Latest ArticlesDue to the relatively sluggish charge carrier separation in metal sulfides, the photocatalytic activity of them is still far lower than expected. Herein, sulfur vacancies and in-plane SnS2/SnO2 heterojunction were successfully introduced into the SnS2 nanosheets through high energy ball-milling. These defective structures were studied by the electron paramagnetic resonance, Raman spectra, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscope analyses. The sulfur vacancies and in-plane heterojunctions strongly accelerate the separation of photoexcited electron-hole pairs, as confirmed by the photoluminescence emission spectra and time-resolved photoluminescence decay spectra. The introduction of sulfur vacancies and in-plane heterojunction in SnS2 nanosheets results in roughly six times higher photodegrading rate for methyl orange and four times higher photocatalytic reduction rate of Cr6+ than those of pure SnS2 nanosheets.
In this paper, a novel mesoporous silica gel evenly doped by Prussian blue nanoparticles (PBMSG) was successfully synthesized by using N, N-dimethylamide as template with a large Barrett-Emmett-Teller (BET) surface area of 505 m2/g and an average pore size of 2.9 nm. The static adsorption experiments showed that the equilibration time of PBMSG for Cs+ was about 30 min. The adsorption isotherm of PBMSG for Cs+ accorded with Langmuir model and the theoretical maximum adsorption capacity was 80.0±2.9 mg/g. When the initial concentration of Cs+ was 1.00 mg/L, the adsorption partition coefficient Kd could reach 3.5×104 mL/g After adsorption, Cs+ could be eluted by dilute hydrochloric acid (pH 2) with an efficiency of 89.8%, while no K+, Fe3+, Fe2+ was eluted. PBMSG exhibited good selectivity toward Cs+ and Rb+. In the presence of high concentration of K+, the selective adsorption of PBMSG could change the mass ratio of K+, Rb+ and Cs+ from 96.63:0.83:1.00–1.12:0.73:1.00. The separation of Cs+ and Rb+ from K+ with similar concentration (100 mg/g) was realized by column experiment. This indicated that PBMSG was suitable for rapid recovery of low concentration of rubidium and cesium from complex matrixes, such as wastewater and salt lake brine, etc.
The removal efficiency of pollutants in Fe(0) electrocoagulation (EC) has been associated closely with the speciation of generated Fe(II)/Fe(III) oxides during this process, which is very complicated and can be affected by various factors. In this work, in-situ Raman, X-ray diffraction and some other techniques have been used to study the speciation of Fe under different conditions and to establish a relationship between Fe speciation and Sb(V) removal efficiency. Results indicated that concentration of dissolved oxygen (DO) is a key factor influencing Fe(0) EC. It was found that green rusts (GRs) were formed and were then transformed into magnetite at lower DO concentration, and Sb(V) removal efficiency reached 99.9% after 30 min of EC. In contrast, γ-FeOOH was formed at high DO concentration, and the removal efficiency of Sb(V) after 30 min of EC was only 72.8%. In the presence of sulfite and phosphate with low concentrations, GRs can be stabilized and benefit the removal of Sb(V). We believe this work will provide some new insights on the mechanism of Fe(0) EC and the effective removal of other pollutants during Fe(0) EC process.
Graphene oxide (GO) membranes show great potential in molecular separation for water treatment. However, the inferior stability of GO membranes is a major bottleneck for practical applications. In this study, bio-inspired polydopamine (PDA) deposition is reported for enhancing the stability of GO membranes. Through simple and mild immersion, PDA is self-polymerized on GO membranes. The blocking of PDA chains to membrane defects improves the rejections for various molecules. Because the inherently strong adhesion and crosslinking of PDA greatly strengthen the interactions of substrates to GO layers and the binding force of GO nanosheets, the prepared PDA-GO membranes exhibit impressive long-term stability in cross-flow filtration, and maintain good nanofiltration performance at various feed pressures, tangential velocities, and even after external scratching. Moreover, because the deposited PDA layers obstruct the direct contact between GO and contaminants, the antifouling property of the PDA-GO membranes increases substantially, with recovery ratio about 98%.
An innovative method for the ultrasensitive detection of mercury by solution anode glow discharge atomic emission spectroscopy (SAGD-AES) coupled with hydride generation (HG) was first investigated. In this method, the mercury vapor generated by the HG was transmitted to the SAGD through the miniature hollow tungsten tube for excitation and detected by a miniaturized spectrograph. A thorough parametric evaluation of the HG and SAGD system was performed, including the type and concentration of carrier acid, He flow rate, concentrations of NaBH4, discharge current and discharge gap. Under optimal operating conditions, the detection limit for Hg2+ achieved 0.03 μg/L, with a relative standard deviation of 1.1% at the Hg2+ concentration of 5 μg/L. Moreover, the correlation coefficient of the calibration curve was 0.9996 in the range between 0.1 and 10 μg/L. The accuracy and practicability of HG-SAGD-AES were verified by measuring GBW09101b (human hair), GBW10029 (fish), soil and rice samples. The results showed good agreement with the certified values and values from direct mercury analyzer (DMA).
