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1.
动态光散射技术原位表征天然有机质存在下纳米零价铁的团聚效应 总被引：1，自引：1，他引：0
纳米零价铁原位修复地下水污染是近年发展起来的新技术,通过改性合成不同种类纳米零价铁可以克服其易团聚易氧化的问题,水体中存在的天然有机质也会对纳米铁的分散性和反应活性产生影响,因此开展原位测试并研究不同种类纳米铁在水中的团聚效应具有重要意义。本文对实验合成的纳米零价铁、羧甲基纤维素包覆纳米零价铁、膨润土负载纳米零价铁以及商用纳米零价铁,基于动态光散射技术(DLS),运用纳米粒度/Zeta电位分析仪,结合透射电子显微镜(TEM)和沉降光谱曲线等手段,对比研究了天然有机质(腐植酸HA)对纳米铁团聚效应的影响。结果表明,羧甲基纤维素包覆或膨润土负载改性提高了纳米零价铁颗粒的分散稳定性,有效抑制了团聚沉降,团聚体粒径分布在1000 nm以下。HA会吸附在纳米铁颗粒表面,从而增加静电排斥力,进一步减缓了团聚效应,尤其是对膨润土负载纳米零价铁的影响最为显著,其团聚体粒径能降至100 nm以下,沉降速率也极大减缓,分散稳定性表现最佳。本研究表明DLS结合TEM表征纳米颗粒是获得更加丰富的微观粒子信息的一种非常重要的手段。 相似文献
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纳米零价铁在多孔介质中的运动能力影响其作为污染地下水修复材料的应用潜力。已有研究多采用一维柱试验研究纳米零价铁的运动行为,对于其二维运动行为的报道有限。自主研发了模拟多孔介质中纳米颗粒运动的模型试验系统,采用细、中、粗3种不同粒径的玻璃珠模拟土体,通过取样测量和图像分析等方法获得了磷负载纳米铁在多孔介质中的运动行为。一维柱试验结果表明磷负载纳米铁在中玻璃珠和粗玻璃珠中均有一定的运动能力,其液相回收率分别为50.3%和41.0%,而在细玻璃珠中运动能力较差;二维模型试验表明磷负载纳米铁在中玻璃珠中的滞留量随距离逐渐降低,而在粗玻璃珠中则呈现出滞留量随距离先升高后降低的趋势。由模型试验结果分析可知,磷负载纳米铁的运动和滞留过程与多孔介质孔隙结构和流速密切相关,颗粒阻塞与表面沉积等不同物理过程的共同作用导致了其在不同粒径多孔介质中运动特性的差异。研究成果可用于评估磷负载纳米铁的运动能力及分析其在多孔介质中的运移和滞留机制,为纳米零价铁技术的工程应用和环境风险评价提供参考依据。 相似文献
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膨润土负载纳米铁去除地下水中六价铬研究 总被引：4，自引：1，他引：3
随着人民生活水平的提高和城市化进程的加快,有机污染物及重金属高强度场地污染对人类健康、生态环境及社会安全构成了严重威胁。地下水中的重金属Cr(Ⅵ)污染逐渐受到重视,纳米零价铁可以有效地将六价铬还原成三价铬,使其沉淀固定下来,从而将污染源区的污染物消减固定,防止其向周围扩散。然而由于纳米铁颗粒微小,易被氧化,极易团聚,自身活性受到限制,因此,纳米铁的分散性、稳定性、良好活性研究至关重要。采用低成本环境友好型粘土矿膨润土作为负载材料制备膨润土负载纳米铁（B-NZVI）,批实验和柱实验研究B NZVI去除模拟地下水中Cr(Ⅵ)。结果表明：(1)自制的膨润土负载纳米铁个体呈球形,呈分散状负载于膨润土;(2)相同铁含量的B-NZVI处理Cr(Ⅵ)的效率远大于纳米铁,还原反应符合伪一级反应动力学模型,表观速率常数K随着B NZVI初始浓度的减小而减小;(3)B NZVI在石英砂柱中基本无迁移,适用于点源污染,Cr(Ⅵ)穿透曲线为B-NZVI的实际应用提供了理论和实验基础。 相似文献
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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
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采用液相还原法成功制备纳米零价铁,并组装出生物质炭负载纳米零价铁复合材料(NZVI/BC)。XRD图谱显示,NZVI/BC由生物质炭(BC)和纳米零价铁(NZVI)两种成分复合而成;SEM图像显示,加入生物质炭之后,NZVI颗粒在炭表面分散良好。研究考察溶液p H值、还原剂投加量、铁/炭比和NO-3初始浓度等因素对NZVI/BC还原性能的影响。结果表明,NZVI/BC显示出优良的还原性能。在相同条件下,反应2 h,NZVI对NO-3的去除率为75%,而NZVI/BC对NO-3的去除率为96%。NZVI/BC是一种具有应用前景的硝态氮净化材料。 相似文献
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零价铁纳米颗粒具有许多异于本体物质的独特性质,在废水处理方面应用潜力巨大。以蒙脱石为载体和分散剂,通过硼氢化钠液相还原法制备了零价铁纳米颗粒。采用电镜及多种谱学技术手段对所得铁纳米颗粒进行了表征。结果表明,铁纳米颗粒大致呈球状形貌,平均粒径约为55 nm,在蒙脱石表面分散良好,具有零价铁内核-铁氧化物外壳结构,提高了纳米铁在空气氛中的稳定性。通过批次实验考察了负载型铁纳米颗粒净化Cr(Ⅵ)的效率、过程及机理。净化效果受p H值影响显著,在最优p H值为1.0条件下,零价铁内核因其表面氧化膜酸溶而出露,可作为有效成分快速高效去除水体中Cr(Ⅵ)污染物,机理为零价铁将吸附至其表面的Cr(Ⅵ)异相还原为Cr(Ⅲ)而去除。属自发放热吸附过程,动力学行为符合准二级模型,吸附等温线可用Langmuir方程较好拟合。研究成果为新型纳米零价铁材料的制备及其铬污染治理提供了理论支撑。 相似文献
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凹凸棒石铁/铝氢氧化物纳米复合材料对磷的吸附动力学研究 总被引：1，自引：0，他引：1
