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Designing an effective photocatalyst for solar-to-chemical fuel conversion presents significant challenges. Herein, g-C3 N4 nanotubes/CuCo2 O4 (CN-NT-CCO) composites decorated with platinum nanoparticles (Pt NPs) were successfully synthesized by chemical and photochemical reductions. The size distribution and location of Pt NPs on the surface of CN-NT-CCO composites were directly observed by TEM. Extended X-ray absorption fine structure (EXAFS) spectra of Pt L3-edge for the above composite confirmed establishment of Pt-N bonds at an atomic distance of 2.09â Å in the photoreduced Pt-bearing composite, which was shorter than in chemically reduced Pt-bearing composites. This proved the stronger interaction of photoreduced Pt NPs with the CN-NT-CCO composite than chemical reduced one. The H2 evolution performance of the photoreduced (PR) Pt@CN-NT-CCO (2079â µmol h-1 g-1 ) was greater than that of the chemically reduced (CR) Pt@CN-NT-CCO composite (1481â µmol h-1 g-1 ). The abundance of catalytically active sites and transfer of electrons from CN-NT to the Pt NPs to participate in the hydrogen evolution are the primary reasons for the improved performance. Furthermore, electrochemical investigations and band edge locations validated the presence of a Z-scheme heterojunction at the Pt@CN-NT-CCO interface. This work offers unique perspectives on the structure and interface design at the atomic level to fabricate high-performance heterojunction photocatalysts.
RESUMO
In this article, we present a sapiential method for producing highly effective oxygen-containing CN with hierarchical porous hollow nanotubes (HTCN) using thermal polycondensation of oxalic acid-assisted supramolecular aggregates. As a result of the synergistic effect of spatial charge separation and optical absorption ability, HTCN outperforms pristine CN nanosheets (NSCN) in photocatalytic hydrogen production. This research will provide a novel cognitive perspective and understanding for constructing contemporary hydrogen production photocatalysts.
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A novel one-pot surfactant-free synthesis is presented for designing bimetallic oxide-nitride electrocatalysts with tunable morphologies using metal salts and nitrogen-rich precursors. This innovative approach eliminates the need for a distinct nitridation process. Bifunctional electrode Co3O4/MoO3/MoxNy achieved a current density of 10 mA cm-2 while maintaining a cell voltage of 1.52 V, outperforming many bimetallic oxide-nitride catalysts in the scientific literature.
RESUMO
In this study, a solution-based synthesis technique was utilized to produce Cu2O nanoparticles (NPs) on TiO2 nanofibers (TNF), which were then subsequently coated with reduced graphene oxide (rGO) nanosheets. In the absence of any cocatalyst, CTNF@rGO-3% composite displayed an ideal photocatalytic H2 evolution rate of 96 µmol g-1 h-1 under visible light irradiation, this was 10 times higher than that of pure TNF. At 420 nm, the apparent quantum efficiency of this composite reached a maximum of 7.18%. Kelvin probe force microscopy demonstrated the formation of an interfacial electric field that was oriented from CTNF to rGO and served as the driving force for interfacial electron transfer. The successful establishment of an intimate interface between CTNF@rGO facilitated the efficient transfer of charges and suppressed the rate of recombination of photogenerated electron-hole pairs, leading to a substantial enhancement in photocatalytic performance. X-ray photoelectron spectroscopy, photoluminescence spectra, and electrochemical characterization provide further confirmation that formation of a heterojunction between CTNF@rGO leads to an extension in the lifetimes of the photogenerated charge carriers. The experimental evidence suggests that a p-n heterojunction is the mechanism responsible for the significant photocatalytic activity observed in the CTNF@rGO composite during H2 evolution.
RESUMO
Metal sulfides are emerging as an important class of materials for photocatalytic applications, because of their high photo responsive nature in the wide visible light range. In this class of materials, CdS with a direct band gap of 2.4 eV, has gained special attention due to the relative position of its conduction band minimum, which is very close to the energies of the reduced protons. However, the photogenerated holes in the valence band of CdS are prone to oxidation and destroy its structure during photocatalysis. Thus constructing a CdS based heterostructure would be an effective strategy for improving the photocatalytic performance. In this work we have done a detail theoretical investigation based on hybrid density functional theory calculation to get insight into the energy band structure, mobility and charge transfer across the CdS/CdSe heterojunction. The results indicate that CdS/CdSe forms type-II heterostructure that has several advantages in improving the photocatalytic efficiency under visible light irradiation.
RESUMO
The electrochemical reduction of CO2 (CO2RR) to produce valuable synthetic fuel like CH3OH not only mitigates the accumulated greenhouse gas from the environment but is also a promising direction toward attenuating our continuous reliance on fossil fuels. However, CO2RR to yield CH3OH suffers because of large overpotential, competitive H2 evolution reaction (HER), and poor product selectivity. In this regard, intermetallic alloy catalysts open up a wide possibility of fine-tuning the electronic property and attain appropriate structures that facilitate selective CO2RR. Here, we report for the first time the CO2RR over carbon-supported PtZn nano-alloys and probed the crucial role of structures and interfaces as active sites. PtZn/C, Pt3Zn/C, and PtxZn/C (1 < x < 3) synthesized from the metal-organic framework material were characterized structurally and morphologically. The catalysts demonstrated structure dependency toward CH3OH selectivity, as the mixed-phase PtxZn/C outperformed the phase-pure PtZn/C and Pt3Zn/C. The structure-dependent reaction mechanism and the kinetics were elucidated over the synthesized catalysts with the help of detail experiments and associated density functional theory calculations. Results showed that in spite of low electrochemically active surface area, PtxZn could not only have facilitated the single electron transfer to adsorbed CO2 but also showed better binding of the intermediate CO2â¢- over its surface. Moreover, the lower bond energy between the mixed-phase surface and -OCH3 compared to the phase-pure catalysts has enabled higher CH3OH selectivity over PtxZn. This work opens a wide possibility of studying the role of interfaces between phase-pure nano-alloys toward CO2RR.