Mingxin Huo

Preparation and enhanced visible-light photocatalytic activity of graphitic carbon nitride/bismuth niobate heterojunctions

A series of graphitic carbon nitride/bismuth niobate (g-C3N4/Bi5Nb3O15) heterojunctions with g-C3N4 doping level of 10-90 wt% were prepared by a facile milling-heat treatment method. The phase and chemical structures, surface compositions, electronic and optical properties as well as morphologies of the prepared g-C3N4/Bi5Nb3O15 were well-characterized. Subsequently, the photocatalytic activity and stability of g-C3N4/Bi5Nb3O15 were evaluated by the degradation of aqueous methyl orange (MO) and 4-chlorophenol (4-CP) under the visible-light irradiation. At suitable g-C3N4 doping levels, g-C3N4/Bi5Nb3O15 exhibited enhanced visible-light photocatalytic activity compared with pure g-C3N4 or Bi5Nb3O15. This excellent photocatalytic activity was revealed in terms of the extension of visible-light response and efficient separation and transportation of the photogenerated electrons and holes due to coupling of g-C3N4 and Bi5Nb3O15. Additionally, the active species yielded in the pure g-C3N4- and g-C3N4/Bi5Nb3O15-catalyzed 4-CP photodegradation systems were investigated by the free radical and hole scavenging experiments.

Photocatalytic degradation of malathion in aqueous solution using an Au–Pd–TiO2 nanotube film

The extensive use of pesticides has promoted the agricultural production, but a series of subsequent environmental issues have drawn the concern of governments and people worldwide, such as groundwater and surface water pollutions. In order to remove these pollutants, photocatalysis has emerged as a powerful method. In this paper, the photocatalytic degradation of an organophosphorus pesticide malathion was investigated using an Au-Pd co-modified TiO(2) nanotube film (Au-Pd-TiO(2)). This film was fabricated by simultaneously photo-depositing Au and Pd precursors on a self-organized TiO(2) nanotube film. Its morphology and structures were well characterized by a scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The photocatalytic experiments revealed that the malathion elimination rate increased by 172% when the photocatalyst of the naked TiO(2) nanotube film was replaced by Au-Pd-TiO(2). Additionally, the amount of H(2)O(2) yielded on the Au-Pd-TiO(2) film in 60 min was 2.89 times that on the naked TiO(2). The enhanced photocatalytic performance could be attributed to both the effective separation of photo-generated charge carriers and the higher synthesis rate of H(2)O(2). The possible photocatalytic mechanism was discussed.

Transport of graphene oxide in saturated porous media: effect of cation composition in mixed Na-Ca electrolyte systems.

The influence of cation composition in mixed Na-Ca electrolyte systems on the transport of graphene oxide particles in saturated porous media was studied. Column experiments were conducted to elucidate the transport behavior of GO by varied molar ratios of Ca2+/Na+ but of constant ionic strength (IS). The results show that retention of GO in sand column is strongly dependent on IS in the presence of Ca2+, featuring serious deposition rates (Rd) at the higher IS of 10 mM. The maximum Rd was 48.22% at 1 mM and 98.53% at 10 mM. However, there was no obvious difference in GO retention in solutions that only contained Na+ when the IS increased from 1 to 10 mM, and the Rd was 35.17% and 38.21% respectively. The molar ratio of Ca2+/Na+ in solution was much more influential in altering the particle retention behavior at the higher IS of 10 mM, compared with little influence at 1 mM. It was supposed that compression of diffuse double layers mainly controlled GO deposition under lower IS, while charge neutrality and metal (Ca2+) bridging played a significant role at the higher IS. A numerical advection-dispersion-retention model considering the combined processes of Langmuirian dynamics blocking and depth-dependent straining was successfully developed to simulate the transport process of GO through the sand column. Derjaguin-Landau-Verwey-Overbeek (DLVO) interaction energy calculations were also performed to better understand the mechanisms of GO mobility. Coupling analysis of breakthrough experiments, DLVO theory and numerical modeling in this work provides insight into the mechanisms of GO transport in saturated porous media and is useful for reliable prediction of nanoparticle penetration through the vadose zone.

