高岭土负载纳米铁在含水层的运移行为及重金属污染修复效能研究

为克服重金属污染物修复过程中纳米零价铁易氧化、团聚等缺陷,本研究将其负载于高岭土表面合成负载型纳米零价铁复合材料（K-nZVI）,并利用批次试验、沉降试验及模拟柱试验研究了K-nZVI在含水层中的运移行为及其对地下水重金属污染的修复效能.结果表明,K-nZVI对Pb、Cu、Cd均有很好的去除效果,去除率随着初始浓度的增加、反应温度的升高、反应时间的延长而升高,且在弱碱性条件下修复效果最好.此外,K-nZVI在含水层中表现出较好的分散和稳定性能,运移行为可通过一维对流-弥散-沉积模型描述,其运移能力随着初始浓度的增加、砂颗粒粒径的减小、地下水流速的降低和离子浓度的升高而逐渐减弱.     

Efficient nitrogen doped porous carbonaceous CO2 adsorbents based on lotus leaf

In this work, the waste biomass lotus leaf was converted into N-doped porous carbonaceous CO₂ adsorbents. The synthesis process includes carbonization of lotus leaf, melamine post-treatment and KOH activation. For the resultant sorbents, high nitrogen content can be contained due to the melamine modification and advanced porous structure were formed by KOH etching. These samples were carefully characterized by different techniques and their CO₂ adsorption properties were investigated in detail. These sorbents hold good CO₂ adsorption abilities, up to 3.87 and 5.89 mmol/g at 25 and 0°C under 1 bar, respectively. By thorough investigation, the combined interplay of N content and narrow microporous volume was found to be responsible for the CO₂ uptake for this series of sorbents. Together with the high CO₂ adsorption abilities, these carbons also display excellent reversibility, high CO₂/N₂ selectivity, applicable heat of adsorption, fast CO₂ adsorption kinetics and good dynamic CO₂ adsorption capacity. This study reveals a universal method of obtaining N-doped porous carbonaceous sorbents from leaves. The low cost of raw materials accompanied by easy synthesis procedure disclose the enormous potential of leaves-based carbons in CO₂ capture as well as many other applications.     

以淀粉为模板多孔纳米氧化铈的制备及其催化性能研究

为获得多孔纳米CeO₂（氧化铈）,以淀粉为生物模板,以Ce（NO₃）₃·6H₂O为铈源,在温和条件下制备出海绵状的多孔纳米CeO₂,同时考察了焙烧温度、碱液、铈源投加量对样品形貌的影响.利用XRD（X射线衍射光谱）、SEM（扫描电镜）、N₂吸附-脱附等表征手段对合成的多孔纳米CeO₂进行物相组成、微观形貌及孔径大小分布的分析.通过湿式催化过氧化试验,探究其对腈纶废水中有机物COD_Cr的催化降解性能.结果表明:①所制备的多孔纳米CeO₂具有多孔结构,孔径分布范围为2~4 nm,孔容为0.225 cm3/g,BET比表面积为256.426 m2/g;②多孔纳米CeO₂的最佳制备条件为1 g淀粉溶解于20 mL水中,加入0.02 mol Ce（NO₃）₃·6H₂O,以5%的氨水调节前驱体混合液pH,以1℃/min升至400℃,焙烧4 h,得到海绵状的多孔纳米CeO₂.③以不同形貌的CeO₂作为湿式催化反应中的催化剂,催化降解腈纶废水中有机物,其中以制备的多孔纳米CeO₂催化性能最佳,COD_Cr去除率可达82.5%.研究显示,焙烧温度、碱液、铈源投加量均可影响样品的形貌,在湿式催化过氧化处理腈纶废水试验中,多孔纳米CeO₂能显著提高废水COD_Cr的去除率.      

