Abstract

The sluggish kinetics of Oxygen Reduction Reaction (ORR) at the cathode in proton exchange membrane fuel cells or metal-air batteries requires highly effective and stable electrocatalysts to boost the reaction. The low abundance and high price of Pt-based electrocatalysts hamper the widespread application of proton exchange membrane fuel cells and metal-air batteries. As promising alternatives, metal-free carbon materials, especially upon doping heteroatoms or creating defects demonstrated excellent ORR activity, which is as efficient as or even superior to commercial platinum on carbon. Significant progress on the development of advanced carbon materials as highly stable and durable catalysts has been achieved, but the catalytic mechanisms of these materials still remain undistinguished. In present review, we summarized the up-to-date progress in the studies of carbon materials, and emphasized on the combination of experiment and theory to clarify the underlying mechanisms of these materials. At last, we proposed the perspectives on the proper strategies of elucidating the mechanisms of carbon materials as electrocatalysts towards ORR.

Highlights

  • Advanced technique for sustainable energy storage and conversion has extensively attracted considerable attention in academia and industry, due to the accelerated depletion of fossil fuels and accompanied environmental pollution.[1]

  • During the discharging process in Proton exchange membrane fuel cells (PEMFCs) or metal-air batteries (MABs), the oxygen reduction reaction (ORR) occurs at the cathode, where O2 molecules are reduced by electrons

  • We reviewed the latest advance in the research of metal-free carbon materials as ORR electrocatalysts, especially the mechanistic understanding on the electrocatalysis

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Summary

REVIEW ARTICLE

A review of oxygen reduction mechanisms for metal-free carbon-based electrocatalysts. The sluggish kinetics of Oxygen Reduction Reaction (ORR) at the cathode in proton exchange membrane fuel cells or metal-air batteries requires highly effective and stable electrocatalysts to boost the reaction. The low abundance and high price of Pt-based electrocatalysts hamper the widespread application of proton exchange membrane fuel cells and metal-air batteries. Significant progress on the development of advanced carbon materials as highly stable and durable catalysts has been achieved, but the catalytic mechanisms of these materials still remain undistinguished. We summarized the up-to-date progress in the studies of carbon materials, and emphasized on the combination of experiment and theory to clarify the underlying mechanisms of these materials. We proposed the perspectives on the proper strategies of elucidating the mechanisms of carbon materials as electrocatalysts towards ORR.

INTRODUCTION
Reaction pathways
Theoretical descriptors
The ORR was analyzed using intermediate species associated with
Experimental indicators
ELECTROCATALYTIC MECHANISMS
Intrinsic defects
CONCLUSIONS AND PERSPECTIVES
Full Text
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