Oxide nanomaterials are indispensable for nanotechnological innovations, because they combine an infinite variety of structural motifs and properties with manifold morphological features. Given that new oxide materials are almost reported on a daily basis, considerable synthetic and technological work remains to be done to fully exploit this ever increasing family of compounds for innovative nano-applications. This calls for reliable and scalable preparative approaches to oxide nanomaterials and their development remains a challenge for many complex nanostructured oxides. Oxide nanomaterials with special physicochemical features and unusual morphologies are still difficult to access by classic synthetic pathways. The limitless options for creating nano-oxide building blocks open up new technological perspectives with the potential to revolutionize areas ranging from data processing to biocatalysis. Oxide nanotechnology of the 21st century thus needs a strong interplay of preparative creativity, analytical skills, and new ideas for synergistic implementations.
The bismuth element synthesized by a facile chemical solution method exhibited an admirable and stable photocatalytic activity towards the removal of NO under 280 nm light irradiation due to the surface plasmon resonance mediated direct photocatalysis, and most strikingly, showed a catalytic "memory" capability following illumination.
Photocatalytic hydrogen evolution is a promising technique for the direct conversion of solar energy into chemical fuels. Colloidal quantum dots with tunable band gap and versatile surface properties remain among the most prominent targets in photocatalysis despite their frequent toxicity, which is detrimental for environmentally friendly technological implementations. In the present work, all-inorganic sulfide-capped InP and InP/ZnS quantum dots are introduced as competitive and far less toxic alternatives for photocatalytic hydrogen evolution in aqueous solution, reaching turnover numbers up to 128,000 based on quantum dots with a maximum internal quantum yield of 31%. In addition to the favorable band gap of InP quantum dots, in-depth studies show that the high efficiency also arises from successful ligand engineering with sulfide ions. Due to their small size and outstanding hole capture properties, sulfide ions effectively extract holes from quantum dots for exciton separation and decrease the physical and electrical barriers for charge transfer.
The synergy between metal alloy nanoparticles (NPs) and single atoms (SAs) should maximize the catalytic activity. However, there are no relevant reports on photocatalytic CO 2 reduction via utilizing the synergy between SAs and alloy NPs. Herein, we developed a facile photodeposition method to coload the Cu SAs and Au−Cu alloy NPs on TiO 2 for the photocatalytic synthesis of solar fuels with CO 2 and H 2 O. The optimized photocatalyst achieved record-high performance with formation rates of 3578.9 for CH 4 and 369.8 μmol g −1 h −1 for C 2 H 4 , making it significantly more realistic to implement sunlightdriven synthesis of value-added solar fuels. The combined in situ FT-IR spectra and DFT calculations revealed the molecular mechanisms of photocatalytic CO 2 reduction and C−C coupling to form C 2 H 4 . We proposed that the synergistic function of Cu SAs and Au−Cu alloy NPs could enhance the adsorption activation of CO 2 and H 2 O and lower the overall activation energy barrier (including the rate-determining step) for the CH 4 and C 2 H 4 formation. These factors all enable highly efficient and stable production of solar fuels of CH 4 and C 2 H 4 . The concept of synergistic SAs and metal alloys cocatalysts can be extended to other systems, thus contributing to the development of more effective cocatalysts.
The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5d and S 2p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO2 reduction. As a result, the product generation rate of AuSA/Cd1−xS manifests a remarkable at least 113-fold enhancement compared with pristine Cd1−xS.
Oxygen vacancies induced exciton dissociation of flexible BiOCl nanosheets for effective photocatalytic CO2 conversion via the CO2 hydrogenation pathway.
Graphitic carbon nitride (g-C3N4) is a visible light photocatalyst, limited by low activity mainly caused by rapid recombination of charge carriers. In the present work, honeycomb-like g-C3N4 was synthesized via thermal condensation of urea with addition of water at 450 °C for 1 h. Prolonging the condensation time caused the morphology of g-C3N4 to change from a porous honeycomb structure to a velvet-like nanoarchitecture. Unlike in previous studies, the photocatalytic activity of g-C3N4 decreased with increasing surface area. The honeycomb-like g-C3N4 with a relatively low surface area showed highly enhanced photocatalytic activity with an NO removal ratio of 48%. The evolution of NO2 intermediate was dramatically inhibited over the honeycomb-like g-C3N4. The short and long lifetimes of the charge carriers for honeycomb-like g-C3N4 were unprecedentedly prolonged to 22.3 and 165.4 ns, respectively. As a result, the honeycomb-like g-C3N4 was highly efficient and stable in activity and could be used repeatedly. Addition of water had the following multiple positive effects on g-C3N4: (1) formation of the honeycomb structure, (2) promotion of charge separation and migration, (3) enlargement of the band gap, (4) increase in production yield, and (5) decrease in energy cost. These advantages make the present preparation method for highly efficient g-C3N4 extremely appealing for large-scale applications. The active species produced from g-C3N4 under illumination were confirmed using DMPO-ESR spin-trapping, the reaction intermediate was monitored, and the reaction mechanism of photocatalytic NO oxidation by g-C3N4 was revealed. This work could provide an attractive alternative method for mass-production of highly active g-C3N4-based photocatalysts for environmental and energetic applications.
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