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Evaluation of 3D gold nanodendrite layers obtained by templated galvanic displacement reactions for SERS sensing and heterogeneous catalysis
摘要： Dense layers of overlapping three-dimensional (3D) gold nanodendrites characterized by high specific surfaces as well as by abundance of sharp edges and vertices creating high densities of SERS hotspots are promising substrates for SERS-based sensing and catalysis. We have evaluated to what extent structural features of 3D gold nanodendrite layers can be optimized by the initiation of 3D gold nanodendrite growth at gold particles rationally positioned on silicon wafers. For this purpose, galvanic displacement reactions yielding 3D gold nanodendrites were guided by hexagonal arrays of parent gold particles with a lattice constant of 1.5 μm obtained by solid-state dewetting of gold on topographically patterned silicon wafers. Initiation of the growth of dendritic features at the edges of the gold particles resulted in the formation of 3D gold nanodendrites while limitation of dendritic growth to the substrate plane was prevented. The regular arrangement of the parent gold particles supported the formation of dense layers of overlapping 3D gold nanodendrites that were sufficiently homogeneous within the resolution limits of Raman microscopy. Consequently, SERS mapping experiments revealed a reasonable degree of uniformity. The proposed preparation algorithm comprises only bottom-up process steps that can be carried out without the use of costly instrumentation.
关键词： heterogeneous catalysis,galvanic displacement reactions,3D gold nanodendrites,SERS sensing,solid-state dewetting
更新于2025-11-19 16:56:35
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Cu3MS4 (M=V, Nb, and Ta) and their solid solutions with sulvanite structure for photocatalytic and photoelectrochemical H2 evolution under visible light irradiation
摘要： Solid solutions with a sulvanite structure between Cu3VS4 and either Cu3NbS4 or Cu3TaS4 (Cu3Nb1-xVxS4, Cu3Ta1-xVxS4) were successfully prepared by a solid-state reaction. Their band gaps were 1.6–1.7 eV corresponding to the absorption of a wide range of visible light. Ru-cocatalyst loaded Cu3MS4 (M=V, Nb, Ta), Cu3Nb1-xVxS4, and Cu3Ta1-xVxS4 showed photocatalytic activities for sacrificial H2 evolution under visible light irradiation. Most solid solutions showed better activities than the single Cu3MS4 (M=V, Nb, Ta). Cu3MS4 (M=V, Nb), Cu3Nb1-xVxS4, and Cu3Ta1-xVxS4 also functioned as a photoelectrode and gave cathodic photocurrents under visible light irradiation, indicating a p-type semiconductor character. Cu3Nb0.9V0.1S4 showed the best photocatalytic and photoelectrochemical performances. When Ru-loaded Cu3Nb0.9V0.1S4 was used as a photocathode with a CoOx-loaded BiVO4 photoanode, photoelectrochemical water splitting proceeded under simulated sunlight irradiation without an external bias.
关键词： Energy conversion,Water splitting,Heterogeneous catalysis,Photocatalysis
更新于2025-11-19 16:51:07
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Covalent organic framework as an efficient, metal-free, heterogeneous photocatalyst for organic transformations under visible light
摘要： Visible-light active, heterogeneous, and organic photocatalysts exhibit a more sustainable and environmentally friendly alternative to classical metal-based catalysts. Two-dimensional covalent organic frameworks (2D-COFs) with permanent porosity, columnar π-arrays and excellent stability, that can become an excellent platform for heterogeneous photocatalysis of organic transformations. Here we report a predesigned imine-based COF with electron donor and acceptor structure. And new framework possesses large surface area, high crystallinity, outstanding stability and broad absorption range in the visible-light region as well as good photoelectric response characteristics. Importantly, it was found to be a highly effective heterogeneous photocatalyst for reductive dehalogenation of phenacyl bromide derivatives and α-alkylation of aldehydes under irradiation of visible-light. In addition, the COF gave good recyclability and could be reused after a simple separation manipulation. The current present still reveals a great prospect for 2D-COFs as metal-free, heterogeneous photocatalysts for organic transformations.
