Integrated removal of NO and mercury from coal combustion flue gas using manganese oxides supported on TiO2

A catalyst composed of manganese oxides supported on titania(MnO_x/TiO_2) synthesized by a sol–gel method was selected to remove nitric oxide and mercury jointly at a relatively low temperature in simulated flue gas from coal-fired power plants. The physico-chemical characteristics of catalysts were investigated by X-ray fluorescence(XRF), X-ray diffraction(XRD), and X-ray photoelectron spectroscopy(XPS) analyses, etc. The effects of Mn loading,reaction temperature and individual flue gas components on denitration and Hg~0 removal were examined. The results indicated that the optimal Mn/Ti molar ratio was 0.8 and the best working temperature was 240°C for NO conversion. O_2 and a proper ratio of [NH_3]/[NO]are essential for the denitration reaction. Both NO conversion and Hg~0 removal efficiency could reach more than 80% when NO and Hg~0 were removed simultaneously using Mn0.8 Tiat 240°C.Hg~0 removal efficiency slightly declined as the Mn content increased in the catalysts. The reaction temperature had no significant effect on Hg~0 removal efficiency. O_2 and HCl had a promotional effect on Hg~0 removal. SO2 and NH_3were observed to weaken Hg~0 removal because of competitive adsorption. NO first facilitated Hg~0 removal and then had an inhibiting effect as NO concentration increased without O_2, and it exhibited weak inhibition of Hg~0 removal efficiency in the presence of O_2. The oxidation of Hg~0 on Mn O x/TiO_2 follows the Mars–Maessen and Langmuir–Hinshelwood mechanisms.     

Removal of Cs from water and soil by ammonium-pillared montmorillonite/Fe3O4 composite

To remove cesium ions from water and soil, a novel adsorbent was synthesized by following a one-step co-precipitation method and using non-toxic raw materials. By combining ammonium-pillared montmorillonite (MMT) and magnetic nanoparticles (Fe₃O₄), an MMT/Fe₃O₄ composite was prepared and characterized. The adsorbent exhibited high selectivity of Cs⁺ and could be rapidly separated from the mixed solution under an external magnetic field. Above all, the adsorbent had high removal efficiency in cesium-contaminated samples (water and soil) and also showed good recycling performance, indicating that the MMT/Fe₃O₄ composite could be widely applied to the remediation of cesium-contaminated environments. It was observed that the pH, solid/liquid ratio and initial concentration affected adsorption capacity. In the presence of coexisting ions, the adsorption capacity decreased in the order of Ca^2 + > Mg^2 + > K⁺ > Na⁺, which is consistent with our theoretical prediction. The adsorption behavior of this new adsorbent could be expressed by the pseudo-second-order model and Freundlich isotherm. In addition, the adsorption mechanism of Cs⁺ was NH₄⁺ ion exchange and surface hydroxyl group coordination, with the former being more predominant.     

A nanocomposite consisting of silica-coated magnetite and phenyl-functionalized graphene oxide for extraction of polycyclic aromatic hydrocarbon from aqueous matrices

In this study,graphene oxide was covalently immobilized on silica-coated magnetite and then modified with 2-phenylethylamine to give a nanocomposite of type Fe_3O_4@SiO_2@GO-PEA that can be applied to the magnetic solid-phase extraction of polycyclic aromatic hydrocarbons(PAHs) from water samples.The resulting microspheres(Fe_3O_4@SiO_2@GO-PEA) were characterized by Fourier transform-infrared spectroscopy(FT-IR),scanning electron microscopy(SEM),CHNS elemental analysis,and vibrating sample magnetometry(VSM) techniques.The adsorbent possesses the magnetic properties of Fe_3O_4 nanoparticles that allow them easily to be separated by an external magnetic field.They also have the high specific surface area of graphene oxide which improves adsorption capacity.Desorption conditions,extraction time,amount of adsorbent,salt concentration,and pH were investigated and optimized.Following desorption,the PAHs were quantified by gas chromatography with flame ionization detection(GC-FID).The limits of detection(at an S/N ratio of 3) were achieved from 0.005 to0.1 μg/L with regression coefficients(R~2) higher than 0.9954.The relative standard deviations(RSDs) were below 5.8%(intraday) and 6.2%(inter-day),respectively.The method was successfully applied to the analysis of PAHs in environmental water samples where it showed recoveries in the range between 71.7%and 106.7%(with RSDs of 1.6%to 8.4%,for n = 3).The results indicated that the Fe_3O_4@SiO_2@GO-PEA microspheres had a great promise to extraction of PAHs from different water samples.     

