A rational synthesis of hierarchically porous, N-doped carbon from Mg-based MOFs: understanding the link between nitrogen content and oxygen reduction electrocatalysis

Controlled mixtures of novel Mg-based metal-organic frameworks (MOFs) were prepared, with H + or K + as counterions. A linear relation was found between synthesis pH and K/H ratio in the resultant mixture, establishing the tunability of the synthesis. Upon pyrolysis, these precursor mixtures yield n...

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Bibliographic Details
Published in:Physical chemistry chemical physics : PCCP 2016-07, Vol.18 (3), p.2778-2783
Main Authors: Eisenberg, David, Stroek, Wowa, Geels, Norbert J, Tanase, Stefania, Ferbinteanu, Marilena, Teat, Simon J, Mettraux, Pierre, Yan, Ning, Rothenberg, Gadi
Format: Article
Language:English
Subjects:
Carbon
Electrocatalysis
Metal-organic frameworks
Nitrogen
Oxygen
Reduction
Synthesis
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Summary:Controlled mixtures of novel Mg-based metal-organic frameworks (MOFs) were prepared, with H + or K + as counterions. A linear relation was found between synthesis pH and K/H ratio in the resultant mixture, establishing the tunability of the synthesis. Upon pyrolysis, these precursor mixtures yield nitrogen-doped, hierarchically porous carbons, which have good activity towards the oxygen reduction reaction (ORR) at pH 13. The nitrogen content varies significantly along the homologous carbon series (>400%, 1.3 at% to 5.7 at%), to a much greater extent than microstructural parameters such as surface area and graphitization. This allows us to isolate the positive correlation between nitrogen content and electrocatalytic oxygen reduction ORR activity in this class of metal-free, N-doped, porous carbons. The nitrogen content of porous carbons prepared from Mg-based MOFs, could be easily controlled by simply varying the solution pH.
ISSN:1463-9076
1463-9084
DOI:10.1039/c6cp04132a