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Metal-Organic Framework-Assisted Synthesis of Compact Fe₂O₃ Nanotubes in Co₃O₄ Host with Enhanced Lithium Storage Properties.

ABSTRACT: Transition metal oxides are promising candidates for the high-capacity anode material in lithium-ion batteries. The electrochemical performance of transition metal oxides can be improved by constructing suitable composite architectures. Herein, we demonstrate a metal-organic framework (MOF)-assisted strategy for the synthesis of a hierarchical hybrid nanostructure composed of Fe₂O₃ nanotubes assembled in Co₃O₄ host. Starting from MOF composite precursors (Fe-based MOF encapsulated in a Co-based host matrix), a complex structure of Co₃O₄ host and engulfed Fe₂O₃ nanotubes was prepared by a simple annealing treatment in air. By virtue of their structural and compositional features, these hierarchical composite particles reveal enhanced lithium storage properties when employed as anodes for lithium-ion batteries.

SUBMITTER: Zhang SL

PROVIDER: S-EPMC6199090 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Precisely locating extra-framework cations in anionic metal-organic framework compounds remains a long-standing, yet crucial, challenge for elucidating structure-performance relationships in functional materials. Single-crystal X-ray diffraction is one of the most powerful approaches for this task, but single crystals of frameworks often degrade when subjected to post-synthetic metalation or reduction. Here, we demonstrate the growth of sizable single crystals of the robust metal-organic framework Fe2(bdp)3 (bdp2- = benzene-1,4-dipyrazolate) and employ single-crystal-to-single-crystal chemical reductions to access the solvated framework materials A2Fe2(bdp)3·yTHF (A = Li+, Na+, K+). X-ray diffraction analysis of the sodium and potassium congeners reveals that the cations are located near the center of the triangular framework channels and are stabilized by weak cation-π interactions with the framework ligands. Freeze-drying with benzene enables isolation of activated single crystals of Na0.5Fe2(bdp)3 and Li2Fe2(bdp)3 and the first structural characterization of activated metal-organic frameworks wherein extra-framework alkali metal cations are also structurally located. Comparison of the solvated and activated sodium-containing structures reveals that the cation positions differ in the two materials, likely due to cation migration that occurs upon solvent removal to maximize stabilizing cation-π interactions. Hydrogen adsorption data indicate that these cation-framework interactions are sufficient to diminish the effective cationic charge, leading to little or no enhancement in gas uptake relative to Fe2(bdp)3. In contrast, Mg0.85Fe2(bdp)3 exhibits enhanced H2 affinity and capacity over the non-reduced parent material. This observation shows that increasing the charge density of the pore-residing cation serves to compensate for charge dampening effects resulting from cation-framework interactions and thereby promotes stronger cation-H2 interactions.

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Metal-Organic Framework-Assisted Synthesis of Compact Fe2O3 Nanotubes in Co3O4 Host with Enhanced Lithium Storage Properties.

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Metal-Organic Framework-Assisted Synthesis of Compact Fe₂O₃ Nanotubes in Co₃O₄ Host with Enhanced Lithium Storage Properties.