4.6 Article

Theoretical Study on a Nitrogen-Doped Graphene Nanoribbon with Edge Defects as the Electrocatalyst for Oxygen Reduction Reaction

期刊

ACS OMEGA
卷 5, 期 10, 页码 5142-5149

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AMER CHEMICAL SOC
DOI: 10.1021/acsomega.9b04146

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资金

  1. National Natural Science Foundation of China [51871114]
  2. Research Foundation of the Education Department of Jiangxi Province of China [GJJ180433, GJJ180477]
  3. Open Funds of the State Key Laboratory of Metastable Materials Science and Technology, Yanshan University [201906]
  4. Jiangxi University of Science and Technology Scientific Research Starting Foundation [jxxjbs17053]

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Both theory and experiment show that sp(2) carbon nanomaterials doped with N have great potential as high-efficiency catalysts for oxygen reduction reactions (ORR). At present, there are theoretical studies that believe that C-sites with positive charge or high-spin density values have higher adsorption capacity, but there are always some counter examples, such as the N-doped graphene nanoribbons with edge defects (ND-GNR) of this paper. In this study, the ORR mechanism of ND-GNR was studied by density functional theory (DFT) calculation, and then the carbon ring resonance energy was analyzed from the perspective of chemical graph theory to elucidate the cause and distribution of active sites in ND-GNR. Finally, it was found that the overpotential of the model can be adjusted by changing the width of the model or dopant atoms while still ensuring proper adsorption energy (between 0.5 and 2.0 eV). The minimum overpotential for these models is approximately 0.36 V. These findings could serve as guidelines for the construction of efficient ORR carbon nanomaterial catalysts.

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