Plasmonic photocatalysts were successfully synthesized by the modification of TiO2 mesocrystals with Au nanoparticles (NPs) a simple impregnation method. The NP sensitizers show strong photoelectrochemical response in visible-light region (400–800 nm) due to their surface plasmon resonance (SPR). diffuse reflectance spectroscopy measurements on wide range time scales (from picoseconds minutes) demonstrate that substantial part electrons, injected from NPs through SPR excitation,...

Titanium dioxide (TiO2) has been extensively investigated for the photocatalytic purification of air and water. In this article, we have focused on mechanisms one-electron redox reactions organic compounds during TiO2 development TiO2-based materials. It was clearly demonstrated that adsorption dynamics substrates intermediates, electronic interaction between adsorbates, band structure morphology nanomaterials are crucial factors establishing efficient reaction systems. The hybrid...

According to the concept of active sites, activity heterogeneous catalysts correlates with number available catalytic sites and binding affinity substrates. Herein, we report a single-molecule, single-particle fluorescence approach elucidate inherent photocatalytic exposed surfaces anatase TiO(2), promising photocatalyst, using redox-responsive fluorogenic dyes. A single-molecule imaging kinetic analysis from products shows that reaction for effective reduction probe molecules are...

Pt-modified Au nanorods (NRs) synthesized by anisotropic overgrowth were used for producing H2 under visible and near-infrared light irradiation. The Pt-tipped sample exhibited much higher activity compared with fully covered samples. Using single-particle spectroscopies combined transmission electron microscopy, we observed obvious quenching phenomena photoluminescence scattering from individual NRs. analysis of energy relaxation plasmon-generated hot electrons indicates the transfer excited to Pt.

Plasmonic bimetal nanostructures can be used to drive the conventional catalytic reactions efficiently at low temperature with utilization of solar energy. This work developed Pd-modified Au nanorods, which as light absorber and catalytically active site simultaneously, exhibit efficient plasmon-enhanced formic acid dehydrogenation even when below room (5 °C). Plasmon-induced interface interaction photoreaction dynamics individual nanorods were investigated by single-particle...

Singlet oxygen (1O2), molecular in the lowest excited state, has a critical role cell-killing mechanism of photodynamic therapy (PDT). Although 1O2 phosphorescence measurement been mainly used to monitor formation during PDT, its intensity is far insufficient obtain two-dimensional images intracellular with subcellular spatial resolution using currently available near-IR detector. Here, we propose new far-red fluorescence probe 1O2, namely, Si-DMA, composed silicon-containing rhodamine and...

Harnessing solar energy to produce value-added fuels and chemicals through photocatalysis techniques holds promise for establishing a sustainable environmentally friendly economy. The intricate dynamics of photogenerated charge carriers lies at the core photocatalysis. balance between trapping band-edge recombination has crucial influence on activity semiconductor photocatalysts. Consequently, regulation traps in photocatalysts becomes key optimizing their activities. Nevertheless, our...

The photocatalytic oxidation reactivities of the photogenerated holes (h+) during ultraviolet or visible laser flash photolysis pure anatase and sulfur- carbon-doped TiO2 powders were investigated using time-resolved diffuse reflectance (TDR) spectroscopy. one-electron processes substrates such as methanol 4-(methylthio)phenyl (MTPM) by h+ at surface examined. TDR spectra time traces observed for charge carriers MTPM radical cation (MTPM•+) revealed that reactions generated 355-nm increased...

Metal-organic frameworks (MOFs), which exhibit large surface area and porosity retention upon solvent removal, have attracted considerable attention due to their elegant topology potential applications in separation, gas storage, nonlinear optics, catalysis. We report herein comprehensive studies on the nature of luminescence transitions MOF-5 nanoparticles, are referred as MOF-5_n, interfacial charge transfer from photoexcited MOF-5_n various organic compounds. The time-resolved diffuse...

Iodine-doped TiO2 powders (I-TiO2) prepared via hydrothermal treatment have absorption in the region of ultraviolet (UV) and visible light, were used as a photocatalyst with irradiation UV or light. The I-TiO2 characterized by XRD, TEM, EDS, XPS, FTIR, steady-state UV−vis diffuse reflectance spectra (DRS), their photocatalytic activities investigated based on photodegradation 4-chlorophenol (4-CP) water. A higher efficiency 4-CP was observed for under UV- visible-light irradiation, when...

This study evaluates the potential application of tin porphyrin- and C60 aminofullerene-derivatized silica (SnP/silica aminoC60/silica) as 1O2 generating systems for photochemical degradation organic pollutants. Photosensitized production with SnP/silica, which was faster than aminoC60/silica, effectively oxidized a variety pharmaceuticals. Significant pharmaceuticals in presence 400-nm UV cutoff filter corroborated visible light activation both photosensitizers. Whereas efficacy...