This study demonstrated interesting ultrafast activation of molecular O2 by copper oxide (CuO) particles and very rapid elimination of aqueous 2, 4-dichlorophenol (2, 4-DCP) within reaction time of 30 s. Electron paramagnetic resonance (EPR) characterization indicated that ·OH, Cu3+, 1O2 and O2·- were generated in the CuO/O2 systems, wherein O2·- would be the main reactive species responsible for 2, 4-DCP degradation. It was further found that the catalytic ability of CuO for O2 activation was highly size dependent and nano-CuO was far reactive than micro-CuO. H2 temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS) and vibrating sample magnetometer (VSM) analyses revealed that both the quantity and the reactivity of the surface reaction sites (surface Cu+ and O2) could determine the catalytic ability of CuO affecting efficient Cu+-based molecular oxygen activation. Moreover, the O2 activation ability of CuO would depend on not only the dimension, but also crystalline factors, for example, the exposed facets.
There is a growing need to eliminate antibiotic resistance genes (ARGs) in the environment and mitigate widespread antibiotic resistance. Graphitic carbon nitride (g-C3N4) was successfully synthesized via facile thermal polymerization approach and its potential for adsorption treatment of ARGs in water was examined. Batch adsorption experimental results revealed that g-C3N4 powders had robust adsorption activity for the gene ampC and ermB. Adsorption kinetics and isotherms were systematically investigated to explain the adsorption mechanism. The apparent adsorption equilibrium could be reached within 180 min. The adsorption process effectively removed ARGs (ampC and ermB) from water with 3.2 log and 4.2 log reductions, respectively. In addition, experimental data were analyzed by several models and simulated well with Langmuir isotherm and pseudo-second-order model. It indicated that adsorption process might be dominated by the chemical rate-limiting step. Moreover, the effects of temperature and pH on the removal of ARGs were conducted and the isoelectric point (IEP) was obtained. Finally, we have demonstrated that the g-C3N4 is a novel adsorbent and can be used as column packing to remove ARGs by filtration.
A magnetic mesoporous expanded perlite-based (EPd-APTES@Fe3O4) composite was designed and synthesized as a novel adsorbent for enrichment of rare earth ions in aqueous solution. Effect of various factors including the pH of solution, contact time and adsorbent dosage on the adsorption behaviors of yttrium(Ⅲ) by the EPd-APTES@Fe3O4 nano-material composites from aqueous solution was investigated. The maximum adsorption capacity of the as-prepared materials for yttrium(Ⅲ) ions was 383.2 mg/g. Among the various isotherm models, the Freundlich isotherm model could well described for the adsorption of the rare earth ions at pH 5.5 and 298.15 K. The kinetic analysis indicated that the adsorption process followed the pseudo-second order kinetics model, and the rate-determining step might be chemical adsorption. Thermodynamic parameters declared that the adsorption process was endothermic. In addition, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and the quantum chemical calculation indicated that the yttrium(Ⅲ) ions were captured on the EPd-APTES@Fe3O4 surface mainly by coordination with functional group of -NH2. More importantly, the adsorption-desorption studies indicated that the EPd-APTES@Fe3O4 nano-material composites had a high stability and good recyclability.
In recent years, oil spills caused by human activities have occurred frequently, and the resultant oil pollution has received extensive attention worldwide. In this paper, a total of 50 water samples were collected from the northeastern part of the South China Sea, and total petroleum hydrocarbons (TPHs) and n-alkane content in the samples were analyzed by gas chromatography-flame ionization detector (GC-FID) technology. The petroleum hydrocarbon characteristic indices, such as carbon predominance index (CPI) and terrigenous/aquatic ratio (TAR), were calculated to trace the source of petroleum hydrocarbons. The measured value of TPHs ranged from 121.31–603.02 μg/L. For surface waters, the TPHs in the northern coastal waters and the central waters were higher than that in the far shore. For vertical waters, the TPHs sharply decreased at first, and then increased slowly and finally reached a steady state. The n-alkanes in the water samples were concentrated in C10-C38, and they were mainly from terrestrial higher plant. The waters in the near shore, mid-layer and deep sea showed a strong reducing terrestrial characteristic, while the surface waters in the open sea showed an obvious oxidizing endogenous characteristic.
The development of photocatalysts for hydrogen evolution is a promising alternative to industrial hydrogen evolution; however, generation of high active, recyclable, inexpensive heterojunctions are still challenging. Herein, a novel strategy was developed to synthesize non-noble metal co-catalyst/solid solution heterojunctions using metal-organic frameworks (MOFs) as a precursor template. By adjusting the content of MOFs, a series of Cu1.8S/ZnxCd1-xS heterojunctions were obtained, and the Cu1.8S(3.7%)/Zn0.35Cd0.65S sample exhibits a maximum hydrogen evolution rate of 14.27 mmol h-1 g-1 with an apparent quantum yield of 3.7% at 420 nm under visible-light irradiation. Subsequently, the relationship between the heterojunction and photocatalytic activity were investigated by detailed characterizations and density functional theory (DFT) calculations, which reveal that loading Cu1.8S can efficiently extend the light absorption, meanwhile, the electrons can efficiently transfer from Zn0.35Cd0.65S to Cu1.8S, thus resulting more photogenerated electrons participating in surface reactions. This result can be valuable inspirations for the exploitation of advanced materials using rationally designed nanostructures for solar energy conversion.
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