Aminotriazine derived N-doped mesoporous carbon with a tunable nitrogen content and their improved oxygen reduction reaction performance

Davidraj, Jefrin M.; Sathish, C. I.; Selvarajan, Premkumar; Fawaz, Mohammed; Perumalsamy, Vibin; Yu, Xiaojiang; Breese, Mark B. H.; Yi, Jiabao; Vinu, Ajayan

Title: Aminotriazine derived N-doped mesoporous carbon with a tunable nitrogen content and their improved oxygen reduction reaction performance
Creator: Davidraj, Jefrin M.; Sathish, C. I.; Selvarajan, Premkumar; Fawaz, Mohammed; Perumalsamy, Vibin; Yu, Xiaojiang; Breese, Mark B. H.; Yi, Jiabao; Vinu, Ajayan
Relation: ARC.DP220103045
Relation: Nanoscale Vol. 16, Issue 35, p. 16439-16450
Publisher Link: http://dx.doi.org/10.1039/d4nr02425g
Publisher: Royal Society of Chemistry
Resource Type: journal article
Date: 2024
Description: The electrocatalytic activity of carbon materials is highly dependent on the controlled modulation of their composition and porosity. Herein, mesoporous N-doped carbon with different amounts of nitrogen was synthesized through a unique strategy of using a high nitrogen containing CN precursor, 3-amino 1,2,4 triazine (3-ATZ) which is generally used for the preparation of carbon nitrides, integrated with the combination of a templating method and high temperature treatment. The nitrogen content and the graphitisation of the prepared materials were finely tuned with the simple adjustment of the carbonisation temperature (800–1100 °C). The optimised sample as an electrocatalyst for oxygen reduction reaction (ORR) exhibited an onset potential of 0.87 V vs. RHE with a current density of 5.1 mA cm−2 and a high kinetic current density (Jk) of 33.1 mA cm−2 at 0.55 V vs. RHE. The characterisation results of the prepared materials indicated that pyridinic and graphitic nitrogen in the carbon framework promoted ORR activity with improved four-electron selectivity and excellent methanol tolerance and stability. DFT calculations demonstrated that the structural and planar defects in the N-doped carbon regulated the surface electronic properties of the electrocatalyst, leading to a reduction in the energy barrier for the ORR activity. This strategy has the potential to unlock a platform for designing a series of catalysts for electrochemical applications.
Subject: carbon nitride; electrocatalysts; nitrogen; doping; oxygen reduction reaction
Identifier: http://hdl.handle.net/1959.13/1515769
Identifier: uon:56912
Identifier: ISSN:2040-3372
Language: eng
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