Abstract

Copper- and nitrogen-codoped reduced graphene oxide material (Cu/N-rGO) was prepared with a hydrothermal method. Its versatile catalytic performances were demonstrated toward the oxidative degradation of rhodamine B (RhB) and oxygen reduction reaction (ORR). The Cu and N codoping of graphene enhanced not only its activation ability toward H2O2, but also its electrocatalytic ability for ORR. It was observed that the use of 3%Cu/N-rGO together with 40 mmol·L−1 H2O2 and 4 mmol·L−1 Na2CO3 could remove more than 94% of the added RhB (30 mg·L−1) in 20 min through a catalytic Fenton-like degradation. Quenching experiments and electron paramagnetic resonance (EPR) measurements indicated that the main reactive species generated in the catalytic oxidation process were surface-bound •OH. The modified graphene also showed good electrocatalytic activity for ORR reaction in alkaline media through a four-electron mechanism. On the electrode of Cu/N-rGO, the ORR reaction exhibited an onset potential of −0.1 V and a half-wave potential of −0.248 V, which were correspondingly close to those on a Pt/C electrode. In comparison with a Pt/C electrode, the 3%Cu/N-rGO electrode showed much greater tolerance to methanol. Such outstanding catalytic properties are attributed to the abundant active sites and the synergism between Cu and N in Cu/N-rGO.

Highlights

  • Due to serious challenges from environmental pollution and energy shortages, various catalysts have been developed to enhance the related pollutant degradation reactions and energy conversion reactions, especially for Fenton-like reactions, and hydrogen evolution and oxygen reduction reactions [1,2,3,4,5]

  • The morphologies of 3%Cu/N-reduced graphene oxide (rGO) and 100%Cu/N-rGO were observed by transmission electron microscopy (TEM)

  • When the doping content of Cu was increased, the TEM image of 100%Cu/N-rGO in Figure 1c clearly reveals that CuO particles were dispersed on the surface of the graphene

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Summary

Introduction

Due to serious challenges from environmental pollution and energy shortages, various catalysts have been developed to enhance the related pollutant degradation reactions and energy conversion reactions, especially for Fenton-like reactions, and hydrogen evolution and oxygen reduction reactions [1,2,3,4,5]. Typical investigations are focused on the designs of heterogeneous catalysts with high catalytic activity and selectivity by using noble metals (Pt and Au) [6,7], metal oxides (Fe3 O4 and ZnO/Co3 O4 ) [8,9], and metal nitrides [10] These catalysts may have the demerits of either high cost (due to noble metals) or poor durability (due to the less noble metals), which are unfavorable to their large-scale deployment. To overcome this problem, it is interesting and important to develop carbon-based versatile catalysts that have good catalytic performances for both the Fenton-like reactions (in the field of environmental chemistry) and electrochemical oxygen reduction reaction (in the field of energy chemistry). Kannan and Kumar [13] reviewed the current status in the design and development of graphene-based oxygen reduction reaction (ORR)

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