Journal
ACS APPLIED ENERGY MATERIALS
Volume 1, Issue 5, Pages 2358-2364Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.8b00491
Keywords
oxygen reduction reaction; polymer electrolyte fuel cell; electrocatalysts; nitrogen-doped graphene; metalloenzymes
Funding
- Program for Development of Environmental Technology using Nanotechnology from the MEXT, Japan
- Nanotechnology Platform Programs of MEXT at Hokkaido University
- JAEA
- Fusion-H program at Hokkaido University
- project Development of Advanced PEFC Utilization Technologies/Development of Fundamental Technologies for PEFC Promotion/Highly-Coupled Analysis of Phenomena in MEA and its Constituents and Evaluation of Cell Performance of NEDO, Japan
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Multinuclear metal active sites are widely used as catalytic reaction centers in metalloenzymes and generally show high catalytic activity. For example, laccases are known to catalyze the oxygen reduction reaction (ORR) to water at a multinuclear copper site with almost no energy loss. The ORR is an important reaction not only in oxygenic respiration but also in future energy generation devices such as polymer electrolyte fuel cells and metal-air batteries. For large-scale commercialization of these devices, there is a need to develop highly active ORR electrocatalysts based on nonprecious metals. Incorporation of multinuclear metal active sites in conductive materials such as carbon will allow us to develop highly active electrocatalysts like metalloenzymes. However, such methods had not been established yet. Herein, we report a copper-based ORR electrocatalyst with multinuclear copper active sites in nitrogen-doped graphene. The electrocatalyst was synthesized from the mixture of graphene oxide and a multinuclear copper complex in a short-period heating method. Electrochemical measurements revealed that the obtained electrocatalyst showed the highest electrocatalytic activity for the ORR in the Cu-based electrocatalysts in neutral aqueous solution. Physicochemical measurements including in situ X-ray absorption spectroscopy revealed the incorporation of multinuclear copper sites. Our synthetic approach will offer guidance for developing highly active electrocatalysts utilizing multinuclear metal sites not only for the ORR but also for other electrocatalytic reactions.
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