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Metal-free polymeric carbon nitrides (PCNs) are promising photocatalysts for solar hydrogen production, but their structure-photoactivity relationship remains elusive. Two PCNs were characterized by dynamic-nuclear-polarization-enhanced solid-state NMR spectroscopy, which circumvented the need for specific labeling with either 13 C- or 15 N-enriched precursors. Rapid 1D and 2D data acquisition was possible, providing insights into the structural contrasts between the PCNs. Compared to PCNB with lower performance, PCNP is a more porous and more active photocatalyst that is richer in terminal N-H bonds not associated with interpolymer chains. It is proposed that terminal N-H groups act as efficient carrier traps and reaction sites.
Li et al. (Tue,) studied this question.