Quantitative Analysis Method for Nitrogen Electron Energy-Loss Near-Edge Structures in Nanocarbons Based on Density Functional Theory Calculations and Linear Regression

Abstract

Nonmetallic heteroatoms found in carbon nanomaterials act as active sites and exhibit excellent catalytic performance. Owing to structural complexity and the limitations of characterization technology, the identification of active sites in nanocarbon is challenging and controversial. Electron energy-loss spectroscopy is an electron microscope technique with high spatial resolution and a powerful tool for identifying the arrangement of heteroatoms. However, structural information regarding the configuration and distribution of heteroatoms is difficult to obtain using existing analytical methods. Herein, we have developed a method for the quantitative analysis of electron energy-loss near-edge structures to identify accurately nitrogen species in nanocarbon. Based on this approach, the relative amounts of nitrogen species were obtained from linear regression with calculated spectra. The concentration distribution of nanocarbon obtained by this method was consistent with the result of X-ray photoelectron spectroscopy analysis at different depths. Therefore, this fitting method can be used for the quantitative analysis of nitrogen K-edge structures. This provides a new strategy for studying the structure–activity relationships of carbon-based materials and the further design of custom nanocarbon catalysts with high active site densities.