用铁/铝盐水解法制备了凹凸棒石/铝氢氧化物(PNCMⅠ)、凹凸棒石/铁氢氧化物(PNCMⅡ)和凹凸棒石/铁铝氢氧化物(PNCMⅢ)3种凹凸棒石纳米复合材料。对比了这3种纳米复合材料对水中磷的吸附净化能力,并利用吸附动力学实验探讨了3种材料对磷的吸附机理。结果发现:负载了铝/铁氢氧化物后凹凸棒石的晶体结构没有改变;温度对于3种吸附剂吸附磷的动力学参数影响不显著;3种吸附剂对磷的实际吸附量、理论吸附量和初始吸附速率均随着磷的初始浓度增大而增大。PNCMⅠ对磷的理论吸附量为18.18 mg/g,较其他2种吸附剂大。当磷的初始浓度从5 mg/L增加到50 mg/L,PNCM I对磷的初始吸附速率从0.125 mg/(g·min)增加到1.425 mg/(g·min)。3种凹凸棒石黏土纳米复合材料对磷的吸附符合准二级动力学方程,表明其吸附均为化学吸附。 相似文献
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比较了3种天然坡缕石粘土对不同程度磷污染水体的吸附净化能力,通过等温吸附实验和吸附动力学实验探讨了坡缕石粘土的磷吸附机制,并研究了不同形态铁负载对坡缕石粘土吸附净化磷污染水体性能和机制的影响.结果发现,3种天然坡缕石粘土对不同程度磷污染水体均有一定的吸附净化能力,其中含白云石较多的坡缕石粘土的磷吸附能力最强,吸附等温曲线呈S型,且Freundlich方程(R2=0.977 6)比Langmuir方程(R2=0.924 9)拟合效果更好;准一级方程、冥函数方程、抛物线扩散方程、准二级方程均能较好地模拟坡缕石粘土对磷的吸附动力学过程,说明坡缕石粘土对磷的吸附可能属于不均匀介质的多分子层吸附.此外,不同形态铁负载均能显著增强坡缕石粘土对不同程度磷污染水体的吸附净化能力,吸附等温曲线呈L型,Langmnir方程(Fe2 :R2=0.96,Fe3 :R2=0.967 7)比Freundlich方程(Fe2 :R2=0.965 7,Fe3 :R2=0.936 1)能略好地拟合铁负载坡缕石粘土的磷吸附等温结果,说明铁负载坡缕石粘土的磷吸附过程可能是均匀介质的单分子吸附.适量白云石有助于提高坡缕石粘土的磷吸附净化性能,铁负载可能通过改变坡缕石的表面电荷和吸附活性位点来改变其磷吸附机制,从而提高其磷吸附性能. 相似文献
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纳米铁还原脱氮动力学及其影响因素 总被引：3，自引：1，他引：2
饮用水中硝酸盐(NO3-)对人体健康有危害。为了去除水溶液中NO3-,在实验室制得纳米铁颗粒。它的粒径为20～40 nm,比表面积(BET)为49.16 m2/g。本研究通过批实验考察了纳米铁对NO3-还原脱氮动力学性质和影响NO3-脱氮快慢的主要因素,如反应pH、纳米铁投加量和NO3-起始浓度。实验结果表明,pH越低越有利于NO 3-还原。在一定范围内,NO 3-还原速率随纳米铁投加量增加而增大,而随NO 3-起始浓度升高而降低,反应遵循准一级反应动力学方程,表面吸附和氧化还原反应是纳米铁对NO3-脱氮的主要去除机理。纳米铁对NO3-还原过程中可能反应的途径进行了讨论,NO3-还原产物取决于反应条件。在本研究条件下,纳米铁对NO3-脱氮的最终产物主要为NH4+-N而不是N2,必须进行更多的研究来解决这一问题。 相似文献
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地下水中三氯乙烯(TCE)严重威胁公众健康和环境安全,纳米零价铁原位注射技术可以还原降解TCE,但是应用中,纳米零价铁存在易氧化团聚而失活、迁移性差等问题。为此,利用天然高分子壳聚糖作包覆剂增强分散性和稳定性,镍作催化剂增强反应活性,成功制备获得壳聚糖包覆纳米铁镍双金属颗粒(CS Fe Ni)。沉降光谱实验表明包覆壳聚糖后纳米铁的分散稳定性得到增强,Zeta电位测试进一步证实颗粒表面负电荷增加,提高了静电排斥力,使得CS Fe Ni分散稳定性明显改善。柱迁移实验表明改性后的CS Fe Ni迁移能力得到提高。批实验表明CS Fe Ni能够高效降解TCE并能完全脱氯,研究结果为纳米铁原位注射技术的实际应用提供了理论基础和实验参考。 相似文献
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六价铬Cr(Ⅵ)有巨毒性,对人类及生态环境有极大危害,运用纳米零价铁(nZVI)去除水中六价铬是一种快速高效的环境修复手段。前人的研究更多报道了pH值、温度、初始浓度等因素的影响,溶解氧(DO)的存在对于nZVI去除水体中Cr(Ⅵ)的作用却少有研究。在对比普通铁粉和纳米铁对六价铬去除的基础上,着重探讨了溶解氧(DO)对水中六价铬去除效果的影响及作用机制。批实验短期结果表明:由于纳米铁有较大的比表面积和更高的反应活性,导致nZVI的除Cr(Ⅵ)效率明显高于普通铁粉;溶解氧的存在促进了nZVI对Cr(Ⅵ)的去除,这是因为氧化作用产生较多的Fe2+,有利于Cr(Ⅵ)的去除,随着nZVI进一步氧化,产生的针铁矿、磁铁矿等铁氧化物能够进一步吸附Cr(Ⅵ),使得在有氧环境下Cr(Ⅵ)的去除效果好于无氧环境。 相似文献
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Highly reactive nano-scale biogenic magnetite (BnM), synthesized by the Fe(III)-reducing bacterium Geobacter sulfurreducens, was tested for the potential to remediate alkaline Cr(VI) contaminated waters associated with chromite ore processing residue (COPR). The performance of this biomaterial, targeting aqueous Cr(VI) removal, was compared to a synthetic alternative, nano-scale zero valent iron (nZVI). Samples of highly contaminated alkaline groundwater and COPR solid waste were obtained from a contaminated site in Glasgow, UK. During