Using the combination of fluorescence resonance energy transfer (FRET) and correlation spectroscopy (FCS) technique, we investigate mechanism dynamics pH-induced conformational change i-motif DNA in bulk phases at single-molecule level. Despite numerous studies on that is formed from cytosine (C)-rich strand slightly acidic pH, its detailed have been rarely reported. FRET technique to provide valuable information structure biomolecules such as a protein DNA, clearly show partially folded...

Abstract The generation of oxidants on illuminated photocatalysts and their participation in subsequent reactions are the main basis widely investigated photocatalytic processes for environmental remediation selective oxidation. Here, diffusion . OH from TiO 2 surface to solution bulk were directly observed using a single‐molecule detection method this molecular phenomenon could explain different macroscopic behavior anatase rutile photocatalysis. mobile is generated but not rutile....

Dye-sensitized TiO2 nanoparticles that were loaded simultaneously with Pt and Al2O3 overlayer (Al2O3/TiO2/Pt) synthesized investigated for photocatalytic activity under visible light. Introducing a thin (∼1 nm thick) on dye-sensitized markedly enhanced the light activities production of hydrogen (in presence EDTA as an electron donor) dechlorination CCl4. The Al2O3/TiO2/Pt powder was characterized by HRTEM, EDX, XPS. In agreement data, photocurrent collected via shuttles electrode immersed...

Single-molecule fluorescent probe: The formation of the highly 4-NHOH form a 3,4-dinitrophenyl-substituted boron dipyrromethane dye can be used to study interfacial electron transfer on individual TiO2 particles (see picture; B yellow, C gray, F green, H white, O red). Kinetic and image analyses resulting fluorescence bursts reveal temporal dynamics molecular interactions reactive-site distributions. Detailed facts importance specialist readers are published as "Supporting Information". Such...

Hematite (α-Fe2O3) is one of the most promising candidates as a photoanode materials for solar water splitting. Owing to difficulty in suppressing significant charge recombination, however, photoelectrochemical (PEC) conversion efficiency hematite still far below theoretical limit. Here we report thick films (∼1500 nm) constructed by highly ordered and intimately attached mesocrystals (MCs) efficient PEC oxidation. Due formation abundant interfacial oxygen vacancies yielding high carrier...

The performance of semiconductor materials in solar water splitting and other applications is strongly influenced by the structure-related dynamics charge carriers these materials. In this study, we assessed trapping, recombination, surface reactions photogenerated electrically injected charges on specific facets promising visible active photocatalyst BiVO4 using single-particle photoluminescence (PL) spectroscopy. Evaluation electric-potential-induced PL properties response to scavengers...

Metal–semiconductor nanocomposites have been widely employed for designing efficient optoelectronic devices and catalysts. The performance of such is significantly influenced by both the method preparation electronic morphological structures metals semiconductors. Here, we synthesized novel containing plate-like anatase TiO2 mesocrystal superstructures noble metal (Au, Pt) nanoparticles. These nanoparticles were preferentially photodeposited on edge mesocrystals. electron transport...

Tungsten trioxide (WO3) is being investigated as one of the most promising materials for water oxidation using solar light. Its inherent surface-related drawbacks (e.g., fast charge recombination caused by surface defect sites, formation peroxo-species, etc.) are nowadays progressively overcome different methods, such passivation and deposition co-catalysts. Among them, role still poorly understood. Herein, transparent WO3 (electrodeposited) Al2O3/WO3 (prepared atomic layer deposition, ALD)...

Materials with intricate nanostructures display fascinating properties, which have inspired extensive research on the synthesis of materials controlled structures. In this study, we investigated properties superstructures TiO2 to understand inter-relationship between structural ordering and photocatalytic performance. The nanoplate anatase mesocrystals were chosen as typical investigation objects, newly synthesized by a topotactic transformation. displayed superstructure crystallographically...

Hydrogen was successfully produced under visible light irradiation in a tin porphyrin (SnP)-sensitized TiO2 system the wide pH range (pH 3–11) although SnP hardly adsorbs on TiO2. The number of H2 SnP/TiO2 after 9 h corresponds to turnover 410. apparent photonic efficiency for evolution estimated be 35% with monochromatic radiation 550 ± 10 nm. photochemical production hydrogen is mediated through formation π-radical anion (SnP˙−) that subsequently transfers electron photogenerated SnP˙−...

Organometal halide perovskites have attracted considerable attention because of their striking electrical and optical properties that are desirable for application in solar cells optoelectronic devices; however, the structure-related dynamics photogenerated charges almost always masked by ensemble averaging conventional spectroscopic methods, making it difficult to clarify underlying mechanism. Here we investigate photoluminescence characteristics CH3NH3PbBr3 perovskite nanoparticles using...