Abstract Quantifying the content of surface nitrogen and oxygen containing functional groups in amorphous nitrogen doped carbons via deconvolution of C 1s x-ray photoelectron (XPS) spectra remains difficult due to limited information in the literature. To improve the interpretation of XPS spectra of nitrogen-doped carbons, the C 1s, N 1s and O 1s core level energy shifts have been calculated for various nitrogenated carbon structures via DFT. Furthermore, we propose an expanded method to improve the self-consistency of the XPS interpretation based on a seven-peak C 1s deconvolution (3 C–C peaks, 3 C–N/-O peaks, and π-π∗ transition peaks). With the DFT calculations, spectral components arising from surface-defect carbons could be distinguished from aromatic sp2 carbon. The deconvolution method proposed provides C/(N + O) ratios in very good agreement (error less than 5%) with those obtained from total C 1s, N 1s and O 1s peaks. Our deconvolution strategy provides a simple guideline for obtaining high-quality fits to experimental data on the basis of a careful evaluation of experimental conditions and results.

中文翻译：

---

解卷积氮掺杂炭的 XPS 光谱：从第一性原理分析

摘要 由于文献中的信息有限，通过 C 1s X 射线光电子 (XPS) 光谱的解卷积来量化非晶氮掺杂碳中表面含氮和含氧官能团的含量仍然很困难。为了改进对氮掺杂碳的 XPS 光谱的解释，已经通过 DFT 计算了各种氮化碳结构的 C 1s、N 1s 和 O 1s 核心能级能量位移。此外，我们提出了一种基于七峰 C 1s 解卷积（3 个 C-C 峰、3 个 C-N/-O 峰和 π-π∗ 跃迁峰）的扩展方法来提高 XPS 解释的自洽性. 通过 DFT 计算，可以将表面缺陷碳产生的光谱成分与芳香 sp2 碳区分开来。所提出的解卷积方法提供的 C/(N + O) 比率与从总 C 1s、N 1s 和 O 1s 峰中获得的比率非常一致（误差小于 5%）。我们的去卷积策略提供了一个简单的指导方针，用于在仔细评估实验条件和结果的基础上获得高质量的实验数据拟合。