关键词： visible light,photocatalysis,heterogeneous catalysis,metal-free,covalent organic frameworks
更新于2025-09-23 15:23:52
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Fabrication of electrochemically nonporous NiO–ZnO/TiO2 nanotubes/Ti plates for photocatalytic disinfection of microbiological pollutants
摘要： Nonporous NiO–ZnO/TiO2 nanotubes/Ti photocatalyst plates were fabricated via facile electrochemical method. The structural and morphological properties of the modified plates were investigated by scanning electron microscopy and X-ray diffraction, while their photoelectrochemical (PEC) characterizations were evaluated by transient photocurrent responses and electrochemical impedance spectroscopy. Antimicrobial activities of the fabricated plates against Escherichia coli bacteria and Candida albicans fungi were studied under UV light irradiation. The results indicated that the photocatalytic and PEC activities of the NiO–ZnO/TiO2 nanotubes/Ti plates are much higher than those of TiO2 nanotubes/Ti, ZnO/TiO2 nanotubes/Ti and NiO/TiO2 nanotubes/Ti. The synergetic effect among NiO, ZnO and TiO2 nanotubes motivated a fast charge separation as well as a slow electron/hole recombination, thus increasing the photocatalytic performance of the nonporous NiO–ZnO/TiO2 nanotubes/Ti photocatalyst plate.
关键词： Microbiological pollutants,Heterogeneous catalysis,Photocatalytic disinfection,NiO–ZnO hybrids
更新于2025-09-23 15:23:52
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Bulk Photodriven CO <sub/>2</sub> Conversion through TiO <sub/>2</sub> @Si(HIPE) Monolithic Macrocellular Foams
摘要： Operating photo-induced reactions exclusively on catalyst surfaces while not exploiting the full catalyst volume generates a major footprint penalty for the photocatalytic reactor and leads to an inefficient use of the catalytic material. Photonic investigations clearly show that the solid foams have a strongly multi-diffusive character, with photons being significantly trapped within the sample cores while addressing a photon mean free path lt = 20.1 ± 1.3 μm. This 3D process both greatly limits back-reactions and promotes outstanding selectivity toward methane (around 80%) generation, and even ethane (around 18%) through C-C coupling reaction, with residual carbon monoxide and dihydrogen contents (around 2%). Silica–titania TiO2@Si(HIPE) self-standing macrocellular catalysts lead to optimal efficient thicknesses up to 20 times those of powders, thereby enhancing the way for real 3D-photodriven catalytic processes above the millimeter scale and up to a 6 mm thickness. A rather simple Langmuir–Hinshelwood based kinetic model is proposed which highlights the strong dependence of photocatalytic reaction rates on light scattering and the crucial role on oxidation back-reactions. In addition, a strong correlation between light attenuation coefficient and photon mean free path and median pore aperture diameter is demonstrated, offering thus a tool for photocatalytic behavior prediction.
关键词： heterogeneous catalysis,CO2 photoreduction,sol–gel process,porous materials,integrative chemistry
更新于2025-09-23 15:22:29
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Controlled synthesis of AgNPs@ZIF-8 composite: Efficient heterogeneous photocatalyst for degradation of methylene blue and congo red
摘要： Photocatalytic degradation of organic dyes using novel metal based composite materials is one of the most intriguing and sustainable ways to reduce water pollution. Herein, facile synthesis of AgNPs@ZIF-8 via in situ generation of AgNPs and ZIF-8 (Zeolitic Imidazolate Framework) was demonstrated, and composites with different Ag contents (abbreviated as SZ, SZ1, SZ2 SZ3) were well characterized by powder X-ray diffraction (PXRD) pattern, X-ray photoelectron spectroscopy (XPS) and Fourier transform infra-red (FT-IR) spectroscopy. Encapsulation/decoration of AgNPs (particle size: 96 nm in SZ and 17.32 ± 2.35 nm in SZ1 to SZ3) in ZIF-8 matrix has been ensured by TEM and EDX analysis. Brunauer-Emmett-Teller (BET) adsorption-desorption studies indicate that the surface area of SZ (982 m2 g?1) is less than those of SZ1 to SZ3 (due to the encapsulation of large amount of Ag nanoparticles in SZ). The synthesized composites are thermally stable up to 400 °C in air and nitrogen atmosphere. AgNPs@ZIF-8 exhibited excellent photocatalytic efficiency to degrade organic dyes compared to ZIF-8 due to its large surface area, highly porous and unique synergistic properties. SZ2 degrades off 97.25 % methylene blue (MB) and 100 % congo red (CR) at pH ≥ 7. Further, degraded fragments were analysed by GC–MS and plausible degradation mechanism was discussed.
