期刊
CHEMISTRY OF MATERIALS
卷 27, 期 16, 页码 5775-5781出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.5b02370
关键词
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资金
- Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy
- Office of Science of the U.S. Department of Energy [DE-AC02-05-CH11231]
Nitrogen doping is an important strategy in tuning the properties and functions of carbonaceous materials. But the chemical speciation of the nitrogen groups in the sp(2)-carbon framework has not been firmly established. Here we address two important questions in nitrogen doping of carbonaceous materials from a computational approach: the relative stability of different nitrogen groups and their X-ray photoelectron spectrum (XPS) signatures of the core-level (N 1s) electron binding energies. Four types of nitrogen groups (graphitic, pyrrolic, aza-pyrrolic, and pyrichnic) in 69 model compounds have been examined. Computed formation energies indicate that pyrrolic and pyridinic nitrogens are significantly more stable (by about 110 kJ/mol) than graphitic and aza-pyrrolic nitrogens. This stability trend can be understood from the Clar's sextet rule. Predicted N is binding energies show relatively high consistency among each dopant type, thereby offering a guide to identify nitrogen groups. The relative stability coupled with predicted N is binding energies can explain the temperature-dependent change in the experimental XPS spectra. The present work therefore provides fundamental insights into nitrogen dopants in carbonaceous materials, which will be useful in understanding the applications of nitrogen-doped carbons in electric energy storage, electrocatalysis, and carbon capture.
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