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Plasmon Assisted Highly Efficient Visible Light Catalytic CO₂ Reduction Over the Noble Metal Decorated Sr-Incorporated g-C₃N₄.

ABSTRACT: The photocatalytic performance of g-C₃N₄ for CO₂ conversion is still inadequate by several shortfalls including the instability, insufficient solar light absorption and rapid charge carrier's recombination rate. To solve these problems, herein, noble metals (Pt and Au) decorated Sr-incorporated g-C₃N₄ photocatalysts are fabricated via the simple calcination and photo-deposition methods. The Sr-incorporation remarkably reduced the g-C₃N₄ band gap from 2.7 to 2.54 eV, as evidenced by the UV-visible absorption spectra and the density functional theory results. The CO₂ conversion performance of the catalysts was evaluated under visible light irradiation. The Pt/0.15Sr-CN sample produced 48.55 and 74.54 µmol h^-1 g^-1 of CH₄ and CO, respectively. These amounts are far greater than that produced by the Au/0.15Sr-CN, 0.15Sr-CN, and CN samples. A high quantum efficiency of 2.92% is predicted for the Pt/0.15Sr-CN sample. Further, the stability of the photocatalyst is confirmed via the photocatalytic recyclable test. The improved CO₂ conversion performance of the catalyst is accredited to the promoted light absorption and remarkably enhanced charge separation via the Sr-incorporated mid gap states and the localized surface plasmon resonance effect induced by noble metal nanoparticles. This work will provide a new approach for promoting the catalytic efficiency of g-C₃N₄ for efficient solar fuel production.

SUBMITTER: Humayun M

PROVIDER: S-EPMC8521553 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The catalytic reduction of O2 to H2O is important for energy transduction in both synthetic and natural systems. Herein, we report a kinetic and thermochemical study of the oxygen reduction reaction (ORR) catalyzed by iron tetraphenylporphyrin (Fe(TPP)) in N, N'-dimethylformamide using decamethylferrocene as a soluble reductant and para-toluenesulfonic acid ( pTsOH) as the proton source. This work identifies and characterizes catalytic intermediates and their thermochemistry, providing a detailed mechanistic understanding of the system. Specifically, reduction of the ferric porphyrin, [FeIII(TPP)]+, forms the ferrous porphyrin, FeII(TPP), which binds O2 reversibly to form the ferric-superoxide porphyrin complex, FeIII(TPP)(O2•-). The temperature dependence of both the electron transfer and O2 binding equilibrium constants has been determined. Kinetic studies over a range of concentrations and temperatures show that the catalyst resting state changes during the course of each catalytic run, necessitating the use of global kinetic modeling to extract rate constants and kinetic barriers. The rate-determining step in oxygen reduction is the protonation of FeIII(TPP)(O2•-) by pTsOH, which proceeds with a substantial kinetic barrier. Computational studies indicate that this barrier for proton transfer arises from an unfavorable preassociation of the proton donor with the superoxide adduct and a transition state that requires significant desolvation of the proton donor. Together, these results are the first example of oxygen reduction by iron tetraphenylporphyrin where the pre-equilibria among ferric, ferrous, and ferric-superoxide intermediates have been quantified under catalytic conditions. This work gives a generalizable model for the mechanism of iron porphyrin-catalyzed ORR and provides an unusually complete mechanistic study of an ORR reaction. More broadly, this study also highlights the kinetic challenges for proton transfer to catalytic intermediates in organic media.

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Plasmon Assisted Highly Efficient Visible Light Catalytic CO₂ Reduction Over the Noble Metal Decorated Sr-Incorporated g-C₃N₄.

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Plasmon Assisted Highly Efficient Visible Light Catalytic CO2 Reduction Over the Noble Metal Decorated Sr-Incorporated g-C3N4.

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Plasmon Assisted Highly Efficient Visible Light Catalytic CO₂ Reduction Over the Noble Metal Decorated Sr-Incorporated g-C₃N₄.