adsorbing at specific sites in a network of quasi-2D NbOx faces with x = {1.3, 1.67, or 2}, donating electrons locally to its neighboring atoms, reducing niobium. Open channels in the structure have low diffusion barriers for ions to migrate between these sites (Eb ∼ 0.28–0.44 eV) comparable to high-performance solid electrolytes. Using a combination of complementary theoretical methods we rationalize this effect in LixNb2O5 for a wide range of compositions (x) and at finite temperatures. Multiple adsorption sites per unit-cell with similar adsorption energies and local charge transfer result in high capacity and energy density, while the interconnected open channels lead to low cost diffusion pathways between these sites, resulting in high power density. The nano-porous structure exhibiting local chemistry in a crystalline framework is the origin of high-rate pseudocapacitance in this new class of intercalation pseudocapacitor materials. This new insight provides guidance for improving the performance of this family of materials.

Graphical abstract: Understanding the origin of high-rate intercalation pseudocapacitance in Nb2O5 crystals

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Publication details

The article was received on 20 Aug 2013, accepted on 02 Oct 2013 and first published on 03 Oct 2013

Article type: Paper
DOI: 10.1039/C3TA13316H
Citation: J. Mater. Chem. A, 2013,1, 14951-14956

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    Understanding the origin of high-rate intercalation pseudocapacitance in Nb2O5 crystals

    A. A. Lubimtsev, P. R. C. Kent, B. G. Sumpter and P. Ganesh, J. Mater. Chem. A, 2013, 1, 14951
    DOI: 10.1039/C3TA13316H

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