Abstract

2D nitrogen-doped mesoporous carbon (NMC) is synthesized by using a mesoporous silica film as hard template, which is then investigated as a non-precious metal catalyst for the oxygen reduction reaction (ORR). The effect of the synthesis conditions on the silica template and carbon is extensively investigated. In this work, we employ dual templates—viz. graphene oxide and triblock copolymer F127—to control the textural features of a 2D silica film. The silica is then used as a template to direct the synthesis of a 2D nitrogen-doped mesoporous carbon. The resultant nitrogen-doped mesoporous carbon is characterized by transmission electron microscopy (TEM), nitrogen ad/desorption isotherms, X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV), and rotating disk electrode measurements (RDE). The electrochemical test reveals that the obtained 2D-film carbon catalyst yields a highly electrochemically active surface area and superior electrocatalytic activity for the ORR compared to the 3D-particle. The superior activity can be firstly attributed to the difference in the specific surface area of the two catalysts. More importantly, the 2D-film morphology makes more active sites accessible to the reactive species, resulting in a much higher utilization efficiency and consequently better activity. Finally, it is noted that all the carbon catalysts exhibit a higher ORR activity than a commercial Pt catalyst, and are promising for use in fuel cells.

Highlights

  • The oxygen reduction reaction (ORR) is one of the most important reactions in energy conversion devices such as fuel cells and metal-air batteries [1,2]

  • We developed a co-operative assembly method with the dual templates of graphene oxide (GO) and tri-block copolymer P123 to synthesize an ultrathin 2D semi-ordered mesoporous silica film [36]

  • When GO is added as a co-template, the resultant silica evolves from the aforementioned 3D particles to a 2D film, and considerable change occurs in both morphology and characteristic dimension

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Summary

Introduction

The oxygen reduction reaction (ORR) is one of the most important reactions in energy conversion devices such as fuel cells and metal-air batteries [1,2]. Pt has been the mostly widely used and effective catalyst for the ORR [3,4,5]; the source scarcity and high cost hinder the large-scale application of fuel cells [6,7]. Nanostructured heteroatom-doped carbon has attracted intensive attention in the past decades [14,15,16,17,18,19,20,21,22,23]. 2D nitrogen-doped carbon is an ideal candidate as an electrocatalyst for the ORR due to its unique features [24,25,26,27]. Mukerjee et al [29]

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