Abstract
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.
Highlights
The excessive use of fossil fuels and the increasing concentrations of the resulting pollutants exert a negative impact on human life, the environment and energy resources in the form of global warming.Intensive endeavors are ongoing to meet the challenges of increasing future demand for fuels and the problems caused by their utilization and need for conservation due to excess pressure on the world energy infrastructure [1,2,3]
The solar energy coming from the sun has enormous potential and is considered a possibly optimal solution to the problem of fossil fuel depletion, but solar energy cannot be used directly, and it must be combined with a carbon-neutral energy source which is a challenge as the system will be solar energy driven, which is an intermittent process
Achieve astudies better visualization of their electronic structures. Along this time-dependent density functional theory (DFT) (TD-DFT) studies were conducted for the geometrical calculation of excited
Summary
The excessive use of fossil fuels and the increasing concentrations of the resulting pollutants exert a negative impact on human life, the environment and energy resources in the form of global warming. Many scientists have explored a variety of fundamental approaches to modifying PCN networks, e.g., heterojunctions [20], noble metal deposition [21], doping [22,23], and morphological control [24,25], that have significantly improved its photocatalytic activity Inspired by these developments, co-polymerization has come forth as a new prominent technique to accomplish this by using new energized organic conjugated co-monomers embedded within the framework of PCN to enhance its photocatalytic properties. Co-polymerization has come forth as a new prominent technique to accomplish this by using new energized organic conjugated co-monomers embedded within the framework of PCN to enhance its photocatalytic properties The introduction of these organic motifs within the PCN structure via the process of co-polymerization optimizes the easy accumulation of the photogenerated electrons and accelerates their transport, fueling improved photocatalytic activity under visible light irradiation, as compared to the original PCN [26]. Possible reaction path for the integration of 2,6-diaminopurine into PCN networks
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