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1.
以镁铁尖晶石MgFe2O4为磁核,在磁核表层包覆MgAl水滑石后经高温焙烧形成MgAl (O)复合氧化物包覆的磁性载体MgFe2O4/MgAl (O),进而负载纳米金属Pd制成磁性催化剂Pd-MgFe2O4/MgAl (O).通过X射线衍射(XRD)、X射线光电子能谱分析(XPS)、傅里叶红外光谱(FT-IR)、透射电镜(TEM)、扫描电子显微镜(SEM)、选区电子衍射(SAED)、比表面积(SBET)和振动样品磁强计(VSM)等手段对催化材料进行表征.结果表明,MgFe2O4-LDH转化为磁性MgFe2O4/MgAl (O)载体有利于催化材料比表面积的增加、结构稳定性的提升及相应催化活性位点的增加,进而有利于提升4-氯苯酚高效加氢脱氯效率.研究进一步考察了催化剂负载量、催化剂用量、底物浓度、反应温度、反应溶剂等条件对4-氯苯酚降解效率的影响.结果发现,在优化反应条件下催化反应的转换频率TOF (0.04 s-1)可媲美常温、常压、无碱性添加剂等温和条件下4-氯苯酚高效加氢脱氯反应的最佳文献报道水平.磁性催化剂Pd-MgFe2O4/MgAl (O)循环使用4次后仍保持很好的催化活性.  相似文献   

2.
磁性纳米复合物非均相类Fenton反应催化降解罗丹明B   总被引:3,自引:2,他引:1  
以锰锌铁氧体Mn0.6Zn0.4Fe2O4(Fe-MNPs)为磁核,利用正硅酸乙酯(TEOS)水解制备得到可磁分离的"核-壳"结构纳米复合物Mn0.6Zn0.4Fe2O4@Si O2(Si-Fe-MNCs),并采用X射线衍射(XRD)、N2吸附-脱附、扫描电镜(SEM)、透射电镜(TEM)、X射线光电子能谱(XPS)和振动样品磁强计(VSM)对Si-Fe-MNCs进行了表征.同时,以难生物降解染料罗丹明B(Rh B)为目标污染物,利用Si-Fe-MNCs催化过氧化氢降解Rh B,考察了不同体系、过氧化氢用量、催化剂投加量及温度等对催化活性的影响.结果表明,当温度为303 K,催化剂用量为0.5 g·L-1,过氧化氢(质量分数15%)加入量为4 m L,Rh B(20 mg·L~(-1))加入量为50 m L时,H2O2利用率为81.3%,罗丹明B降解率为95%,CODC r去除率为98.0%;自由基验证实验及XPS表征结果表明,Rh B与Si-Fe-MNCs催化H2O2产生的·OH反应而得以降解,该反应为固液界面催化反应,FeMNPs中存在的氧空位对催化反应起到协同强化作用.  相似文献   

3.
Sorption of U(VI) onto TiO2 as functions of pH, ionic strength, contact time, soil humic acid (SHA), solid-to-liquid ratio and temperature was studied under ambient conditions using batch and spectroscopic approaches. The sorption of U(VI) on TiO2 was significantly dependent on pH and ionic strength. The presence of SHA slightly enhanced the sorption of U(VI) on TiO2 below pH 4.0, while it inhibited U(VI) sorption in the higher pH range. U(VI) sorption on TiO2 was favored at high temperatures, and the sorption process was estimated to be endothermic and spontaneous. Reduction of U(VI) to lower valent species was confirmed by X-ray photo-electron spectroscopy analysis. It is very interesting to find that U(VI) sorption on TiO2 was promoted in solutions with higher back-ground electrolyte concentrations. In the presence of U(VI), higher back-ground electrolyte made more TiO2 particles aggregate through (001) facets, leading more (101) facets to be exposed. Therefore, the reduction of U(VI) was enhanced by the exposed (101) facets and more U(VI) removal was observed.  相似文献   

