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1.
传统原位化学氧化地下水修复技术存在氧化剂迁移距离短和利用率低等问题。本研究在双井循环模式促进传质的基础上,通过注水井中的地下水电解原位提供O 2和H 2,配合乙二胺四乙酸(ethylenediamine tetraacetic acid,EDTA)络合溶解出含水层Fe(Ⅱ),活化O 2产生羟基自由基(•OH),实现地下水三氯乙烯(TCE)的氧化降解。在填充了砂土和黏土互层的二维砂槽中,设置电流为0.2 A、流速为72 cm/d、初始TCE浓度为3 mg/L,经过9 d的连续通电处理后,TCE浓度降低到1 mg/L,降解率达到67%。通电前投加0.5 mmol/L EDTA,经过1 d水流循环后含水层中溶解态Fe(Ⅱ)浓度从02 mg/L增加到414 mg/L,黏土区域较高。通电过程中,循环井促进O 2、Fe(Ⅱ)-EDTA和TCE的有效接触与反应,使TCE氧化降解。通电初期,黏土区域Fe(Ⅱ)氧化速率、TCE降解速率较周围慢,后期差异逐渐减小。未通电时加入醋酸钠可促进Fe(Ⅲ)还原,使含水层中铁循环利用。该修复过程通过循环井提升了氧化剂迁移距离,使用源于含水层的Fe(Ⅱ)-EDTA和稳定性较好的O 2提高了氧化剂利用率,有望应用于有机污染地下水修复。 相似文献
2.
本文通过两组不同水镁石-苯酚投料比的实验,研究固体沉淀物与水质变化的关系。实验显示,水镁石解离出的Mg 2+与苯酚降解的中间产物能形成难溶盐,并发生沉淀分离,促进含苯酚废水臭氧化降解的效率。当苯酚的初始浓度为47 g/L,初始碳镁原子比(C/Mg)为30时,经3小时充分臭氧化曝气后,投加的水镁石全部耗尽。XRD、TG/DSC结果显示新形成的沉淀物为草酸镁。反应终点的pH值在4以下,TOC去除率为40%。当体系的初始C/Mg(原子比)为1,苯酚的初始浓度为1.5 g/L时,同样的臭氧化曝气过程体系残留的沉淀物仍是水镁石。反应终点的pH值在10左右,TOC去除率为92.8%。研究证明,苯酚臭氧化过程也是体系酸化的过程,至少在高C/Mg比条件下新生的质子能与水镁石解离出的羟基中和,水镁石解离出的Mg 2+可与草酸根结合沉淀出草酸镁。 相似文献
3.
研究了La 0.5 Sr 0.5 Co 0.8 Mn 0.2 O 3-δ钙钛矿活化过氧单硫酸盐对四溴双酚A(TBBPA)的降解作用,重点探讨不同的煅烧温度制备镧锶钴锰钙钛矿(LSCM82)的催化性能对过一硫酸盐降解TBBPA的影响,以及溶液的不同初始pH条件对优选材料体系降解效率的影响。结果发现,变价离子的氧化还原对Co3+/Co2+和(Mn4++Mn3+)/Mn2+是催化剂活性的主要贡献者。煅烧温度为950 ℃且具有适量间隙氧及比表面积的LSCM82-950催化反应速率较高。在中性pH环境条件下应用LSCM82-950活化过一硫酸盐降解水中TBBPA污染物,既可以使催化剂钴浸出很少,又能达到最大程度的TBBPA降解效果。 相似文献
4.