batch reactivity tests, Cr(VI) removal from groundwater was inhibited by ∼25% (BnM) and ∼50% (nZVI) when compared to the treatment of less chemically complex model pH 12 Cr(VI) solutions. In both the model Cr(VI) solutions and contaminated groundwater experiments the surface of the nanoparticles became passivated, preventing complete coupling of their available electrons to Cr(VI) reduction. To investigate this process, the surfaces of the reacted samples were analyzed by TEM-EDX, XAS and XPS, confirming Cr(VI) reduction to the less soluble Cr(III) on the nanoparticle surface. In groundwater reacted samples the presence of Ca, Si and S was also noted on the surface of the nanoparticles, and is likely responsible for earlier onset of passivation. Treatment of the solid COPR material in contact with water, by addition of increasing weight % of the nanoparticles, resulted in a decrease in aqueous Cr(VI) concentrations to below detection limits, via the addition of ⩾5% w/w BnM or ⩾1% w/w nZVI. XANES analysis of the Cr K edge, showed that the % Cr(VI) in the COPR dropped from 26% to a minimum of 4–7% by the addition of 5% w/w BnM or 2% w/w nZVI, with higher additions unable to reduce the remaining Cr(VI). The treated materials exhibited minimal re-mobilization of soluble Cr(VI) by re-equilibration with atmospheric oxygen, with the bulk of the Cr remaining in the solid fraction. Both nanoparticles exhibited a considerable capacity for the remediation of COPR related Cr(VI) contamination, with the synthetic nZVI demonstrating greater reactivity than the BnM. However, the biosynthesized BnM was also capable of significant Cr(VI) reduction and demonstrated a greater efficiency for the coupling of its electrons towards Cr(VI) reduction than the nZVI. 相似文献
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René van Herwijnen Tim Laverye Jane Poole Mark E. Hodson Tony R. Hutchings 《Applied Geochemistry》2007
Organic materials such as compost are often proposed as suitable materials for the remediation of contaminated brownfield sites intended for soft end-use. In addition to vitalising the soil, they are also believed to immobilise metals thereby breaking contaminant-receptor pathways and reducing the ecotoxicity of the contaminants. However, some research has demonstrated contradictory effects between composts on metal immobilisation. In the present study, four different composts and a liming product containing organic matter (LimeX70) were tested to examine both their metal retention and toxicity reduction capabilities on three different metal contaminated soils. Leaching tests, a plant growth test with Greek cress (Lepidium sativum), an earthworm (Eisenia fetida) survival