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1.
ChemSusChem ; : e202301881, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38467567

RESUMO

Conversion of CO2 into high-value chemicals using solar energy is one of promising approaches to achieve carbon neutrality. However, the oxidation of water in the photocatalytic CO2 reduction is kinetically unfavorable due to multi-electron and proton transfer processes, along with the difficulty in generating O-O bonds. To tackle these challenges, this study investigated the coupling reaction of photocatalytic CO2 reduction and selective propane oxidation using the Pd/P25 (1 wt%) catalyst. Our findings reveal a significant improvement in CO2 reduction, nearly fivefold higher, achieved by substituting water oxidation with selective propane oxidation. This substitution not only accelerates the process of CO2 reduction but also yields valuable propylene. The relative ease of propane oxidation, compared to water, appears to increase the density of photogenerated electrons, ultimately enhancing the efficiency of CO2 reduction. We further found that hydroxyl radicals and reduced intermediate (carboxylate species) played important roles in the photocatalytic reaction. These findings not only propose a potential approach for the efficient utilization of CO2 through the coupling of selective propane oxidation into propylene, but also provide insights into the mechanistic understanding of the coupling reaction.

2.
Nanoscale ; 16(3): 1147-1155, 2024 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-38186376

RESUMO

The regulation of hollow morphology, band structure modulation of solid solution, and introduction of cocatalysts greatly promote the separation of electron-hole pairs in photocatalytic processes, which is of great significance for the process of photocatalytic hydrogen evolution (PHE). In this study, we constructed Zn1-xCdxS hollow solid solution photocatalysts using template and ion exchange methods, and successfully loaded PdS quantum dots (PdS QDs) onto the solid solution through in situ sulfidation. Significantly, the 0.5 wt% PdS QDs/Zn0.6Cd0.4S composite material achieved a H2 production rate of 27.63 mmol g-1 h-1 in the PHE process. The hollow structure of the composite material enhances processes such as light reflection and scattering, the band structure modulation of the solid solution enables the electron-hole pairs to reach an optimal exciton recombination balance, and the modification of PdS QDs provides abundant sites for oxidation, thereby promoting the proton reduction and hydrogen evolution rate. This work provides valuable guidance for the rational design of efficient composite PHE catalysts with strong internal electric field.

3.
Chemosphere ; 313: 137351, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36574576

RESUMO

Photocatalysis has been vastly employed as a feasible and efficient strategy for the removal of environmental pollutants. In this study, a well-designed core-shell heterojunction of WO3 decorated with ZnIn2S4 nanosheets were fabricated under mild in-situ conditions, and fabricated processes were systematically investigated with different fabrication durations. The coupling of WO3 and ZnIn2S4 (ZIS) resulted in a Z-scheme mechanism for charge carrier transfer, holding the respective redox capacity. The as-prepared 1D/2D WO3@ZIS heterostructure displayed the highest removal efficiency within 30 min for 25 mg L-1 Cr(VI), 89.3 and 29.7 times higher than pure WO3 and ZnIn2S4. 1D/2D WO3@ZIS remained excellently stable after 5 cycling experiments. Moreover, 40 mg L-1 RhB could be degraded within 50 min. The broad and short photogenerated electron transportation path is guaranteed by the 1D/2D and Z-scheme charge separation mechanism. It efficiently prevented photo-generated charge carriers from recombination, resulting in a longer carrier lifespan and better photocurrent responses than that of pure ones. This photocatalytic system showed promising results and also provides a framework for an efficient system for photocatalysis with potential for environmental application.

4.
J Org Chem ; 85(15): 10222-10231, 2020 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-32633122

RESUMO

An efficient copper-catalyzed electrophilic amination strategy has been established for the rapid synthesis of N-aryl-2-aminophenones from readily available arylboronic acids/esters and anthranils. This protocol features good functional group tolerance, broad substrate scope, and operational simplicity. Moreover, a tandem C-H borylation and C-N coupling protocol has also been developed to transform simple arenes to the valuable N-aryl-2-aminophenones in one pot. Additionally, the synthetic potential of this methodology is further demonstrated by the synthesis of various useful N-heterocycles and derivatives.

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