花岗伟晶岩型矿床是稀有金属矿床重要的类型之一。在花岗伟晶岩中,稀有金属元素Li、Be、Nb和Ta主要以独立矿物的形式存在,前人对稀有金属独立矿物在硅酸盐熔体中的溶解度及其影响因素展开了系统研究。本文综合分析了已有的实验数据,其结果表明,影响稀有金属独立矿物溶解度最为重要的2个参数是温度( T)和铝饱和指数(ASI)。因此本文建立了稀有金属独立矿物,尤其是铌锰矿和钽锰矿溶解度,与温度( T)和铝饱和指数(ASI)之间的定量关系: lg [ w(Li)/10 -6]=-0.37×[1 000/( T/K)]+4.56, R2=0.44 lg [ w(BeO)/10 -6]=-4.21×[1 000/( T/K)]+6.86, R2=0.91 lg [K sp(Nb)/(mg 2·kg -2)]=-(2.86±0.14)×ASI (Mn+Li)-(4.95±0.31)×[1 000/( T/K)]+(4.20+0.28), R2=0.86 lg [K sp(Ta)/(mg 2·kg -2)]=-(2.46±0.11)×ASI (Mn+Li)-(4.86±0.30)×[1 000/( T/K)]+(4.00+0.30), R2=0.80 式中,温度 T为热力学温度,ASI (Mn+Li)(ASI=Al 2O 3/(CaO+Na 2O+K 2O+Li 2O+MnO),摩尔分数比)和 T的适用范围分别为0.6~1.2和1 073~1 373 K的范围内。上述公式为估算硅酸盐熔体中稀有金属含量提供了便利,为量化花岗伟晶岩成矿模型提供了基础。 稀有金属独立矿物溶解度随温度降低和铝饱和指数的增加而急剧降低,因此,在岩浆演化过程中,由岩浆侵位、分离结晶以及流体作用等因素引起的岩浆温度降低和铝饱和指数的增加,是导致稀有金属独立矿物结晶的主要机制。 相似文献
5.
斜向扩张是超慢速扩张洋中脊独特的构造特征,其地形分段特征明显区别于经典的快速-慢速端元洋中脊模型,是理解超慢速扩张洋中脊地质过程的重要切入点。基于西南印度洋中脊Indomed-Gallieni和Shaka-DuToit段多波束地形数据,分析了不同斜向扩张角度( α)洋中脊的地形分段样式。其中,46.5°~47.5°E( α=5°)、16°~25°E( α=10°)和48.5°~52°E( α=15°)为近正向扩张段,发育雁列式叠置的中央火山脊;47.5°~48.5°E( α=50°)和16°~25°E( α=60°)为斜向扩张段,仅在洋脊段中部形成中央火山脊。利用有限差分+颗粒法(FD+MIC)数值模拟技术研究了洋中脊应变分布特征对不同 α值的响应,结合地形分析,认为斜向扩张角度和温度异常分布共同控制了洋中脊地形分段样式。近正向扩张洋中脊( α＜20 °)在温度异常处形成地壳伸展应变的集中区,有利于岩浆汇聚,发育雁列式叠置的中央火山脊,其位置随温度异常分布的变化而改变;斜向扩张洋中脊(α>20 °)地壳伸展应变集中区的位置受斜向扩张几何样式控制,在洋脊段中部发育中央火山脊,对温度异常不敏感,形成位置长期固定的岩浆活动中心。 相似文献
6.
采用浸渍法制备了用于常温常压下催化Fenton法的负载型Fe2O3/凹凸棒石催化剂,并将其用于处理十二烷基苯磺酸钠废水.采用BET,SEM,FT-IR对其进行了表征,并考察了Fe2O3/凹凸棒石催化剂的催化活性和稳定性.对于初始浓度为40 mg/L的十二烷基苯磺酸钠模拟废水,当Fe2O3/凹凸棒石催化剂和H2O2氧化剂的投加量分别为20 g/L和0.392 mol/L时,pH为5时,反应温度为80℃时,处理1h时染料的十二烷基苯磺酸钠的去除率可达到99.99％.与传统Fenton试剂法相比,以Fe2O3/凹凸棒石为催化剂的Fenton法,具有pH范围广(2～10),降解程度高和催化剂易回收再用的优点. 相似文献
7.
云南大丫口祖母绿常出现颜色环带,且伴随明显成分变化,而目前颜色环带的成因仍存争议,相关的多阶段成矿假说尚缺少明确证据。文章通过电子探针和激光剥蚀电感耦合等离子质谱仪对大丫口祖母绿的颜色环带及黑色矿物包裹体进行主微量元素成分分析,并对不同类型岩脉祖母绿中流体包裹体进行显微测温分析,进而探讨祖母绿颜色环带成因与多阶段成矿的联系。成分测试结果表明,从浅绿白核部至绿色边部,V(970×10 -6→10 077×10 -6)、Rb(9.6×10 -6→27.4×10 -6)、Cs(535×10 -6→3 108×10 -6)、Fe(1 376×10 -6→2 199×10 -6)和Ga(4×10 -6→14.7×10 -6)等微量元素的含量急剧增加。结合绿色晶体边部中同生黑色富钒电气石包裹体的分布,有力证明了大丫口祖母绿颜色分带的形成与晶体的多阶段成矿有关。流体包裹体测试结果表明,含矿长石-方解石脉、含矿石英脉和伟晶岩-变粒岩接触带中矿物的流体包裹体盐度范围分别为3.39%~10.36%(NaCl eq)、5.71%~12.29%(NaCl eq)和8%~18.72%(NaCl eq),指示了伟晶岩脉中祖母绿的多阶段结晶,且表明随结晶阶段演变,成矿流体的盐度逐渐升高。同时,成矿流体盐度升高也是晚期云英岩化阶段致色元素含量剧增的原因。 相似文献
8.