Adsorption of Ca2+ on single layer graphene oxide

Graphene oxide(GO) holds great promise for a broad array of applications in many fields,but also poses serious potential risks to human health and the environment.In this study,the adsorptive properties of GO toward Ca~(2+) and Na+were investigated using batch adsorption experiments,zeta potential measurements,and spectroscopic analysis.When pH increased from 4 to 9,Ca~(2+)adsorption by GO and the zeta potential of GO increased significantly.Raman spectra suggest that Ca~(2+)was strongly adsorbed on the GO via –COO Ca~+ formation.On the other hand,Na+was adsorbed into the electrical diffuse layer as an inert counterion to increase the diffuse layer zeta potential.While the GO suspension became unstable with increasing pH from 4 to 10 in the presence of Ca~(2+),it was more stable at higher pH in the NaC l solution.The findings of this research provide insights in the adsorption of Ca~(2+)on GO and fundamental basis for prediction of its effect on the colloidal stability of GO in the environment.     

Ammonia and greenhouse gas emissions from a subtropical wheat field under different nitrogen fertilization strategies

Minimizing soil ammonia (NH₃) and nitrous oxide (N₂O) emission factors (EFs) has significant implications in regional air quality and greenhouse gas (GHG) emissions besides nitrogen (N) nutrient loss. The aim of this study was to investigate the impacts of different N fertilizer treatments of conventional urea, polymer-coated urea, ammonia sulfate, urease inhibitor (NBPT, N-(n-butyl) thiophosphoric triamide)-treated urea, and nitrification inhibitor (DCD, dicyandiamide)-treated urea on emissions of NH₃ and GHGs from subtropical wheat cultivation. A field study was established in a Cancienne silt loam soil. During growth season, NH₃ emission following N fertilization was characterized using active chamber method whereas GHG emissions of N₂O, carbon dioxide (CO₂), and methane (CH₄) were by passive chamber method. The results showed that coated urea exhibited the largest reduction (49%) in the EF of NH₃-N followed by NBPT-treated urea (39%) and DCD-treated urea (24%) over conventional urea, whereas DCD-treated urea had the greatest suppression on N₂O-N (87%) followed by coated urea (76%) and NBPT-treated urea (69%). Split fertilization of ammonium sulfate-urea significantly lowered both NH₃-N and N₂O-N EF values but split urea treatment had no impact over one-time application of urea. Both NBPT and DCD-treated urea treatments lowered CO₂-C flux but had no effect on CH₄-C flux. Overall, application of coated urea or urea with NPBT or DCD could be used as a mitigation strategy for reducing NH₃ and N₂O emissions in subtropical wheat production in Southern USA.     

Combined effects of adsorption and photocatalysis by hybrid TiO2/ZnO-calcium alginate beads for the removal of copper

The use of nanosized titanium dioxide(TiO_2) and zinc oxide(ZnO) in the suspension form during treatment makes the recovering and recycling of photocatalysts difficult.Hence,supported photocatalysts are preferred for practical water treatment applications.This study was conducted to investigate the efficiency of calcium alginate(CaAlg) beads that were immobilized with hybrid photocatalysts,TiO_2/ZnO to form TiO_2/ZnO-CaAlg.These immobilized beads,with three different mass ratios of TiO_2:ZnO(1:1,1:2,and 2:1) were used to remove Cu(Ⅱ) in aqueous solutions in the presence of ultraviolet light.These beads were subjected to three cycles of photocatalytic treatment with different initial Cu(Ⅱ) concentrations(10-80 ppm).EDX spectra have confirmed the inclusion of Ti and Zn on the surface of the CaAlg beads.Meanwhile,the surface morphology of the beads as determined using SEM,has indicated differences of before and after the photocatalytic treatment of Cu(Ⅱ).Among all three,the equivalent mass ratio TiO_2/ZnO-CaAlg beads have shown the best performance in removing Cu(Ⅱ) during all three recycling experiments.Those TiO_2/ZnO-CaAlg beads have also shown consistent removal of Cu,ranging from 7.14-52.0 ppm(first cycle) for initial concentrations of10-80 ppm.In comparison,bare CaAlg was only able to remove 6.9-48 ppm of similar initial Cu concentrations.Thus,the potential use of TiO_2/ZnO-CaAlg beads as environmentally friendly composite material can be further extended for heavy metal removal from contaminated water.     

