Collection of Enviromental Materials
Electrocatalytic hydrodechlorination technology possesses great potential in the field of chlorinated organic compound treatment due to the high efficiency, environmental friendliness, etc. The amorphous Pd-P/polypyrrole(PPy)/foam Ni electrode was prepared by electrochemical deposition for electrochemical hydrodechlorination of the pentachlorophenol (PCP). Morphology and chemical structure of Pd-P on the PPy/foam Ni electrode was investigated by the Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction analysis (XRD), and X-ray photoelectron spectroscope (XPS). The result indicated that the Pd-P catalyst was evenly dispersed on the PPy/foam Ni electrode with small particles and changed from crystalline state to amorphous state. The electrocatalytic reduction of PCP certificated that the doping of P significantly increased the catalytic activity of the electrode. The degradation efficiency of PCP reached 90.8% after electrocatalytic reduction for 180 min under the condition of n(Pd)/n(P)=1 : 3, Pd loading=0.15 mg/cm 2, CH2SO4=0.20 mol/L and Vcathode=-1.2 V. In addition, the Pd-P/PPy/foam Ni electrode exhibited high electrocatalytic stability after reused for 8 times without any notable deactivation.
To clarify the effect of N sources on the photocatalytic reduction of Re (VII) in amorphous TiO2/g-C3N4 (TCN) composites, g-C3N4 were prepared via a thermal decomposition of three precursors (Urea, Thiourea and Melamine). Three kinds of TCN composite photocatalysts were then prepared by recombining with amorphous TiO2 separately. All three photocatalysts were characterized by differnent methods, and their differences in photocatalytic reduction of Re(VII) were compared in detail. The experimental results show that U-TCN using urea as the N source has more uniform appearance, the largest specific surface area (474 m2/g), and the most excellent light absorption performance, leading to its photocatalytic reduction efficiency (90%) for Re (VII) being significantly higher than T-TCN (20%) and M-TCN (15%). Transient photocurrent and electrochemical impedance (EIS) analyses prove that U-TCN exhibits the highest efficiency of photo-generated electron/holes separation. Electron paramagnetic resonance spectroscopy (EPR) analysis shows that U-TCN generates more hydroxyl radicals (?OH), so that there are stronger reducing ?CO2 radicals produced by the reaction with formic acid, which is more conducive to the reduction of Re (VII). X-ray absorption spectra are employed to analyze the valence state and coordination environment of Ti element, which demonstrates an excellent photochemical stability of U-TCN. The study not only illustrates the effects of N sources on the photocatalytic performance of TCN composites, but also provides a promising photocatalyst for reduction and removal of Tc(VII) from waste water.
Phosphorus is an important nutrient element that affects the growth of algae. The sorption of phosphorus on the sediments plays an important role in its bio-geochemical cycle, with metal oxides such as alumina being one of the important active components for the process. The sorption behavior of phosphorus on two kinds of alumina (γ-Al2O3, amorphous alumina) was studied through batch methods. Both kinetics and thermodynamics of the process were investigated, as well as the effects of temperature, salinity, and pH of the medium on the process. The sorption kinetic curves could be described by a two-compartment first order equation, and the isotherms fit Freundlich equation well. The amorphous alumina has a larger specific surface area, and its sorption ability is stronger than that of γ-Al2O3. Based on the results of surface acid-base titration, the sorption behavior is also considered to be related to the surface acidity and alkalinity of the aluminum oxides. Compared with NaNO3 medium, the sorption of phosphorus in seawater was weakened. The sorption capacity decreases with the increase of the ionic strength. pH significantly affected the sorption ability of the oxides with the maximum capacity at pH=5. Higher temperatures are favorable to the sorption progress, which is endothermic and spontaneous with entropy increasing. The difference in the thermodynamic parameters of the two alumina seemed unremarkable.
Hierarchically porous silica-aluminum is an important support material for metal-catalysts, because of its excellent properties. Herein, an efficient hydrothermal approach for the production of hierarchical aluminum- doped silica (Al-SiO2) architectures was reported by employing aluminum nitrate as an aluminium source and TEOS as silicon source. Effects of the structure-oriented agent on the structure of Al-SiO2 were investigated. Structural features of Al-SiO2 were characterized by XRD, SEM and N2-physisorption. The results showed that hierarchical Al-SiO2 with "worm-like" porous of 30-40 nm can be synthesized by using TPAOH as the structure-oriented agent and hydrothermal treatment at 80 ℃. The cobalt catalysts were prepared by the wetness impregnation method. Compared with commercial SiO2 supported cobalt catalysts, the Fischer-Tropsch synthesis performance of the catalyst Co/Al-SiO2 is significantly enhanced, i.e., CO conversion nearly doubled, CH4 selectivity reduced by 19.3wt%, C2-C4 selectivity reduced by 13.3wt%, and the selectivity of gasoline products (C5-C12) reached 53.3wt%.