4.
The effect of ammonium sulfate ((NH4)2SO4) and urea (CO(NH2)2) on polychlorinated dibenzo-p-dioxin and dibenzofuran (PCDD/F) formation from active carbon was investigated in this study. Both additives could significantly inhibit PCDD/F formation, and PCDD/F (TEQ) generation was reduced to 98.5% (98%) or 64.5% (77.2%) after 5% (NH4)2S04 or CO(NH2)2 was added into model ash, respectively. The inhibition efficiency of PCDDs was higher than the value of PCDFs, however, the reduction of PCDD/F yield was mainly from PCDFs decreasing. In addition, the solid-phase products were reduced more than the gas-phase compounds by inhibitors. By the measurement of chlorine emission in the phase of ion (Cl[Cl^-]) and molecule gas (Cl[Cl2]), it was observed that both Cl[Cl^-] and Cl[Cl2] were reduced after inhibitors were added into ash. Cl[Cl2] was reduced to 51.0% by urea addition, which was supposed as one possible mechanism of PCDD/F inhibition.  相似文献   

5.
对南京市的18个采样点进行PM_(2.5)样品采集,并利用电感耦合等离子体质谱仪以及液相电感耦合等离子体质谱联用仪分别对样品中的总砷和4种水溶性砷进行测量,在此基础上研究PM_(2.5)中砷的形态及其时空分布特征.结果表明:南京市PM_(2.5)中的砷以无机砷为主,有机砷为辅.无机砷以三价砷(As(III))为主,五价砷(As(V))为辅,As(III)/As(V)的平均值为0.39±0.03.有机砷以二甲基胂酸(DMAs(V))为主,所有样品均未检出甲基胂酸(MMAs(V)).总砷(As_T)、As(III)、As(V)和DMAs(V)的年平均浓度分别为6.90、0.99、3.20和0.03 ng·m~(-3).PM_(2.5)中的砷浓度具有明显季节变化:总砷和As(V)最大浓度出现在冬季,As(III)最大浓度出现在夏季,DMAs(V)只在夏季出现.T检验表明:As(III)、总砷和DMAs(V)年平均浓度在城区和郊区之间存在显著差异.空间变异系数的计算结果表明DMAs(V)的空间变化最大,其空间变异系数为0.6.总砷和3种水溶性砷年平均浓度由大到小排列为:农村郊区城区.道路采样点和城市背景点的总砷年平均浓度比为0.92,说明城区交通源对PM_(2.5)中砷污染的贡献不明显.As(III)和As(V)的主要排放源可能为燃煤电厂和钢铁冶炼厂,而DMAs(V)可能主要来源于生物挥发产物的二次生成.  相似文献   

6.
Carbon dioxide (CO2) adsorption on a standard metal-organic framework Mg2(dobdc) (Mg/DOBDC or Mg-MOF-74) and a tetraethylenepentamine (TEPA) modified Mgz(dobdc) (TEPA-Mg/DOBDC) were investigated and compared. The structural information, surface chemistry and thermal behavior of the adsorbent samples were characterized by X-ray powder diffraction (XRD), infrared spectroscopy (IR), thermogravimetric analysis (TGA) and nitrogen adsorption-desorption isotherm analysis. CO2 adsorption capacity was measured by dynamic adsorption experiments with N2-CO2 mixed gases at 60℃. Results showed that the CO2 adsorption capacity of Mg/DOBDC was significantly improved after amine modification, with an increase from 2.67 to 6.06 mmol CO2/g adsorbent. Moreover, CO2 adsorption on the TEPA-Mg/DOBDC adsorbent was promoted by water vapor, and the adsorption capacity was enhanced to 8.31 mmol CO2/g absorbent. The adsorption capacity of the TEPA-Mg/DOBDC adsorbent dropped only 3% after 5 consecutive adsorption]desorption cycles. Therefore, this kind of adsorbent can be considered as a promising material for the capture of CO2 from flue gas.  相似文献   

