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Confinement of single polyoxometalate clusters in molecular-scale cages for improved flexible solid-state supercapacitors

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Abstract

Herein, we realized the supramolecular confinement of a single polyoxometalate (POM) cluster precisely in a polypyrrole (PPy) hydrogel-wrapped CNT framework with molecular-scale cages. This hybrid hydrogel framework demonstrated an ultra-high loading (67.5 wt%) and extremely uniform dispersion of individual of H3[P(Mo3O10)4] (PMo12) molecules, as demonstrated by sub-ångström-resolution HAADF-STEM. Consequently, it exhibited a better supercapacitor performance than that of the conventional composite system. The flexible solid-state supercapacitor exhibited a high energy density of 67.5 μW h cm−2 at a power density of 700 μW cm−2 and delivered a high capacitance retention of 85.7% after 3000 cycles. Moreover, the flexible device exhibited excellent mechanical stability. Density functional theory calculations revealed that the wrapped “fishnet-like” hydrogel creates a cage structure with a size of 1.8 nm for the precise storage of the PMo12 molecule (diameter = 1.05 nm), leading to the mono-dispersion of single PMo12 molecules on the hybrid hydrogel. The “caging” effect also activates the PMo12 molecule to enhance its charging/discharging performance by introducing new reactive sites for proton transfer. We believe that this design for suitable cage structures can be used for the construction of other POM-based hybrid hydrogels, thereby achieving mono-dispersity and performance enhancement.

Graphical abstract: Confinement of single polyoxometalate clusters in molecular-scale cages for improved flexible solid-state supercapacitors

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Supplementary files

Article information


Submitted
07 Feb 2020
Accepted
01 Apr 2020
First published
01 Apr 2020

Nanoscale, 2020, Advance Article
Article type
Paper

Confinement of single polyoxometalate clusters in molecular-scale cages for improved flexible solid-state supercapacitors

M. Wang, Y. Zhang, T. Zhang, Y. Li, M. Cui, X. Cao, Y. Lu, D. Peng, W. Liu, X. Liu, T. Wang and Y. Huang, Nanoscale, 2020, Advance Article , DOI: 10.1039/D0NR01070G

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