4.7 Article

Molecular engineering control defects within carbon nitride for optimized co-catalyst Pt induced photocatalytic CO2 reduction and NO2 oxidation reaction

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 47, Issue 31, Pages 14280-14293

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2022.01.219

Keywords

Carbon nitride (CN); 2,4-Dihydroxyoxazole (DHO); Dual-phase photocatalytic CO2 reduction; Photocatalytic NO2 oxidation

Funding

  1. Princess Nourah bint Abdulrahman University, Riyadh, Saudi Arabia [PNURSP2022R185]
  2. King Khalid University through Research Center for Advanced Materials Science (RCAMS) [RCAMS/KKU//006/21]
  3. Taif University, Taif, KSA [TURSP-2020/03]
  4. Ministry of higher education, Malaysia (MOHE) under PRGS grants: Universiti Teknologi MARA (UiTM) [PRGS/1/2021/STG04/UITM/02/1]

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A specific copolymerization method was used to integrate 2,4-dihydroxyoxazole monomer into the carbon nitride framework, forming the composite material xCN/DHO. This composite material exhibits a sophisticated dual-phase photocatalytic activity, capable of both reducing and oxidizing CO2 and NO2 in aqueous solutions, as well as oxidizing olefins in organic states. The lipophilicity elevation of the olefins is attributed to the presence of DHO within the CN semiconductor shell, which allows the olefin molecules to be escorted into the bulk of CN and associated with the oxidation of *OH radicals. The copolymerized CN shows the greatest reduction/oxidation potential and superior overall performance under solar irradiation.
We confirmed a specific copolymerization (molecular doping) method for the covalent integration of 2,4-dihydroxyoxazole (DHO) monomer within the framework of carbon nitride (CN). The obtained composites xCN/DHO reveal a sophisticated dual-phase photocatalytic activity, which can effectively reduce and oxidize the CO2 and NO2 sources in an aqueous solution and simultaneously performed the oxidation of olefin (C]C) in an organic state. This momentous dual state activity is concerned with the lipophilicity elevation from the convolution of oxazole (DHO) monomer within the shell of CN semiconductor. This modulation demonstrates the probability of hydrophobic olefin molecules, escorted in the bulk of CN and associated with the oxidation of hydroxyl radicals (*OH) caused by photogenerated electrons/holes. In this approach, the olefinic compound allusively consumes the photoinduced electrons/holes through elevated CN/DHO, thus stimulating the entire photocatalytic route. Recent research provides a novel strategy for the production of solar fuels upon organic synthesis via the oxidizing capacity of photoinduced holes within free semiconductors of amphiphilic metals. Likewise, the results of the NO2 photocatalytic reaction demonstrated that molecular doping drastically reduces the oxidative capacity and improves its reducing propensity. More importantly, the CO2 reduction process supervenes into an extreme aggregation of methane (CH4) as well as carbon monoxide (CO) in the presence of co-catalyst Pt respectively. The photocatalytic results demonstrate that the copolymerized CN provide the greatest reduction/oxidation potential, which is due to its chemical oxidation phase that causes superior fluctuations in whole performance under solar irradiation.(C) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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