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

Abstract

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.

Novel electrical properties and applications in kaleidoscopic graphene nanoribbons

“…Precious metal catalysts have always been an obstacle in the eld of research. [206][207][208][209][210][211][212] This kind of non-noble metal and metalfree catalyst are ideal materials. The low-cost material will be widely used.…”

Mechanism of Oxygen Reduction Reaction in Alkaline Medium on Nitrogen‐Doped Graphyne and Graphdiyne Families: A First Principles Study

“…[15] In particular, carbon-based two-dimensional structures have garnered the most interest as they are capable of delivering excellent electrical conductivity: a highly desirable trait for a fuel cell electrocatalyst. [16,17] Recent investigations have demonstrated that boron/nitrogen/phosphorous/sulphur doped graphene [18][19][20][21] /graphene composites [22,23] /defect graphene [24,25] / graphitic carbon nitride [26] etc. hold great prospects as cathode materials in electrocatalysis.…”

Synergic effects between boron and nitrogen atoms in BN-codoped C59−nBNnfullerenes (n= 1–3) for metal-free reduction of greenhouse N2O gas

“…Likewise, N-doping has also been suggested as a useful strategy for tuning the electronic structure and properties of carbon-based nanomaterials. [35][36][37][38] For example, graphene layers doped with nitrogen atoms are among the most studied systems with novel and superior catalytic activity in different chemical reactions. [39][40][41][42] In addition to large electronegativity, which causes a positive charge over the nearest carbon atoms, the presence of nitrogen atoms can bring an asymmetric spin density in carbon nanomaterials.…”