To investigate the modification mechanism of mixed heterogeneous on photocatalysis, a series of Nd3+-doped BiVO4 photo-catalysts with different Nd3+ contents were synthesized through a facile hydrothermal reaction. The samples exhibit Nd3+ content-dependent phase transition from monoclinic to tetragonal phase, as demonstrated by XRD and Raman analyses. SEM images show that the phase transition is accompanied by obvious morphology variation. Less than 1at% Nd3+-doped monocline BiVO4 is composed of irregular particles, while more than 7at% Nd3+ doping results in tetragonal phase BiVO4 of sphere-like or kernel with groove surface. When Nd3+content is in the range of 1at%-7at%, the micron cuboid bars appear in the samples. More importantly, monoclinic and tetragonal phase is concomitant in the product and a heterogeneous junction with staggered band structure is formed. The Rhodamine B degradation efficiencies of all Nd3+-doped samples are higher than those of undoped samples due to the regular morphology after doping. The formed heterogeneous junction inhibits photo-generated electrons and holes recombination of Nd3+-doped BiVO4, inducing 99.4% catalytic efficiency in 4at% Nd3+-doped sample. The novel morphology and the intrinsic mechanism of photocatalysis enhancement upon Nd3+-doped BiVO4 are obtained from the synthesis strategy and the energy band structure.
The hydrothermally treated red phosphorus (HRP) was dispersed on exfoliated bentonite (EB) supporter to prepare the EB/HRP photocatalyst for improving photocatalytic performance. The as-synthesized samples were characterized by different methods. Rhodamine B was selected as the model pollutant to evaluate the photodegradation property of EB/HRP. Results showed that the photodegradation efficiency of the EB/HRP photocatalyst composite increased with increased EB mass fraction, and decreased after reaching the highest value. When the mass fraction of EB was 9%, the EB9/HRP photocatalyst composite exhibited the maximum adsorption performance and photodegradation activity. Its degradation rate constant k was 0.0641 min-1, which was two times that of HRP. In addition, after five cycles of photodegradation experiments, EB9/HRP still had high photocatalytic activity (96.8%). Therefore, the EB9/HRP catalyst composite had good photocatalytic activity and stability, which can be an efficient and stable photocatalyst for the degradation of pollutants.
Fabricating Z-scheme photocatalysts is a promising method for improving photocatalytic activity by effectively enhancing charge separation. A new Z-scheme BiVO4/GO/g-C3N4 photocatalyst was prepared by two steps of impregnation-calcination and hydrothermal method, and then characterized by different methods. In the photocatalytic process of BiVO4/GO/g-C3N4, GO nanosheet act as fast transmission channels between BiVO4 and g-C3N4 and can suppress electron-hole recombination, which significantly promotes the charge separation and improves the redox ability of the ternary heterojunction. The ternary photocatalyst has good photocatalytic degradation of Rhodamine B (RhB) as compared to the single-component or binary composite. It is capable of degrading 85% of RhB in 120 min under visible light irradiation and the hole (h+) plays a major role in the reaction. This work provides a simple preparation method for a ternary photocatalyst system in which g-C3N4 coupled with BiVO4 by GO to significantly improve photocatalytic activity.
Metal-organic frameworks (MOF) as piezoelectrical materials used in mechano-catalytic degradation of organic dye are rarely investigated. In this work, NH2-UiO-66 was synthesized by the solvothermal method and applied in mechano-catalytic degradation of Rhodamine B under ultrasonic vibration. The results show that NH2- UiO-66 behaves a high mechano-catalytic decomposition efficiency of 80% for Rhodamine B within 5 h vibration and possesses a good stability. The piezoelectrically induced electric charges on the surfaces of NH2-UiO-66 via the piezoelectric effect could induce hydroxyl radicals as strong oxidants to decompose Rhodamine B. The piezoelectrical effect of MOFs is potential in utilizing vibration energy for dye wastewater treatment.