Issue 27, 2018

Designing highly efficient dual-metal single-atom electrocatalysts for the oxygen reduction reaction inspired by biological enzyme systems

Abstract

Biological heme–copper oxidases (HCOs) play a critical role in the four-electron, four-proton reduction of O2 to H2O in biosystems. HCOs exhibit high enzymatic activity due to their natural structure with heme–non-heme metal active sites, and the non-heme metal plays a role in conferring and fine-tuning the O2 reduction activity of the HCOs. Inspired by this binuclear active enzyme, herein, we designed an efficient electrocatalyst (Fe, Mn–N/C) for the oxygen reduction reaction, which contains two types of metal–Nx active site incorporated within the graphene framework of porous carbon. The catalyst displayed remarkable ORR performance with a half-potential of 0.904 V and kinetic current density of 33.33 mA cm−2, which is 4.9 times that of 20% Pt/C (6.76 mA cm−2). When the Fe, Mn–N/C catalyst was applied as an air electrode in a Zn–air battery, it exhibited a superior performance compared to commercial Pt/C. Its discharge curve showed that the change in output voltage was negligible at 20 mA cm−2 for 23 000 seconds (6.4 h). First principles calculations revealed that Fe, Mn–N/C needs less energy for the protonation of O* to OH* in ORR procedures compared with Fe–N/C. This catalyst, with its bimetal reactive center mimicking a metal enzyme, will pave a new way to design efficient electrocatalysts for the ORR in fuel cells.

Graphical abstract: Designing highly efficient dual-metal single-atom electrocatalysts for the oxygen reduction reaction inspired by biological enzyme systems

Supplementary files

Article information

Article type
Paper
Submitted
16 May 2018
Accepted
06 Jun 2018
First published
08 Jun 2018

J. Mater. Chem. A, 2018,6, 13254-13262

Designing highly efficient dual-metal single-atom electrocatalysts for the oxygen reduction reaction inspired by biological enzyme systems

S. Gong, C. Wang, P. Jiang, L. Hu, H. Lei and Q. Chen, J. Mater. Chem. A, 2018, 6, 13254 DOI: 10.1039/C8TA04564J

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