Materials dictate carbon neutral industrial chemical processes. Visible-light photoelectrocatalysts from abundant resources will play a key role in exploiting solar irradiation. Anionic doping via pre-organization of precursors and further co-polymerization creates tuneable semiconductors. Triazole derivative-purpald, an unexplored precursor with sulfur (S) container, combined in different initial ratios with melamine during one solid-state polycondensation with two thermal steps yields hybrid S-doped carbon nitrides (C3 N4 ). The series of S-doped/C3 N4 -based materials show enhanced optical, electronic, structural, textural, and morphological properties and exhibit higher performance in organic benzylamine photooxidation, oxygen evolution, and similar energy storage (capacitor brief investigation). 50M-50P exhibits the highest photooxidation conversion (84 ± 3%) of benzylamine to imine at 535 nm - green light for 48 h, due to a discrete shoulder (≈700) nm, high sulfur content, preservation of crystal size, new intraband energy states, structural defects by layer distortion, and 10-16 nm pores with arbitrary depth. This work innovates by studying the concomitant relationships between: 1) the precursor decomposition while C3 N4 is formed, 2) the insertion of S impurities, 3) the S-doped C3 N4 property-activity relationships, and 4) combinatorial surface, bulk, structural, optical, and electronic characterization analysis. This work contributes to the development of disordered long-visible-light photocatalysts for solar energy conversion and storage.
Keywords: benzylamine photooxidation; disordered carbon nitride; photoelectrocatalysts; purpald; sulfur doping.
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