当家寺花岗岩体是青海南山印支期花岗岩带中东部较大的一个岩体,形成于早三叠世(243.5±2.9 Ma、247.2±1.7 Ma)—中三叠世(240.1±2.1 Ma、241.0±2.6 Ma)。岩体内发育有众多的中-酸性脉岩,岩石类型主要为闪长玢岩、石英闪长玢岩、花岗斑岩等,本研究获得闪长玢岩脉LA-MC-ICP-MS锆石U-Pb年龄为(235.6±2.4 Ma),表明其形成于晚三叠世早期,稍晚于当家寺岩体侵位时限。脉岩作为一种浅成侵入体,其与当家寺花岗岩体分布的构造位置相似,矿物组成及地球化学特征具有近似的特点,说明二者岩石成因及构造背景类似,可能为同一源区壳-幔岩浆混合作用的产物。岩石地球化学分析表明中性脉岩SiO 2含量低(54.68%~64.75%),酸性脉岩SiO 2含量高(66.00%~77.13%),二者都具高铝(Al 2O 3=12.24%~17.11%)、高钾钙碱性准铝质-弱铝质的特点(A/CNK=0.85~1.04),具有典型的岛弧花岗岩和碰撞花岗岩的特征。脉岩富集LREE、Rb、Th、K,亏损HREE、Nb、Ta、P、Ti、Ba,(La/Yb) N=5.05~17.61,表现出中等强度Eu的负异常。综合分析认为,脉岩形成于晚三叠世共和裂谷闭合碰撞造山后构造环境由挤压向板内稳定-伸展的变迁阶段,指示晚三叠世早期共和盆地周缘已进入后碰撞的陆内环境。 相似文献
9.
内蒙古北山白云山蛇绿混杂岩带南部中酸性侵入岩主要以脉岩形式产出。采用LA-ICP-MS锆石U-Pb定年和岩石地球化学分析,对脉岩的岩石类型、年代学、构造背景等进行研究,为北山洋的拼合碰撞时限提供年代学约束。研究结果显示:石英闪长岩的年龄为(420.0±1.0) Ma,花岗闪长岩的年龄为(404.6±2.6) Ma,表明脉岩形成时期为晚志留世—早泥盆世。中酸性侵入岩脉SiO 2含量为58.38%~69.46%,K 2O含量为0.74%~1.38%,Al 2O 3含量为15.54%~16.95%,Na 2O含量为4.15%~5.36%,岩石类型为钙碱性石英闪长岩和过铝质低钾拉斑系列的花岗闪长岩。石英闪长岩与花岗闪长岩源于陆缘火山弧区和同碰撞区,二者轻稀土元素相对重稀土元素明显富集, δEu负异常,高场强元素Ta、Nb亏损,显示出岛弧环境的典型特征,表明由于洋壳俯冲作用,研究区在晚志留世—早泥盆世发育了岛弧岩浆岩侵入体。随着俯冲作用深入,北山洋在晚志留世—早泥盆世早期完成闭合碰撞,并在研究区形成同碰撞花岗岩,碰撞时间应早于(404.6±2.6) Ma。 相似文献
10.
在对微电解、H 2O 2氧化机理研究的基础上,对装涂油漆废水提出利用微电解-化学氧化法处理的方案,通过实验确定出最佳的微电解反应条件及氧化条件。实验结果表明,该方法可使原水的ρ(COD cr)从4 000 mg/L降至100 mg/L,废水的COD cr去除率>95%,出水达到排放标准。本研究对微电解方案存在的问题进行了分析,并提出部分解决措施。 相似文献
11.
