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Issue 2, 2016
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Nitrogen-doped carbons prepared from eutectic mixtures as metal-free oxygen reduction catalysts

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Abstract

Deep eutectic solvents (DESs) composed of resorcinol, either 2-cyanophenol or 4-cyanophenol, and choline chloride were used for the synthesis of hierarchical nitrogen-doped carbon molecular sieves. Carbons were obtained with high conversions by polycondensation of resorcinol and either 2-cyanophenol or 4-cyanophenol with formaldehyde, and subsequent carbonization at 800 °C in nitrogen atmosphere. The nitrogen content was ca. 2.4 wt%, revealing an excellent nitrogen-doping efficiency for cyanophenol derivatives when used in the form of DES. The use of either 2-cyanophenol or 4-cyanophenol modified the contribution of quaternary-Nvalley groups in the resulting carbons, being larger in carbons coming from 4-cyanophenol than in those coming from 2-cyanophenol. The hierarchical porous structure was composed of micro-, meso- and macropores, and the diameter distribution of mesopores was also related to the use of either 2-cyanophenol or 4-cyanophenol. These structural and compositional differences were critical for the use of the resulting hierarchical nitrogen-doped carbons as efficient metal-free electrocatalysts. In particular, the carbons coming 4-cyanophenol proved particularly effective in the direct reduction of oxygen to OH (H2O in acidic solution) through a four-electron (4e) process with high catalytic activity and selectivity, and longer stability and stronger tolerance to crossover effects than platinum-based electrocatalysts.

Graphical abstract: Nitrogen-doped carbons prepared from eutectic mixtures as metal-free oxygen reduction catalysts

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The article was received on 27 Oct 2015, accepted on 24 Nov 2015 and first published on 27 Nov 2015


Article type: Paper
DOI: 10.1039/C5TA08630B
Author version available: Download Author version (PDF)
Citation: J. Mater. Chem. A, 2016,4, 478-488
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    Nitrogen-doped carbons prepared from eutectic mixtures as metal-free oxygen reduction catalysts

    N. López-Salas, M. C. Gutiérrez, C. O. Ania, M. A. Muñoz-Márquez, M. Luisa Ferrer and F. D. Monte, J. Mater. Chem. A, 2016, 4, 478
    DOI: 10.1039/C5TA08630B

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