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Issue 5, 2017
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Spontaneous linker-free binding of polyoxometalates on nitrogen-doped carbon nanotubes for efficient water oxidation

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Abstract

Efficient water oxidation remains a principal challenge for clean fuels via water splitting. Polyoxometalates (POMs) are promising water oxidation catalysts in a neutral medium but their application is commonly limited by low electrical conductivity and poor adhesiveness arising from bulky and electrically insulating ligands. Here we report linker-free spontaneous binding of tetracobalt-based polyoxometalates (Co4POMs) on nitrogen-doped carbon nanotubes (NCNTs) via electrostatic hybridization. Protonated nitrogen-dopant sites at NCNTs enable linker-free immobilization of the Co4POMs and fluent electron transfer in the resultant Co4POM/NCNT hybrid structures, as demonstrated by the low overpotential of 370 mV for the water oxidation at pH 7. Accordingly, the hybrids exhibit fast reaction kinetics with a turnover frequency of 0.211 s−1 at 2.01 V vs. RHE. Density functional theory calculation proposes that POMs vertically align at the NCNT surface exposing the maximal catalytic surfaces. This work suggests a reliable route to highly efficient water oxidation catalysis by employing POMs under neutral conditions and NCNTs as self-binding nanoelectrodes in a synergistic well-oriented hybrid structure.

Graphical abstract: Spontaneous linker-free binding of polyoxometalates on nitrogen-doped carbon nanotubes for efficient water oxidation

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Publication details

The article was received on 27 Oct 2016, accepted on 03 Jan 2017 and first published on 03 Jan 2017


Article type: Communication
DOI: 10.1039/C6TA09306J
Citation: J. Mater. Chem. A, 2017,5, 1941-1947
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    Spontaneous linker-free binding of polyoxometalates on nitrogen-doped carbon nanotubes for efficient water oxidation

    G. Y. Lee, I. Kim, J. Lim, M. Y. Yang, D. S. Choi, Y. Gu, Y. Oh, S. H. Kang, Y. S. Nam and S. O. Kim, J. Mater. Chem. A, 2017, 5, 1941
    DOI: 10.1039/C6TA09306J

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