本研究采用臭氧-超声（O 3/US）联用技术处理聚乙烯醇（PVA）废水,分别考察了PVA初始质量浓度、初始pH、臭氧通入速率、超声功率、超声频率及反应时间对PVA和COD去除效率的影响,并在此基础上通过正交实验确定了降解PVA和COD的最佳实验条件。研究结果表明,超声频率对去除率有显著影响,PVA初始质量浓度对去除效率的影响较大,反应时间、超声功率、臭氧通入速率和初始pH的影响相对较小。通过影响实验和正交实验确定的最佳降解条件为:PVA初始质量浓度100 mg/L、初始pH=9、臭氧通入速率4 g/h、超声功率320 W、超声频率40 kHz、反应时间20 min,此时COD和PVA的去除效率分别为86.4%和99.3%。超声对臭氧降解聚乙烯醇废水具有明显的协同作用,在最佳条件下,臭氧-超声联用技术比单独臭氧技术对PVA的去除率增加了5.1%,对COD去除率增加了19.4%。 相似文献
12.
As a result of the collapse of a mine tailing dam, a large extension of the Guadiamar valley was covered with a layer of pyritic sludge. Despite the removal of most of the sludge, a small amount remained in the soil, constituting a potential risk of water contamination. The kinetics of the sludge oxidation was studied by means of laboratory flow-through experiments at different pH and oxygen pressures. The sludge is composed mainly of pyrite (76%), together with quartz, gypsum, clays, and sulphides of zinc, copper, and lead. Trace elements, such as arsenic and cadmium, also constitute a potential source of pollution. The sludge is fine grained (median of 12 μm) and exhibits a large surface (BET area of 1.4±0.2 m 2 g −1). The dissolution rate law of sludge obtained is r=10−6.1(±0.3) [O2(aq)]0.41(±0.04) aH+0.09(±0.06) gsludge m−2 s−1 (22 °C, pH=2.5–4.7). The dissolution rate law of pyrite obtained is r=10−7.8(±0.3) [O2(aq)]0.50(±0.04) aH+0.10(±0.08) mol m−2 s−1 (22 °C, pH=2.5–4.7). Under the same experimental conditions, sphalerite dissolved faster than pyrite but chalcopyrite dissolves at a rate similar to that of pyrite. No clear dependence on pH or oxygen pressure was observed. Only galena dissolution seemed to be promoted by proton activity. Arsenic and antimony were released consistently with sulphate, except at low pH conditions under which they were released faster, suggesting that additional sources other than pyrite such as arsenopyrite could be present in the sludge. Cobalt dissolved congruently with pyrite, but Tl and Cd seemed to be related to galena and sphalerite, respectively. A mechanism for pyrite dissolution where the rate-limiting step is the surface oxidation of sulphide to sulphate after the adsorption of O2 onto pyrite surface is proposed. 相似文献
13.
We measured the Fe isotope fractionation during the reactions of Fe(II) with goethite in the presence and absence of a strong Fe(III) chelator (desferrioxamine mesylate, DFAM). All experiments were completed in an O 2-free glove box. The concentrations of aqueous Fe(II) ([Fe(II) aq]) decreased below the initial total dissolved Fe concentrations ([Fe(II) total], 2.15 mM) due to fast adsorption within 0.2 day. The concentration of adsorbed Fe(II) ([Fe(II) ads]) was determined as the difference between [Fe(II) aq] and the concentration of extracted Fe(II) in 0.5 M HCl ([Fe(II) extr]) (i.e., [Fe(II) ads] = [Fe(II) extr] − [Fe(II) aq]). [Fe(II) ads] also decreased with time in experiments with and without DFAM, documenting that fast adsorption was accompanied by a second, slower reaction. Interestingly, [Fe(II) extr] was always smaller than [Fe(II) total], indicating that some Fe(II) was sequestered into a pool that is not HCl-extractable. The difference was attributed to Fe(II) incorporated into goethite structure (i.e., [Fe(II) inc] = [Fe(II) total] −[Fe(II) extr]). More Fe(II) was incorporated in the presence of DFAM than in its absence at all time steps. Regardless of the presence of DFAM, both aqueous and extracted Fe(II) ( δ56/54Fe(II) aq and δ56/54Fe(II) extr) became isotopically lighter than or similar to goethite (− 0.27‰) at day 7, implying that the isotope exchange occurred between bulk goethite and aqueous Fe. Consistently, the mass balance indicated that the incorporated Fe is isotopically heavier than extracted Fe. These observations suggested that (i) co-adsorption of Fe(II) with DFAM resulted in more pervasive electron transfer, (ii) the electron transfer from heavy Fe(II) in the adsorbed Fe(II) to light Fe(III) in goethite results in the fixation of heavy adsorbed Fe(III) on the surface and accumulation of Fe(II) within the goethite, and (iii) desorption of the reduced, light Fe from goethite does not necessarily occur at the same surface sites where adsorption occurred. 相似文献
14.