7.
三峡澎溪河流域消落区与岸边土壤磷形态特征   总被引:5,自引:3,他引:2  
黄俊杰  王超  方博  冯磊  方芳  李哲  郭劲松 《环境科学》2017,38(9):3673-3681
选取了落干期澎溪河流域6个消落区点位,分析了消落区土壤磷形态分布特征,并探讨了各形态磷之间的相关性.结果表明,(1)采用SMT法测定了消落区土壤总磷、无机磷和有机磷含量,其总磷TP含量均值为575.29 mg·kg~(-1),有机磷OP含量均值为91.23 mg·kg~(-1).(2)采用Hedley法分析了消落区土壤磷的5种赋存形态,其中WA-Pi、PA-Pi、Fe/Al-Pi等3种易迁移的无机磷形态之和占可提取Pi的11.61%,且低于岸边土壤;WA-Po、PA-Po两种生物可利用性较高的有机磷形态含量之和占可提取Po的22.28%,而中活性有机磷Fe/Al-Po占可提取Po的66.30%,且消落区土壤各形态Po含量均低于岸边土壤,又以Fe/Al-Po含量差异最大.(3)消落区土壤TP与活性较强的WA-Pt、PA-Pt呈显著相关,表明消落区土壤活性磷含量主要受TP影响;各形态磷之间不具有显著相关性,表明不同形态磷的来源可能不同;消落区土壤Fe/Al-Pt与土壤有机质OM呈显著相关,表明土壤有机质的含量可能影响铁铝结合态磷含量.在淹水条件下,消落区土壤磷组分的释放对上覆水体的潜在影响不容忽视.  相似文献   

8.
以过一硫酸氢盐(PMS)作为氧化剂,利用化学吸收氧化法去除甲硫醇(CH3SH)恶臭气体.研究了p H(2~13)对CH3SH吸收过程、PMS氧化降解CH3SH过程的影响.结果表明,PMS不同于H2O2,在p H小于CH3SH p Ka(10.3)的弱碱性条件(p H=8~10)下,也可以有效去除CH3SH,而此时H2O2对CH3SH没有去除效果.可能的原因是,在弱碱性条件(p H=8~10)下PMS或可能产生的活性物种在气液相界面直接快速氧化CH3SH分子.  相似文献   

9.
利用臭氧氧化技术对铅锌硫化矿浮选过程各单元作业废水及尾矿库外排水进行处理,根据硫酸根离子浓度增量计算废水中低价态硫(价态小于+6)浓度.采用吹扫捕集-气相色谱质谱联用仪(PTC-GC/MS)检测浮选药剂(丁基二硫代碳酸钠(n-BX)、二乙基二硫代氨基甲酸钠(DDTC)、腐殖酸钠(SH)、松醇油)水溶液的自然降解产物、尾矿库进水及外排水中的挥发性有机硫化物(VOSCs).结果表明,尾矿库主要进水水源中低价态硫浓度为112 mg·L-1,其中,二硫化碳(CS2)在检测组分中所占相对比例为35.60%,是主要的VOSCs物质.各单元作业中浮选作业工段加入大量浮选药剂,浮选药剂水溶液自然降解产物中均检出CS2,而用药量最大的n-BX(C5H9Na OS2)自然降解产物中CS2相对比例最高(80.33%),因此,n-BX是浮选废水中VOSCs主要药剂来源.尾矿库外排水中低价态硫浓度为22 mg·L-1,其中,VOSCs物质主要有3,6-二甲基-1,2,4,5-四硫环己烷(C2H4S4)、N-巯基-甲酰胺(CH2SNO)和2-甲基-3-噻唑啉(C4H7NS),尾矿库外排水中C2H4S4所占相对比例为22.59%,是主要VOSCs物质.尾矿库水体中微生物通过消耗CS2生成C2H4S4进行新陈代谢.本研究结果可为铅锌硫化矿浮选工艺改进和安全排放提供参考.  相似文献   

10.
使用TaPL3模型对兰州地区16种PAHs通过大气和水体的长距离迁移潜力(LRTP)和总持久性(Pov)进行了模拟研究,比较了不同环数多环芳烃(PAHs)的特征迁移距离(CTD)和Pov的大小,对两者的关系进行了分析讨论,并以BaP为例对关键参数进行了灵敏度分析.研究结果表明,16种PAHs在兰州地区通过大气的特征迁移距离(CTDAir)在18.9km(BghiP)和734.9km(PYR)之间,总持久性(PovAir)在0.41d(ACE)和1304.76d(BaP)之间;通过水体的特征迁移距离(CTDWater)在511.1km(NAP)和34472.6km(BghiP)之间,PovWater在5.35d(NAP)和4156.59d(BghiP)之间.16种PAHs中,芘在空气中的LRTP最大,苯并[ghi]芘在水中的LRTP最大.中、高环数PAHs的PovAir和PovWater要比低环数PAHs高.此外,CTD和Pov没有表现出直接的关系.与国外的同类研究相比,BaP在兰州地区的CTDAir明显偏低.  相似文献   