and condition test and a bacterial toxicity test using Vibrio fischeri were carried out. The leaching test results showed that spent mushroom compost caused an increase in metal concentration in the leachates, while LimeX70 caused a decrease. The variation in behaviour between different amendments for each soil was high, so a generic conclusion could not be drawn. Toxicity tests showed significant reduction of metal bioavailability and toxicity for Greek cress, earthworms and bacteria. The results also suggest that more research should be undertaken to understand the mechanisms involved in metal complexation using different types of organic matter, in order to optimise the use of organic materials like compost for soil remediation. 相似文献
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Study of diclofenac removal by the application of combined zero-valent iron and calcium peroxide nanoparticles in groundwater 
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下载免费PDF全文 Liang Wen Zhou Nian-qing Dai Chao-meng Duan Yan-ping Zhou Lang Tu Yao-jen 《地下水科学与工程》2021,9(3):171-180
Diclofenac(DCF) is one of the most frequently detected pharmaceuticals in groundwater, posing a great threat to the environment and human health due to its toxicity. To mitigate the DCF contamination,experiments on DCF degradation by the combined process of zero-valent iron nanoparticles(nZVI) and nano calcium peroxide(nCaO_2) were performed. A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO_2 nanoparticles and pH value on the DCF removal.In the meantime, the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO_2 nanoparticles in the reaction system. The results show that the nZVI/nCaO_2 can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO_2 added, resulting in a removal rate of greater than 90% in a 2-hour reaction with an initial pH of 5. The degradation rate of DCF was positively correlated with the dosage of nCaO_2, and negatively correlated with both nZVI dosage and the initial pH value. The order of significance of the three factors is identified as pH value nZVI dosage nCaO_2 dosage. In the continuous-flow reaction system, the DCF removal rates remained above 75% within 150 minutes at the pH of 5, with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO_2. These results provide a theoretical basis for the nZVI/nCaO_2 application to remove DCF in groundwater. 相似文献
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污染物事故性排放、工矿企业搬迁后遗留的污染场地修复面临各种问题,给地下水资源的使用带来严重威胁。地下水VOCs污染,具有易扩散迁移、毒性高、风险大的特点,修复难度较高。本文结合典型深层地下水修复案例,充分分析场地地质背景、水文地质条件等,根据污染物的特性、污染范围和分布特征,探讨各种修复技术的修复机理、修复对象和技术特点,针对VOCs污染修复进行性能比较及适用性分析。同时通过两个阶段的试验综合研究,原位和异位技术相结合,为开展类似地下水VOCs污染修复实践和管理提供了依据和思路。 相似文献
17.