氯代烃的污染治理已成为当今世界最热门的研究领域之一。以水体中最常见的氯代烃污染物1,1-二氯乙烯（1,1-DCE）、林丹（γ-HCH）为主要目标污染物,探讨了不同条件下负载型纳米Pd/Fe对氯代烃的去除效果。负载型纳米Pd/Fe采用浸渍→液相还原→还原沉淀的方法制备,透射电镜显示采用该方法制备的负载型金属钯和铁的平均粒径均在纳米级范围内。负载型纳米Pd/Fe具有较高的表面反应活性,当负载型纳米Pd/Fe 用量为40 g/L、反应时间达2 h时,1.1-二氯乙烯和林丹的去除率分别达到85%和100%。脱氯率与Pd/Fe投加量、钯含量、初始pH值、反应温度等因素有关,与溶液的初始浓度关系不大。负载型纳米Pd/Fe对11-DCE和γ-HCH去除均符合一级反应动力学方程,速率常数分别为0-528 3 h -1及2-012 9 h -1,反应的半衰期t1/2分别为1.31 h和0.34 h。推断在反应过程中,Fe腐蚀产生的H2为主要还原剂,Pd是良好的加氢催化剂,在金属颗粒表面形成高浓度反应相,使反应短时间内完成。 相似文献
15.
山西五台县北约15 km的白云村一带出露有叶蜡石矿及金矿化点,其形成特点与关系对区域深部找矿具有重要启示意义。该叶蜡石矿体产于经历古元古代绿片岩相变质的新太古代酸性火山岩之中(绢英片岩),切割区域片理并被晚期的辉绿玢岩截切。矿体总体呈透镜状产出,倾向北西,近东-西向延伸大于5 km,最厚处约1 km,未见底。该叶蜡石矿形成于中生代早白垩世。矿石矿物以叶蜡石和石英为主,含少量绢云母、伊利石、硬水铝石和赤铁矿等,反映出蚀变流体酸性及氧化的特征。叶蜡石矿体外围发育黄铁绢英岩化带,强度由近及远逐渐减弱。在靠近叶蜡石矿的黄铁绢英岩中,硫化物颗粒边缘常见赤铁矿化现象,应与叶蜡石化流体叠加有关。以上蚀变特征与叶蜡石化细脉灌入黄铁绢英岩相吻合。叶蜡石矿体上盘的黄铁绢英岩化带宽约0.4 km,其内发育一小型石英脉型金矿(岭底金矿),下盘的黄铁绢英岩化带最宽约1.5 km,局部发育金矿化现象((1~18)×10 -6)。黄铁绢英岩中硫化物以黄铁矿为主,可见少量黄铜矿、斑铜矿和辉铜矿。金矿化黄铁绢英岩以发育大量浸染型黄铁矿为特征,该类黄铁矿无韧性变形,未见其他共生硫化物,SEM-EDS分析结果显示其内发育有明显的不可见金。黄铁绢英岩化可依据矿物变形与否分为两期。早期的蚀变分布局限,见于新太古代糜棱岩化奥长花岗岩与酸性火山岩(绢英片岩)接触带,其中的黄铁矿、绢云母和石英等矿物发育韧性变形特征;晚期的蚀变带内硫化物、绢云母和石英均无韧性变形特征。依据样品的岩相学及全岩Au、As含量特征,可以确认金矿化与晚期黄铁绢英岩化有关,与早期蚀变无关。叶蜡石矿石的H-O同位素组成( δ18O V-SMOW=11.2‰~13.9‰; δD V-SMOW=-34‰~-20‰)显示流体以气相为主,且缺乏大气水的混合。上述特征说明白云叶蜡石矿是深部岩浆侵位固结后出溶的以气相为主的热液与浅部新太古代变质火山岩反应的结果,类似于斑岩成矿系统中普遍发育的高级泥化带(岩帽)的底部蚀变特征。 相似文献
16.
