RESUMEN
Heterogeneous catalytic ozonation (HCO) enables the destruction of organic pollutants in wastewater via oxidation by powerful hydroxyl radicals (·OH). However, the availability of short-lived ·OH in aqueous bulk is low in practical treatment scenarios due to mass transfer limitations and quenching of water constituents. Herein, we overcome these challenges by loading MgO catalysts inside the pores of a tubular ceramic membrane (denoted as CCM) to confine ·OH within the nanopores and achieve efficient pollutant removal. When the pore size of the membrane was reduced from 1000 to 50 nm, the removal of ibuprofen (IBU) by CCM was increased from 49.6 % to 90.2 % due to the enhancement of ·OH enrichment in the nanospace. In addition, the CCM exhibited high catalytic activity in the presence of co-existing ions and over a wide pH range, as well as good self-cleaning ability in treating secondary wastewater. The experimental results revealed that ·OH were the dominant reactive oxygen species (ROS) in pollutant degradation, while surface hydroxyl groups were active sites for the generation of ·OH via ozone decomposition. This work provides a promising strategy to enhance the utilization of ·OH in HCO for the efficient degradation of organic pollutants in wastewater under spatial confinement.
RESUMEN
Twisted moiré superlattice is featured with its moiré potential energy, the depth of which renders an effective approach to strengthening the exciton-exciton interaction and exciton localization toward high-performance quantum photonic devices. However, it remains as a long-standing challenge to further push the limit of moiré potential depth. Herein, owing to the pz orbital induced band edge states enabled by the unique sp-C in bilayer γ-graphdiyne (GDY), an ultradeep moiré potential of â¼289 meV is yielded. After being twisted into the hole-to-hole layer stacking configuration, the interlayer coupling is substantially intensified to augment the lattice potential of bilayer GDY up to 475%. The presence of lateral constrained moiré potential shifts the spatial distribution of electrons and holes in excitons from the regular alternating mode to their respective separated and localized mode. According to the well-established wave function distribution of electrons contained in excitons, the AA-stacked site is identified to serve for exciton localization. This work extends the materials systems available for moiré superlattice design further to serial carbon allotropes featured with benzene ring-alkyne chain coupling, unlocking tremendous potential for twistronic-based quantum device applications.
RESUMEN
π electron configuration plays a pivotal role in metal-free carbon catalysts, and its delocalization degree overwhelmingly dominates catalytic activity. However, precise and targeted regulation of inherent π electrons still remain challenging. Here, one chemical-bond-targeted physical clipping strategy is proposed and effectively adopted in the cutting-edge carbon material system of graphdiyne (GDY) as a concept-of-proof. The delocalized electrons are expected to be periodically reformatted for substantially enhancing π electron delocalization. Via theoretical screening and well-designed experiments, periodical interruption of Csp-Csp2 bonds in GDY can render sp-C sites with decent activity, ultimately yielding top-ranking electrocatalytic performance without intentionally introducing external decoration. The as-proposed concept endows a universal prescription to push the limit of delocalization degree, thus shedding novel light on the rational design of decent metal-free catalysts.
RESUMEN
Anatase TiO2 with {001} facets is much more active than that with {101} facets, which has been verified via experiments and theoretical calculations. Graphene has garnered much attention since it was initially synthesized, due to its unique properties. In this study, reduced graphene oxide (RGO)/{001} faceted TiO2 composites were fabricated via a solvothermal method. The composites were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectrophotometry, photoluminescence and Raman analysis. The results revealed that the graphene oxide was reduced during the preparation process of the {001} faceted TiO2, and combined with the surface of {001} TiO2. The photocatalytic activities of the composites were evaluated through the degradation of basic violet, under both white light (λ > 390 nm) and visible light (λ = 420 nm) irradiation. The results indicated that the photocatalytic activities of the {001} faceted TiO2 were significantly improved following the incorporation of RGO, particularly under visible light irradiation. Theoretical calculations showed that the band structure of the {001} faceted TiO2 was modified via graphene hybridization, where the separation of photoinduced electron-hole pairs was promoted; thus, the photocatalytic activity was enhanced.
RESUMEN
The establishment of p-n heterojunction between semiconductors is an effective means to improve the performance of semiconductor photocatalysts. For the first time, we synthesize SnO2/BiOBr heterojunction photocatalysts using a one-step hydrothermal method. Systematic material characterizations suggest that the photocatalysts consist of irregular BiOBr nanosheets with the length about 200 nm and width about 150 nm, and SnO2 nanoparticles are anchored uniformly onto the nanosheets. Most importantly, electrochemical characterizations including transient photocurrent profiles and electrochemical impedance spectra suggest that SnO2/BiOBr heterojunctions are created, which facilitates the charge separation and transfer efficiency of photogenerated charge carriers. As such, SnO2/BiOBr photocatalysts exhibit remarkable photocatalytic activities in terms of degrading a series of organic pollutants. Radical trapping experiments and electron spin resonance spectra suggest that superoxide radicals (â¢O2-) and hydroxyl radicals (â¢OH) are primary medium species running through the photocatalytic degradation process and enhanced photocatalytic performance.