11.
The selective recovery of copper from strongly acidic wastewater containing mixed metal ions remains a significant challenge. In this study, a novel reagent zinc dimethyldithiocarbamate (Zn(DMDC)2) was developed for the selective removal of Cu(II). The removal efficiency of Cu(II) reached 99.6% after 120 min reaction at 30°C when the mole ratio Zn(DMDC)2/Cu(II) was 1:1. The mechanism investigation indicates that the Cu(DMDC)2 products formed as a result of the displacement of Zn(II) from the added Zn(DMDC)2 by Cu(II) in wastewater, due to the formation of stronger coordination bonds between Cu(II) and the dithiocarbamate groups of Zn(DMDC)2. Subsequently, we put forward an innovative process of resource recovery for strongly acidic wastewater. Firstly, the selective removal of Cu(II) from actual wastewater using Zn(DMDC)2, with a removal efficiency of 99.7%. Secondly, high-value CuO was recovered by calcining the Cu(DMDC)2 at 800°C, with a copper recovery efficiency of 98.3%. Moreover, the residual As(III) and Cd(II) were removed by introducing H2S gas, and the purified acidic wastewater was used to dissolve ZnO for preparation of valuable ZnSO4·H2O. The total economic benefit of resource recovery is estimated to be 11.54 $/m3. Accordingly, this study provides a new route for the resource recovery of the treatment of copper-containing acidic wastewater.  相似文献   

12.
Despite the (TTAGG)n telomeric repeat supposed being the ancestral DNA motif of telomeres in insects, it was repeatedly lost within some insect orders. Notably, parasitoid hymenopterans and the social wasp Metapolybia decorata (Gribodo) lack the (TTAGG)n sequence, but in other representatives of Hymenoptera, this motif was noticed, such as different ant species and the honeybee. These findings raise the question of whether the insect telomeric repeat is or not phylogenetically predominant in Hymenoptera. Thus, we evaluated the occurrence of both the (TTAGG)n sequence and the vertebrate telomere sequence (TTAGGG)n using dot-blotting hybridization in 25 aculeate species of Hymenoptera. Our results revealed the absence of (TTAGG)n sequence in all tested species, elevating the number of hymenopteran families lacking this telomeric sequence to 13 out of the 15 tested families so far. The (TTAGGG)n was not observed in any tested species. Based on our data and compiled information, we suggest that the (TTAGG)n sequence was putatively lost in the ancestor of Apocrita with at least two subsequent independent regains (in Formicidae and Apidae).  相似文献   

13.
模拟高藻期碱性水源水,采用高铁酸钾对水中以颤藻和二甲基三硫醚为代表的藻类及微量嗅味污染物进行同步控制研究.在高铁酸钾与聚合氯化铁(PFC)单独混凝对藻类的控制效果对比的基础上,展开了高铁酸钾与高锰酸钾预氧化-PFC联用方法对藻类及嗅味污染物的控制效果对比,探讨了pH、预氧化时间和浊度等条件对控制效果的影响.结果表明,PFC单独混凝除藻率最高为90.6%,以Fe计的等量投加条件下,高铁酸钾控藻效果较PFC混凝好,除藻率可达92.4%.高锰酸钾对PFC具有强化混凝效果,可明显提高除藻率(94.5%).高铁酸钾较高锰酸钾预氧化对二甲基三硫醚的去除效果理想,且氧化时间大大缩短,高铁酸钾氧化时间1 min可去除92.5%二甲基三硫醚,高于高锰酸钾预氧化10 min后达到的去除率(74.6%).  相似文献   

