“…The global XPS spectra (Figure S5) reveal C and N as the main elements in TCN-M, HCN-Me, and THCN-M 9 Me 1 . The high-resolution C 1s XPS spectra (Figure c) are deconvoluted into four peaks centered at binding energies (BEs) of 284.8, 286.4, 288.1, and 289.0 eV, assigned to the adventitious sp 2 hybridized C from the carbonaceous environment, CN–C in the aromatic heterocycles of the CN framework, – C–NH 2 /CN species, and C–O generated on the surface under thermal condensation in air, respectively. , In addition to these, TCN-M shows a characteristic shakeup line at a BE of 290.4 eV, corresponding to π–π* transition loss . The N 1s XPS spectra of all CN samples (Figure d) can be deconvoluted into three distinct peaks with BEs of 398.6, 399.8, and 401.0 eV, suggesting that the N species exist in the form of sp 2 -hybridized N in CN heterocycles (CN–C), tertiary nitrogen (N–(C) 3 ), and a marginal amino or cyano group (C–NH/CN), respectively .…”