Formation of C-N containing compounds from plasma-catalytic coupling of CH and N over various transition metals (Ni, Pd, Cu, Ag, and Au) is investigated using a multimodal spectroscopic approach, combining polarization-modulation infrared reflection-absorption spectroscopy (PM-IRAS) and optical emission spectroscopy (OES). Through sequential experiments utilizing CH and N nonthermal plasmas, we minimize plasma-phase reactions and identify key intermediates for C-N coupling on metal surfaces. Results show that simultaneous CH and N exposure with plasma stimulation produces surface C-N species. However, N-CH sequential exposure does not lead to C-N species formation, while CH-N sequential exposure reveals the presence of CH surface species and CN radical species as key precursors to C-N species formation. From further analysis using X-ray photoelectron spectroscopy and liquid chromatography-mass spectrometry, the influence of exposure conditions on the degree of nitrogen incorporation and the nature of C-N species formed were revealed. The work highlights the importance of surface chemistry and exposure conditions in surface C-N coupling with plasma stimulation.
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