Simulated sunlight photodegradation of aqueous phthalate esters catalyzed by the polyoxotungstate/titania nanocomposite

A series of porous polyoxotungstate/titania nanocomposites (PW(12)/TiO(2)) with particle size lower than 10nm and BET surface area of ca. 200 m(2)g(-1) was prepared by sol-gel chemistry combined with solvothermal treatment. The composites were successfully applied to the degradation of aqueous phthalate esters (PAEs) including di-n-butyl phthalate (DBP), diethyl phthalate (DEP), and dimethyl phthalate (DMP) under the simulated sunlight irradiation (lambda=320-680 nm) for the first time, and the conversion of DBP, DEP, and DMP reached to 98%, 84%, and 80%, respectively, after the simulated sunlight irradiation the suspension including PAE (5 mg L(-1), 100 mL) and PW(12)/TiO(2)-19.8 (100 mg) for 90 min. In addition, nearly total mineralization of DBP and DEP was realized by further increasing light irradiation time to 12h. Based on the intermediates identified in the reaction system, the photocatalytic degradation pathway of PAEs was put forward.

Ultra low dielectric constant soluble polyhedral oligomeric silsesquioxane (POSS)–poly(aryl ether ketone) nanocomposites with excellent thermal and mechanical properties

A series of novel ultra low dielectric constant soluble organic–inorganic nanocomposites in which nanoscale octa-aminophenyl polyhedral oligomeric silsesquioxanes (octaAmino POSS-Ph8) were covalently linked onto the fluoropoly(ether ether ketone)s (PEEK-CF3-COOH) were prepared and characterized. The chemical structures of the polymer matrix and nanocomposites were confirmed by 1H NMR and FT-IR spectra. The analysis of wide-angle X-ray diffraction (WAXD) and X-ray photoelectron spectra (XPS) indicated that the POSS clusters were successfully incorporated into the polymer matrix and the homogeneous dispersion of POSS cages in the polymer matrix was evidenced by scanning electron microscopy (SEM) and energy dispersive spectrometer (EDS) (Si-mapping). Furthermore, the influence of the incorporation of POSS particles on the properties of nanocomposites is investigated. The dielectric constants of the organic–inorganic nanocomposites were drastically reduced relative to neat PEEK-CF3-COOH films and the dielectric constant could achieve as low as 1.71 (1 MHz). Besides, the thermal and mechanical properties of the nanocomposites were significantly improved by incorporation of octaAmino POSS-Ph8 moieties. Meanwhile, the nanocomposite thin films still retained the good transparency.

Effects of surfactants on graphene oxide nanoparticles transport in saturated porous media

Transport behaviors of graphene oxide nanoparticles (GONPs) in saturated porous media were examined as a function of the presence and concentration of anionic surfactant (SDBS) and non-ionic surfactant (Triton X-100) under different ionic strength (IS). The results showed that the GONPs were retained obviously in the sand columns at both IS of 50 and 200mmol/L, and they were more mobile at lower IS. The presence and concentration of surfactants could enhance the GONP transport, particularly as observed at higher IS. It was interesting to see that the GONP transport was surfactant type dependent, and SDBS was more effective to facilitate GONP transport than Triton X-100 in our experimental conditions. The advection-dispersion-retention numerical modeling followed this trend and depicted the difference quantitatively. Derjaguin-Landau-Verwey-Overbeek (DLVO) interaction calculations also were performed to interpret these effects, indicating that secondary minimum deposition was critical in this study.

A novel conversion of the groundwater treatment sludge to magnetic particles for the adsorption of methylene blue.

