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Designing Highly Efficient Dual-Metal Single-Atom Electrocatalysts for Oxygen Reduction Reaction Inspired by Biological Enzyme System

Abstract

Biological Heme-copper oxidases (HCOs) play a critical role in the four-electron, four-proton reduction of O2 to H2O in biosystem. The HCOs exhibit high enzymatic activity due to their natural structure with heme-nonheme metal active sites, and the nonheme metal plays a role in conferring and fine-tuning O2 reduction activity of the HCOs. Inspired by this binucleus active enzyme, herein we designed an efficient electrocatalyst (Fe, Mn-N/C) for oxygen reduction reaction, which contains two types of Metal-Nx active sites incorporated within the graphene frameworks of porous carbon. The catalysts displayed remarkable ORR performance with a half-potential of 0.904V and kinetic current density of 33.33mV cm-2 that was 4.9 times as that of 20% Pt/C (6.76 mA cm-2). When Fe, Mn-N/C catalyst was applied as air electrode in Zn-air battery, it exhibited a superior performance compared to commercial Pt/C. Its discharge curve showed the change in output voltage was negligible at 20mA cm-2 for 23000 seconds (6.4 h). The first principle calculations revealed that Fe, Mn-N/C needs less energy for the protonation of O* to OH* in ORR procedure compared with Fe-N/C. This catalyst with bimetal reactive center mimicking metal enzyme will pave a new way to design efficient electrocatalysts for ORR in fuel cells.

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Publication details

The article was received on 16 May 2018, accepted on 06 Jun 2018 and first published on 08 Jun 2018


Article type: Paper
DOI: 10.1039/C8TA04564J
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Designing Highly Efficient Dual-Metal Single-Atom Electrocatalysts for Oxygen Reduction Reaction Inspired by Biological Enzyme System

    S. Gong, C. Wang, P. Jiang, L. Hu, H. Lei and Q. Chen, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA04564J

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