关键词： Silver nanoparticles,Organic pollutants,Photocatalyst,Heterogeneous catalysis,Composite materials
更新于2025-09-23 15:21:01
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Extending Surface‐Enhanced Raman Spectroscopy to Liquids using Shell‐Isolated Plasmonic Superstructures
摘要： Plasmonic superstructures (PS) based on Au/SiO2 were prepared for Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy (SHINERS) in liquid phase applications. These superstructures are composed of functionalized SiO2 spheres with plasmonic Au nanoparticles (NPs) on their surface. Functionalization was performed with (3-aminopropyl)-trimethoxysilane, and poly(ethylene-imine) (PEI). Of these three, PEI-functionalized spheres showed the highest adsorption density of Au NPs in TEM, UV/Vis and dynamic light scattering (DLS) experiments. Upon decreasing the Au NP/SiO2 sphere size ratio, an increase in adsorption density was also observed. To optimize plasmonic activity, 61 nm Au NPs were adsorbed onto 900 nm SiO2-PEI spheres and these PS were coated with an ultrathin layer (1–2 nm) of SiO2 to obtain Shell-Isolated Plasmonic Superstructures (SHIPS), preventing direct contact between Au NPs and the liquid medium. Zeta potential measurements, TEM and SHINERS showed that SiO2 coating was successful. The detection limit for SHINERS using SHIPS and a 638 nm laser was around 10?12 m of Rhodamine (10?15 m for uncoated PS), all with acquisition settings suitable for catalysis applications.
关键词： Raman spectroscopy,plasmonic nanoparticles,reaction monitoring,heterogeneous catalysis,SERS
更新于2025-09-19 17:13:59
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TEM Sample Preparation of Patterned Quantum Dots
摘要： Electrochemistry and heterogeneous catalysis continue to attract enormous interest. In situ surface analysis is a dynamic research field capable of elucidating the catalytic mechanisms of reaction processes. Shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) is a non-destructive technique that has been cumulatively used to probe and analyze catalytic-reaction processes, providing important spectral evidence about reaction intermediates produced on catalyst surfaces. In this perspective, we review recent electrochemical- and heterogeneous-catalysis studies using SHINERS, highlight its advantages, summarize the flaws and prospects for improving the SHINERS technique, and give insight into its future research directions.
关键词： Catalytic mechanisms,In situ surface analysis,SHINERS,Heterogeneous catalysis,Reaction intermediates,Electrochemistry,Shell-isolated nanoparticle-enhanced Raman spectroscopy
更新于2025-09-11 14:15:04
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Metal-free Semiconductor Photocatalysis for sp2 C-H Functionalization with Molecular Oxygen
摘要： Designing metal-free catalysts for solar energy conversion is a long-standing challenge in semiconductor photoredox catalysis (SPC). With visible-light-responsive hexagonal boron carbon nitride (h-BCN) as a non-metal photocatalyst, this system affords C–H/N–H coupling products with broad substitution tolerance and high efficiency with molecular oxygen as the terminal oxidant. The catalyst exhibits remarkable performance for the selective C-H functionalization of electron-rich arenes to C-N products (yields up to 95%) and good stability (6 recycles). Both nitrogen heteroarenes and amine salts are competent coupling nucleophiles. Mechanically, the reactive oxygen species are superoxide anion radical (O2??) and H2O2, which are proved by electron spin resonance (ESR) data, KI-starch, and control experiments. In addition, kinetic isotope effect (KIE) experiments indicate that C–H bond cleavage is not involved in the rate limiting step. This semiconductor-based photoredox system allows for C–H amination free of any metals, ligands, strong oxidants, and additives. It provides a complementary avenue to C–H functionalizations and enables synthetic applications efficiently in a sustainable manner.
关键词： Radical,Semiconductor Photoredox Catalysis,Heterogeneous Catalysis,Visible Light,C-H Fuctionalizaition
更新于2025-09-10 09:29:36
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Benzyl Alcohol Oxidation Using Gold Catalysts Derived from Au8 Clusters on TiO2
摘要： Atomically-precise gold clusters have gained attraction in catalysis due to high fraction of low-coordinated gold atoms, unique structural geometry and ligand effect. Phosphine-ligated gold clusters offer an advantage in the light of the labile gold-phosphorous bond for easy ligand removal. Here, heterogeneous gold catalysts were prepared by depositing atomically-precise phosphine-ligated gold clusters, Au8(PPh3)8(NO3)2 onto anatase-phase TiO2 nanoparticles. The catalysts were then calcined under two different conditions: O2 (Au8/TiO2:O2) and O2 followed by H2 (Au8/TiO2:O2–H2) at 200 °C, to dislodge phosphine ligands from the Au core. It was found that Au8/TiO2:O2–H2 catalyst showed a decent catalytic activity in benzyl alcohol oxidation while Au8/TiO2 and Au8/TiO2:O2 were completely inactive. Such results imply that small-size gold clusters (2–3 nm) alone do not always contribute to high catalytic activity of gold catalysts. It is suggested that the presence of NO3 species defines the catalytic activity of supported gold clusters in benzyl alcohol oxidation in the case of these catalysts and reinforces our initial claim in the previous work.
关键词： Heterogeneous catalysis,Oxidation,Alcohols,Green chemistry
更新于2025-09-10 09:29:36