Iron sludge, produced from filtration and backwash of groundwater treatment plant, has long been considered as a waste for landfill. In this study, iron sludge was reused to synthesize Fe3O4 magnetic particles (MPs) by using a novel solvothermal process. Iron sludge contained abundant amounts of silicon, iron, and aluminum and did not exhibit magnetic properties. After treatment for 4h, the amorphous Fe in iron sludge was transformed into magnetite Fe3O4, which could be easily separated from aqueous solution with a magnet. The prepared particles demonstrated the intrinsic properties of soft magnetic materials and could aggregate into a size of 1 μm. MPs treated for 10h exhibited excellent magnetic properties and a saturation magnetization value of 9 emu/g. The obtained particles presented the optimal adsorption of methylene blue under mild conditions, and the maximum adsorption capacity was 99.4 mg/g, which was higher than that of granular active carbon. The simple solvothermal method can be used to prepare Fe3O4 MPs from iron sludge, and the products could be applied to treatment of dyeing wastewater.

Fabrication of carbon nitride nanotubes by a simple water-induced morphological transformation process and their efficient visible-light photocatalytic activity

Carbon nitride nanotubes (C3N4 NTs) were synthesized based on the nanosheets roll-up mechanism by a simple water-induced morphological transformation process using graphitic carbon nitride (g-C3N4) as a precursor. Water was used as the phase-transfer reagent, making the preparation process environmentally friendly. The visible-light photocatalytic activity of the as-prepared C3N4 NTs significantly increased compared to bulk g-C3N4 and g-C3N4 nanosheets toward rhodamine B degradation and hydrogen evolution from water-splitting. This result can be attributed to the high photogenerated carrier transfer efficiency, excellent mass transfer capability, sufficient active sites, and enhanced light utilization efficiency of C3N4 NTs.

Application of Porous Nickel-Coated TiO2 for the Photocatalytic Degradation of Aqueous Quinoline in an Internal Airlift Loop Reactor

P25 film, prepared by a facile dip-coating method without any binder, was further developed in a recirculating reactor for quinoline removal from synthetic wastewater. Macroporous foam Ni, which has an open three-dimensional network structure, was utilized as a substrate to make good use of UV rays. Field emission scanning electron microscopy and X-ray diffraction analysis showed that the coated/calcinated P25 films consisted of two crystal phases, and had a number of uniform microcracks on the surface. The effects of initial quinoline concentration, light intensity, reaction temperature, aeration, and initial pH were studied. Increased reaction time, light intensity, environmental temperature, and gas aeration were found to significantly improve the quinoline removal efficiency. The aeration effect of oxygen dependency on the quinoline degradation had the trend pure oxygen > air > no gas > pure nitrogen with free O2. The solution pH crucially affected quinoline photodegradation; the high electrostatic adsorption of quinoline molecules on the TiO2 surface was strongly pH dependent. 2-Pyridine-carboxaldehyde, 3-pyridinecarboxaldehyde, and 2(1H)-quinolinone were identified as the major intermediates of quinoline degradation. Based on these intermediates, a primary degradation mechanism was proposed. This reusable P25 film benefits the photodegradation of water contaminants and has potential in other various applications.

Fabrication of a micellar heteropolyacid with Lewis–Brønsted acid sites and application for the production of 5-hydroxymethylfurfural from saccharides in water

Supramolecular complexes (CnH2n+1N(CH3)3)H4PW11TiO40 (n = 4, 8, 12, 14, 16, and 18) consisting of heteropolyacids (HPAs) and amphiphilic quaternary ammonium were fabricated through self-assembly. (C16H33N(CH3)3)H4PW11TiO40 was found to exhibit both Lewis acidity and Bronsted acidity. Meanwhile its amphiphilic property resulted in self-assembly in water, which could concentrate sugar molecules around the catalytic sites. Its unique structures contributed to its high performance in the production of 5-hydroxymethylfurfural (HMF) from saccharides with HMF yields of 53.7, and 50.8% for fructose and glucose in water, 66.4, 55.9, and 40.6% for sucrose, cellobiose and cellulose in biphasic solvent, respectively. Moreover, the catalyst can be recycled and reused about six times with negligible loss in activity.