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Maximizing the utilization of Fe-NxC/CNx centres for an air-cathode material and practical demonstration of metal-air batteries

Nandan, R and Gautam, A and Nanda, K K (2017) Maximizing the utilization of Fe-NxC/CNx centres for an air-cathode material and practical demonstration of metal-air batteries. In: JOURNAL OF MATERIALS CHEMISTRY A, 5 (38). pp. 20252-20262.

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Official URL: http://doi.org/10.1039/c7ta06254k


Noble-metal free carbon-based electrocatalysts for oxygen reduction/evolution reaction (ORR/OER) in an alkaline medium have drawn significant attention in the search of suitable/potential replacement of commercial expensive Pt/Ru/Ir-based electrocatalysts. In this regard, nitrogen-doped carbon nanotubes (NCNTs) have emerged as potential candidates for ORR/OER and they emulate Pt/Ru-based catalysts. However, the unexposed/unused active sites rendered by N-doping, responsible for bamboo-shaped compartment formation, in NCNTs are hardly accessible to the reactant species and thus barely contribute to ORR/OER. To maximize the utilization of the active centres, Fe-Fe3C nanoparticles entrapped in the graphitic layers and hollow structures of NCNTs are fabricated by pyrolyzing melamine with excess of ferrocene. Annealing at 375 degrees C in an oxygen environment removes the protective graphitic layers around Fe-Fe3C, and acid-treatment provides an opening to the bamboo compartments of NCNTs (ANCNTs); this offers maximum accessibility of the active sites via the creation of more edges and roughness that enhances the ORR/OER activity. Interestingly, more positive ORR onset and halfwave potentials with excellent accelerated stability (similar to 98% current retention) and fuel tolerance along with lower onset and E-j=10(OER) potential with high OER current density as compared to those of commercial state-of-the-art electrocatalyst suggest the superior bifunctional behaviour of ANCNTs. The poisoning study with NaSCN on ANCNTs shows the direct involvement of Fe-based centres in oxygen electrochemistry. The overall oxygen electroactivity Delta E = E-j(OER)=10 - E-1/2(ORR) = 0.72 V for ANCNTs is much lower than that of the commercial and recently reported various state-of-the-art bifunctional catalysts. Finally, a prototype battery arrangement using NCNTs as a cathode electrode for powering a light-emitting diode has been demonstrated. Overall, NCNTs can serve as non-precious electrocatalysts for electrochemical energy devices.

Item Type: Journal Article
Additional Information: Copy right for this article belongs to the ROYAL SOC CHEMISTRY, THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND
Department/Centre: Division of Chemical Sciences > Materials Research Centre
Division of Electrical Sciences > Electronic Systems Engineering (Formerly Centre for Electronic Design & Technology)
Depositing User: Id for Latest eprints
Date Deposited: 03 Nov 2017 10:41
Last Modified: 03 Nov 2017 10:41
URI: http://eprints.iisc.ac.in/id/eprint/58152

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