硫化纳米铁（S-nZVI）是一种具有壳核结构的新型纳米铁（nZVI）改性材料,在多种污染物的去除上表现出超越nZVI的反应活性。本文采用两步合成法制备了S-nZVI,并采用透射电镜-能量色散X射线（TEM-EDX）、X射线衍射（XRD）和X射线光电子能谱分析（XPS）方法对S-nZVI和nZVI进行表征,探讨了不同硫铁摩尔比（n（S）/n（Fe））、初始pH值、试剂投加量和地下水化学成分对nZVI及S-nZVI去除Cr（Ⅵ）的影响。结果表明：S-nZVI具有明显的壳核结构,其Fe0核外层包覆着非晶的硫化亚铁和多硫化物;S-nZVI去除Cr（Ⅵ）的最佳n（S）/n（Fe）为0.14;增加S-nZVI投加量会提高其对Cr（Ⅵ）的去除率,投加量相同时,S-nZVI对Cr（Ⅵ）的去除率显著高于nZVI;提高初始pH值时,S-nZVI和nZVI对Cr（Ⅵ）的去除率均逐渐降低,但在相同pH值条件下,S-nZVI对Cr（Ⅵ）的去除率和去除速率始终高于nZVI,尤其是在pH=5时,S-nZVI仍能去除100%的Cr（Ⅵ）,而nZVI只能去除85%;K+、Na+、Ca2+、Mg2+、SO42-、NO3-和Cl-对S-nZVI和nZVI去除Cr（Ⅵ）均有促进作用,但对S-nZVI体系的促进作用更强;HCO3-的存在会使溶液的pH值升高从而抑制S-nZVI和nZVI对Cr（Ⅵ）的去除,对nZVI的抑制作用强于S-nZVI。总体来说,S-nZVI对Cr（Ⅵ）的去除率在不同pH值和多种地下水化学组分影响条件下均高于nZVI,因此具有更广泛的应用前景。 相似文献
18.
Initial risk assessment characterization carried out in a tailing pond, called “El Lirio”, came from metal mining showed that these soils have low fertility; low amounts of nitrogen, organic carbon, phosphorous, and carbonates; and high concentrations of total metals (10,719 mg Zn kg?1, 2,821 mg Pb kg?1, and 30 mg Cd kg?1), diethylenetriaminepentaacetic acid (DTPA)-extractable metals, and water-soluble metals, which suggest an urgent need for remediation. Different amendments have been selected, including three anthropogenic wastes: pig manure, sewage sludge, and lime; all were added to the constructed plots in the mine pond. The objectives were to: (1) reduce acid mine drainage, metal mobilization, and toxicity and (2) provide nutrients which enable plant establishment. Results showed an increase in pH, electrical conductivity, total nitrogen, organic carbon, and equivalent calcium carbonate contents. Although water- and DTPA-extractable Zn, Pb, and Cd were reduced, there was an increment in DTPA- and water-extractable Cu due to the addition of organic matter. The amendments also enhanced the establishment of plants. This study constitutes the first stage of a successful remediation programme that can be applied in similar mining areas. The chemical stabilization of metals is a cost-effective alternative for remediation of mine areas in SE Spain. 相似文献