Ag–AgBr/TiO2/RGO nanocomposite: Synthesis, characterization, photocatalytic activity and aggregation evaluation

Ag–AgBr/TiO_2 supported on reduced graphene oxide(Ag–AgBr/TiO_2/RGO) with different mass ratios of grapheme oxide(GO) to TiO_2 were synthesized via a facile solvothermal-photo reduction method. Compared to the single-, two-and three-component nanocomposites,the four-component nanocomposite, Ag–AgBr/TiO_2/RGO-1 with mass ratio of GO to TiO_2at 1%, exhibited a much higher photocatalytic activity for the degradation of penicillin G(PG)under white light-emitting diode(LED-W) irradiation. The PG degradation efficiency increased with the increase of mass ratio of GO to TiO_2 from 0.2% to 1%, then it decreased with the increase of mass ratio of GO to TiO_2 from 1% to 5%. The zeta potentials of RGO-nanocomposites became more negative with the presence of humic acid(HA) due to the negatively charged HA adsorption, resulting in the shift of points of zero charge to lower values of pH. The aggregations of nanocomposites were more significant due to the bridging effect of HA. Furthermore, the aggregated particle sizes were larger for RGO-nanocomposites compared to other nanoparticles, due to the bindings of the carboxylic and phenolic functional groups in HA with the oxygen-containing functional groups in the RGO-nanocomposites.The microfiltration(MF) membrane was effective for the nanocomposites separation. In the continuous flow through submerged membrane photoreactor(sMPR) system, backwashing operation could efficiently reduce membrane fouling and recover TiO_2, and thus indirectly facilitate the PG removal.     

基于神经网络模型绿色合成纳米氧化锰及其性能研究

近年来,基于对纳米材料生物毒性和合成成本的考虑,纳米材料的绿色合成和应用在环境领域受到了广泛关注,但迄今仍面临纳米材料的绿色合成机制尚未明确及去除效率不理想两个问题.本研究选择As（III）和As（V）作为目标污染物,通过神经网络模型对纳米氧化锰（MONPs）的合成条件进行优化,发现当污染物浓度和材料投加量分别为0.1 mg?L^-1和5 mg?L^-1时,优化后的MONPs对As（III）和As（V）的去除 效率分别从43.9%、80.0%提高到90.2%、92.2%.从SEM的结果中发现优化后的材料粒径更小,根据EDS和FTIR结果,可以证明优化后材料中的Mn元素比例显著增加.另外,XRD和XPS结果则证明优化后材料从原来的Mn（II）变为Mn（IV）,提高了材料的氧化能力.Zeta电位结果表明优化后材料表面的负电荷减少,进而循环伏安法结果证实了材料电子转移能力的提高,均有利于As的去除.最后,优化后MONPs在经过5次重复利用后仍具高的性能,同时对多种重金属具有一定的吸附能力.显然,基于神经网络模型绿色合成氧化锰纳米材料对砷污染修复具有 较强的针对性和实用性.     

铜锰基整体式催化剂对烧结烟气CO净化特性

基于改性铜锰氧化物作为CO催化活性组分,分别制备了催化剂原粉、以泡沫金属、堇青石为载体的两种整体式催化剂,在实验室配气条件下对比了3种样品的CO催化效率及稳定性,优选了堇青石整体式催化剂,并在某钢厂实际烧结烟气条件下测试了其在不同催化剂负载量、空速、温度下的CO催化效率、稳定性以及衰减后样品催化特性;最后批量制备了2m³优选整体式催化剂并开展了6000m³/h烧结烟气CO净化中试实验.结果表明,烟气高浓水蒸气显著抑制CO催化反应,经240h催化后T₉₀最大提升38℃;催化剂负载量越高,T₉₀越低,催化效率衰减时间越短,稳定后的效率越高,但随着空速增加,该优势减小;1440h(2个月)中试实验中,进气温度185~195℃下,CO催化效率大于85%(平均90%),出口CO浓度低于1000×10^-6,出口平均烟温达220℃,具有节能减排双重效益.     

The combined toxicity and mechanism of multi-walled carbon nanotubes and nano copper oxide toward freshwater algae: Tetradesmus obliquus

Nanoparticles(NPs) are widely used for their special physical properties and released into the natural environment. When two types of NPs exist in the same environment, the presence of one type of NP may affect the properties of the other type of NP. This study investigated the toxic effects of multi-walled carbon nanotubes(MWCNTs) and copper oxide nanoparticles(Cu O NPs) on Tetradesmus obliquus. Both NPs had toxic effects on algae, and the toxic effects of MWCNTs were significantly stronger tha...