This work incorporates a variety of conjugated donor-acceptor (DA) co-monomers such as 2,6-diaminopurine (DP) into the structure of a polymeric carbon nitride (PCN) backbone using a unique nanostructure co-polymerization strategy and examines its photocatalytic activity performance in the field of photocatalytic CO2 reduction to CO and H2 under visible light irradiation. The as-synthesized samples were successfully analyzed using different characterization methods to explain their electronic and optical properties, crystal phase, microstructure, and their morphology that influenced the performance due to the interactions between the PCN and the DPco-monomer. Based on the density functional theory (DFT) calculation result, pure PCN and CNU-DP15.0 trimers (interpreted as incorporation of the co-monomer at two different positions) were extensively evaluated and exhibited remarkable structural optimization without the inclusion of any symmetry constraints (the non-modified sample derived from urea, named as CNU), and their optical and electronic properties were also manipulated to control occupation of their respective highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). Also, co-polymerization of the donor–acceptor 2,6-diamino-purine co-monomer with PCN influenced the chemical affinities, polarities, and acid–base functions of the PCN, remarkably enhancing the photocatalytic activity for the production of CO and H2 from CO2 by 15.02-fold compared than that of the parental CNU, while also improving the selectivity.
To effectively address environmental pollution, we synthesized Au-loaded ZnO nanocomposites and applied for the photocatalytic degradation of 2-chlorophenol (2-CP) under visible light irradiation. The as-prepared nanophotocatalysts delivered much improved photocatalytic degradation activities as compared to the bare ZnO nanoparticles and 32% of the pollutant was degraded with 2AuZnO in 1 hr. These improved photoactivities are attributed to the extended visible light absorption due to the surface plasmon resonance property of the loaded Au nanoparticles. Moreover, Au nanoparticles played important role in charge separation by inducting excited electrons to the conduction band of ZnO photocatalyst and surface catalysis as confirmed from photoluminescence spectra and amount of the generated hydroxyl radicals. The trapping experiments confirmed that positive holes were the major degrading species during the photocatalytic degradation of 2-CP. This work provides a feasible way to improve the photocatalysis by introducing a proper amount of noble metals over the surface of semiconductor photocatalysts.
The alarming energy crises has forced the scientific community to work for sustainable energy modules to meet energy requirements. As for this, ZnO/g-C3N4 nanocomposites with proper heterojunction were fabricated by coupling a proper amount of ZnO with 2D graphitic carbon nitride (g-C3N4) nanosheets and the obtained nanocomposites were applied for photocatalytic hydrogen generation from water under visible light illumination (λ > 420 nm). The morphologies and the hydrogen generation performance of fabricated photocatalysts were characterized in detail. Results showed that the optimized 5ZnO/g-C3N4 nanocomposite produced 70 µmol hydrogen gas in 1 h compare to 8 µmol by pure g-C3N4 under identical illumination conditions in the presence of methanol without the addition of cocatalyst. The much improved photoactivities of the nanocomposites were attributed to the enhanced charge separation through the heterojunction as confirmed from photoluminescence study, capacity of the fabricated samples for •OH radical generation and steady state surface photovoltage spectroscopic (SS-SPS) measurements. We believe that this work would help to fabricate low cost and effective visible light driven photocatalyst for energy production.
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