14.
基于2013—2015年南昌市9个空气环境监测点的连续数据,分析了空气PM_(2.5)、PM_(10)质量浓度(以下简称浓度)的时空变异规律,并以景观格局指数为定量指标,研究了监测点的两种颗粒物浓度与其周边500 m半径、1000 m半径缓冲区的土地利用状况的关系.结果表明:(1)南昌市3年来PM_(2.5)和PM_(10)浓度逐年显著降低.(2)通过聚类分析,9个监测站依据颗粒物污染可分为4大类,表现出一致的城乡梯度差异.(3)在斑块类型水平上,PM_(2.5)和PM_(10)浓度与500、1000 m半径缓冲区的C-PLAND(建筑用地覆盖率)、C-SHDI(建筑用地多样性指数)显著正相关,与1000m缓冲区的F-ED(林地边界密度)显著正相关;与F-PLAND(林地覆盖率)、C-Fi(建筑用地分离度指数)、F-MPS(林地平均斑块面积)显著负相关.在景观水平上,PM_(2.5)和PM_(10)浓度在500 m缓冲区与LPI(最大斑块所占景观比例)显著负相关;与1000 m缓冲区的MPS(平均斑块面积)显著负相关.景观格局指数直接反映土地利用状况,它与PM_(2.5)和PM_(10)浓度的相关性,表现出生态学中典型的"源汇景观"关系.  相似文献   

15.
Using a liquid–solid phase inversion method, a hybrid matrix poly(vinylidene fluoride)(PVDF) membrane was prepared with alumina(Al2O3) nanoparticle addition. Pd/Fe nanoparticles(NPs) were successfully immobilized on the Al2O3/PVDF membrane, which was characterized by Scanning Electron Microscopy(SEM) and Transmission Electron Microscopy(TEM). The micrographs showed that the Pd/Fe NPs were dispersed homogeneously. Several important experimental parameters were optimized, including the mechanical properties, contact angle and surface area of Al2O3/PVDF composite membranes with different Al2O3 contents. At the same time, the ferrous ion concentration and the effect of hydrophilization were studied. The results showed that the modified Al2O3/PVDF membrane functioned well as a support. The Al2O3/PVDF membrane with immobilized Pd/Fe NPs exhibited high efficiency in terms of dichloroacetic acid(DCAA) dechlorination. Additionally, a reaction pathway for DCAA dechlorination by Pd/Fe NPs immobilized on the Al2O3/PVDF membrane system was proposed.  相似文献   

16.
采用化学热力学平衡分析方法,应用污泥实测数据模拟计算了深度脱水后污泥焚烧过程中调理剂的热转化过程及逸出产物,并预测了含Cl调理剂与CaO耦合作用对重金属迁移转化及排放的影响.研究结果表明,污泥添加单一调理剂Al_2(SO_4)_3、Fe_2(SO_4)_3、FeSO_4、AlCl_3及FeCl_3后,Fe和Al在高温下主要以Al_2O_3(s)和Fe_2O_3(s)存在,主要气态产物是HCl和SO_2.调理剂CaO和FeCl_3共存且含量增加时,焚烧过程中HCl(g)逸出过程变慢,并且Fe_2O_3(s)易于和CaO(s)作用导致Fe_2O_3(s)存在温度区间变窄.污泥未添加调理剂焚烧过程中,重金属Cd、Pb、Cr、Tl、Hg、As易于以Cd(OH)_2(g)、PbO(g)、CrO_2(OH)_2(g)、AsO(g)、Hg(g)、Tl(g)形式挥发,而Cu、Zn、Ni以其氧化物形式存在而难挥发.调理剂FeCl_3及CaO添加到污泥后,重金属(Cd、Pb、Cu、Zn、Ni、Hg、Tl)的分布受FeCl3的影响大于CaO,导致其形成重金属氯化物而挥发,而Cr和As与CaO作用生成CaCr_2O_4(s)、Ca_3(AsO_4)_2(s)热稳定化学物,抑制了Cr、As的挥发.当脱水污泥与含硫化物掺烧时,重金属(Pb、Cu、Zn、Ni)挥发受到Cl的影响大于S,在低温区间其主要以硫酸盐为主,在中高温区间以氯化物存在,而Hg和Tl不受硫化物影响.  相似文献   