Pyrite and marcasite were precipitated by both slow addition of aqueous Fe 2+ and SiO 32− to an H 2S solution and by mixing aqueous Fe 2+ and Na 2S 4 solutions at 75°C. H 2S 2 or HS 2− and H 2S 4 or HS 4− were formed in the S 2O 32− and Na 2S 4 experiments, respectively. Marcasite formed at pH < pK 1 of the polysulfide species present (for H2S2, pK1 = 5.0; for H2S4, pK1 = 3.8 at 25° C). Marcasite forms when the neutral sulfane is the dominant polysulfide, whereas pyrite forms when mono-or divalent polysulfides are dominant. In natural solutions where H 2S 2 and HS 2 are likely to be the dominant polysulfides, marcasite will form only below pH 5 at all temperatures. The pH-dependent precipitation of pyrite and marcasite may be caused by electrostatic interactions between polysulfide species and pyrite or marcasite growth surfaces: the protonated ends of H2S2 and HS2 are repelled from pyrite growth sites but not from marcasite growth sites. The negative ions HS2 and S22− are strongly attracted to the positive pyrite growth sites. Masking of 1πg* electrons in the S2 group by the protons makes HS2 and H2S2 isoelectronic with AsS2− and As22−, respectively (
et al., 1981). Thus, the loellingitederivative structure (marcasite) results when both ends of the polysulfide are protonated. Marcasite occurs abundantly only for conditions below pH 5 and where H2S2 was formed near the site of deposition by either partial oxidation of aqueous H2S by O2 or by the reaction of higher oxidation state sulfur species that are reactive with H2S at the conditions of formation e.g., S2O32− but not SO42−. The temperature of formation of natural marcasite may be as high as 240°C (
and
, 1985), but preservation on a multimillion-year scale seems to require post-depositional temperatures of below about 160°C (
, 1973;
and
, 1985). 相似文献
17.
The dissolution and precipitation rates of boehmite, AlOOH, at 100.3 °C and limited precipitation kinetics of gibbsite, Al(OH) 3, at 50.0 °C were measured in neutral to basic solutions at 0.1 molal ionic strength (NaCl + NaOH + NaAl(OH) 4) near-equilibrium using a pH-jump technique with a hydrogen-electrode concentration cell. This approach allowed relatively rapid reactions to be studied from under- and over-saturation by continuous in situ pH monitoring after addition of basic or acidic titrant, respectively, to a pre-equilibrated, well-stirred suspension of the solid powder. The magnitude of each perturbation was kept small to maintain near-equilibrium conditions. For the case of boehmite, multiple pH-jumps at different starting pHs from over- and under-saturated solutions gave the same observed, first order rate constant consistent with the simple or elementary reaction: . This relaxation technique allowed us to apply a steady-state approximation to the change in aluminum concentration within the overall principle of detailed balancing and gave a resulting mean rate constant, (2.2 ± 0.3) × 10−5 kg m−2 s−1, corresponding to a 1σ uncertainty of 15%, in good agreement with those obtained from the traditional approach of considering the rate of reaction as a function of saturation index. Using the more traditional treatment, all dissolution and precipitation data for boehmite at 100.3 °C were found to follow closely the simple rate expression: Rnet,boehmite=10-5.485{mOH-}{1-exp(ΔGr/RT)}, with Rnet in units of mol m−2 s−1. This is consistent with Transition State Theory for a reversible elementary reaction that is first order in OH− concentration involving a single critical activated complex. The relationship applies over the experimental ΔGr range of 0.4–5.5 kJ mol−1 for precipitation and −0.1 to −1.9 kJ mol−1 for dissolution, and the pHm ≡ −log(mH+) range of 6–9.6. The gibbsite precipitation data at 50 °C could also be treated adequately with the same model:Rnet,gibbsite=10-5.86{mOH-}{1-exp(ΔGr/RT)}, over a more limited experimental range of ΔGr (0.7–3.7 kJ mol−1) and pHm (8.2–9.7). 相似文献
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