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Modification of carbon nitride based polymeric 2D materials for tailoring their optical, electronic and chemical properties for various applications has gained significant interest. The present report demonstrates the synthesis of a novel modified carbon nitride framework with a remarkable 3:5 C:N stoichiometry (C 3 N 5 ) and an electronic bandgap of 1.76 eV, by thermal deammoniation of the melem hydrazine precursor. Characterization revealed that in the C 3 N 5 polymer, two s-heptazine units are bridged together with azo linkage, which constitutes an entirely new and different bonding fashion from g-C 3 N 4 where three heptazine units are linked together with tertiary nitrogen. Extended conjugation due to overlap of azo nitrogens and increased electron density on heptazine nucleus due to the aromatic π network of heptazine units lead to an upward shift of the valence band maximum resulting in bandgap reduction down to 1.76 eV. XRD, He-ion imaging, HR-TEM, EELS, PL, fluorescence lifetime imaging, Raman, FTIR, TGA, KPFM, XPS, NMR and EPR clearly show that the properties of C 3 N 5 are distinct from pristine carbon nitride (g-C 3 N 4 ). When used as an electron transport layer (ETL) in MAPbBr 3 based halide perovskite solar cells, C 3 N 5 outperformed g-C 3 N 4 , in particular generating an open circuit photovoltage as high as 1.3 V, while C 3 N 5 blended with MA x FA 1- x Pb(I 0.85 Br 0.15 ) 3 perovskite active layer achieved a photoconversion efficiency (PCE) up to 16.7%. C 3 N 5 was also shown to be an effective visible light sensitizer for TiO 2 photoanodes in photoelectrochemical water splitting. Because of its electron-rich character, the C 3 N 5 material displayed instantaneous adsorption of methylene blue from aqueous solution reaching complete equilibrium within 10 min, which is significantly faster than pristine g-C 3 N 4 and other carbon based materials. C 3 N 5 coupled with plasmonic silver nanocubes promotes plasmon-exciton coinduced surface catalytic reactions reaching completion at much low laser intensity (1.0 mW) than g-C 3 N 4 , which showed sluggish performance even at high laser power (10.0 mW). The relatively narrow bandgap and 2D structure of C 3 N 5 make it an interesting air-stable and temperature-resistant semiconductor for optoelectronic applications while its electron-rich character and intrasheet cavity make it an attractive supramolecular adsorbent for environmental applications.

journal of the american chemical society

C<sub>3</sub>N<sub>5</sub>: A Low Bandgap Semiconductor Containing an Azo-Linked Carbon Nitride Framework for Photocatalytic, Photovoltaic and Adsorbent Applications

C3N5: A Low Bandgap Semiconductor Containing an Azo-Linked Carbon Nitride Framework for Photocatalytic, Photovoltaic and Adsorbent Applications

C₃N₅: A Low Bandgap Semiconductor Containing an Azo-Linked Carbon Nitride Framework for Photocatalytic, Photovoltaic and Adsorbent Applications