17.
The fraction of oil (C10-C40) became more biodegradable after graded modified Fenton’s oxidation, therefore, it can be considered a mild pre-treatment method to obtain more effective bioremediation for oil contaminated soil.  相似文献   

18.
活性炭催化过氧化氢去除荧光增白剂   总被引:1,自引:1,他引:0  
刘海龙  张忠民  赵霞  焦茹媛 《环境科学》2014,35(6):2201-2208
研究了活性炭(activated carbon,AC)吸附、改性活性炭(activated carbon modified,ACM)吸附、过氧化氢(H2O2)氧化、AC催化H2O2等方法对水体中荧光增白剂VBL的处理效果,并通过自由基俘获剂叔丁醇、催化过程气体分析等探讨了AC催化H2O2分解VBL的机制.结果表明,经硝酸铁[Fe(NO3)3]改性过的ACM对VBL的吸附去除率高于未改性的AC.活性炭催化H2O2对VBL的去除效果明显,但未改性AC催化去除率高于ACM.60 min时,AC催化氧化去除率即可达到95%以上,而ACM仅为58%.叔丁醇的加入降低了AC和ACM催化氧化对VBL的去除率,表明AC催化H2O2氧化能促进H2O2形成羟基自由基(·OH)和原子氧参与反应.AC催化H2O2分解及释放气体分析表明,AC能催化H2O2形成氧气并放热,且ACM明显快于AC.结合催化H2O2去除VBL效率的结果分析,ACM催化反应时活性中间物(自由基和原子氧等)产生速率快于AC,活性中间物自身消耗形成氧气,而不是用于分解VBL.催化反应中活性中间产物的形成速率与反应物供给速率的不匹配可能是导致ACM催化效果弱于AC的重要原因.  相似文献   

19.
热处理对SnO2/Ti电化学催化降解p-苯醌的影响   总被引:3,自引:3,他引:0  
用热分解方法制备了钛基二氧化锡阳极(SnO2/Ti),对比研究了空气/氧气2种热处理气氛对电极性能的影响.用扫描电镜(SEM)观察了电极表面形貌,对电极表面主要膜元素的化学状态进行了X射线光电子能谱(XPS)分析,对电极在不同溶液的动电位极化行为进行了测试,研究了2种电极在5mA/cm2恒电流状态下对p-苯醌的电解催化去除性能.SEM观察表明,2种电极表面都为典型的泥裂形貌,但在氧气气氛中退火处理的电极具有更大的活性表面积.XPS分析发现,在氧气气氛中退火处理的电极表面Sn3d5/2、Sb3d5/2电子的结合能较在空气气氛中退火处理的低0.15eV.动电位极化测试结果与恒电流电解实验结果都表明,在氧气气氛中退火处理的电极对水中p-苯醌具有更好的电化学催化去除性能.在电解进行至溶液完全脱色的情况下,氧气气氛中退火处理的电极对水中TOC的去除率为76.3%,而空气气氛中退火处理的电极对水中TOC的去除率为63.3%.在2种电极条件下,溶液中TOC浓度随电解时间的变化规律均符合指数变化规律.  相似文献   

20.
The catalytic oxidation effect of MnSO4 on As(III) by air in an alkaline solution was investigated. According to the X-ray diffraction (XRD), scanning electron microscope-energy dispersive spectrometer (SEM-EDS) and X-ray photoelectron spectroscopy (XPS) analysis results of the product, it was shown that the introduction of MnSO4 in the form of solution would generate Na0.55Mn2O4·1.5H2O with strong catalytic oxidation ability in the aerobic alkaline solution, whereas the catalytic effect of the other product MnOOH is not satisfactory. Under the optimal reaction conditions of temperature 90°C, As/Mn molar ratio 12.74:1, air flow rate 1.0 L/min, and stirring speed 300 r/min, As(III) can be completely oxidized after 2 hr reaction. The excellent catalytic oxidation ability of MnSO4 on As(III) was mainly attributed to the indirect oxidation of As(III) by the product Na0.55Mn2O4·1.5H2O. This study shows a convenient and efficient process for the oxidation of As(III) in alkali solutions, which has potential application value for the pre-oxidation of arsenic-containing solution or the detoxification of As(III).  相似文献   

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