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Highly Efficient Oxygen Reduction Catalysts by Rational Synthesis of Nanoconfined Maghemite in a Nitrogen-Doped Graphene Framework

Qiu, K; Chai, G; Jiang, C; Ling, M; Tang, J; Guo, Z; (2016) Highly Efficient Oxygen Reduction Catalysts by Rational Synthesis of Nanoconfined Maghemite in a Nitrogen-Doped Graphene Framework. ACS Catalysis , 6 (6) pp. 3558-3568. 10.1021/acscatal.6b00531. Green open access

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Abstract

The oxygen reduction reaction (ORR) is critical for electrochemical energy storage and conversion: e.g., in fuel cells and metal–air batteries. A major challenge is to develop cost-effective and durable ORR catalysts, to replace the relatively expensive platinum-loaded carbon (PtC) counterparts, particularly for large-scale applications. Despite progress over the past few decades in developing efficient non-precious-metal (NPM) catalysts, such as Fe/N/C-based materials (the best-known alternatives), most of the reported catalytic activities have yet to match that of PtC. Herein we propose a two-step process for the production of highly efficient NPM catalysts that outperform PtC in alkaline media: (1) a hierarchical porosity of a supporting substrate is generated and optimized in advance, especially to achieve a high total pore volume for rapid mass transfer, and (2) an appropriate amount of NPM precursor is added to the optimized substrate to boost the reduction potential while maintaining the hierarchically porous structure. Such a scheme was successfully applied to a case of nanoconfined maghemite (γ-Fe2O3) in a nitrogen-doped graphene framework. The resulting catalyst system surpasses the performance of the equivalent commercial PtC, in terms of a higher reduction potential, a significantly lower peroxide formation ratio, more than tripled kinetic current density, smaller Tafel slope, better durability, etc. The reported catalyst is also among the best of all the existing Fe-based ORR catalysts, indicating the great potential of γ-Fe2O3 for ORR in practical applications.

Type: Article
Title: Highly Efficient Oxygen Reduction Catalysts by Rational Synthesis of Nanoconfined Maghemite in a Nitrogen-Doped Graphene Framework
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acscatal.6b00531
Publisher version: http://dx.doi.org/10.1021/acscatal.6b00531
Language: English
Additional information: ACS AuthorChoice - This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Keywords: Science & Technology, Physical Sciences, Chemistry, Physical, Chemistry, oxygen reduction reaction, hierarchical graphene framework, nitrogen doping, maghemite, alkaline electrolyte, HIGH-PERFORMANCE ELECTROCATALYST, CARBON CATALYSTS, ALKALINE MEDIA, POROUS CARBON, IRON PHTHALOCYANINE, TRANSITION-METALS, GRAPHITIC LAYERS, FE-N/C, CO, NANOPARTICLES
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/1508236
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