Analytical solutions of three-dimensional contaminant transport in uniform flow field in porous media: A library

The purpose of this study is to present a library of analytical solutions for the three-dimensional contaminant transport in uniform flow field in porous media with the first-order decay, linear sorption, and zero-order production. The library is constructed using Green’s function method (GFM) in combination with available solutions. The library covers a wide range of solutions for various conditions. The aquifer can be vertically finite, semi-infinitive or infinitive, and laterally semi-infinitive or infinitive. The geometry of the sources can be of point, line, plane or volumetric body; and the source release can be continuous, instantaneous, or by following a given function over time. Dimensionless forms of the solutions are also proposed. A computer code FlowCAS is developed to calculate the solutions. Calculated results demonstrate the correctness of the presented solutions. The library is widely applicable to solve contaminant transport problems of one- or multiple- dimensions in uniform flow fields.     

硅藻土基多孔吸附填料的制备及其对Pb2+的吸附

以硅藻土为主要原料,添加超细碳粉、烧结助剂和粘结剂,按一定比例混合、搅拌、造粒,在设定程序下煅烧,制备了硅藻土基多孔吸附填料(DBPAF),探讨了烧成温度、造孔剂添加量、硅藻土粉体粒径对DBPAF孔隙特征的影响,运用扫描电子显微镜(SEM)和X射线衍射仪(XRD)对DBPAF的微观形貌和物相组成进行了观察和分析,采用动态吸附实验研究了DBPAF的可操作性,采用静态吸附实验研究了DBPAF吸附Pb2+的性能和机制.结果表明,最适烧成温度范围为900~1000℃,最适造孔剂添加量为7.0%,最适硅藻土粉体粒径为2.40μm;与硅藻土原土(粉体)相比,DBPAF的可操作性明显提高,孔隙结构得到了明显改善,物相组成以方石英相为主.研究还表明,烧制过程升温速率以2~5℃/min为宜以保证DBPAF气孔分布均匀;DBPAF对Pb2+吸附容量较硅藻土原土(粉体)提高了78.0%,吸附过程速率控制步骤为Pb2+与DBPAF孔道内的基团发生的化学反应,吸附动力学符合拟二级动力学模型.     

露天堆场防风抑尘网后湍流结构及抑尘效率的数值模拟

建立了开放性露天堆场周围空气流动的三维数学物理模型,选择应用标准k-ε紊流模型进行了静态流场的数值模拟;分析了典型棱形堆迎风面、平顶面和背风面周围空气的湍流结构和表面受力特性;基于流场数据揭示了防风抑尘网不同孔隙率下空气动力学结构的分布规律.结果显示:物料堆平顶面剪切力随孔隙率增大而增大;料堆迎风面在孔隙率较小时出现局部涡流,表面剪切力方向向下,孔隙率较大时,网后空气垂直方向压差作用显著,表面剪切力方向向上;背风面始终处于回流区,表面剪切力和回流点数随孔隙率大小变化不显著.综合流场结构和受力分布可得最佳孔隙率为0.2~0.4.该研究中对物料堆逐个表面进行空气动力学模拟可以避免由于剪切力方向不同产生矢量抵消而带来的计算失真.     

露天堆场防风抑尘网的动力学数值模拟

开放性露天堆场的散尘是大气颗粒物的重要来源. 来流空气在棱形物料堆的上部绕流,使其表面的空气流动结构逐点不同,而料堆表面的空气动力学结构又决定着堆场的散尘机理及散尘量. 分析了典型单一棱形料堆周围空气湍流结构,并应用三维标准k-ε紊流模型对其流场进行了数值模拟;计算了来流方向抑尘网前后不同断面处风速的垂直分布;分析了不同孔隙率(0、0.2、0.3、0.4、0.5、0.6和1.0)抑尘网后料堆迎风面和背风面沿高度方向、平顶面沿水平方向的剪切应力特性和分布规律. 结果表明:抑尘网前3倍网高距离处的风速较无网工况(孔隙率为1.0)略有减小,降幅随孔隙率增大而减小, 孔隙率为0时最大降幅为5.1%;网前2倍网高距离处与抑尘网之间区域的风速廓线与无网工况相差甚远,孔隙率为0时近网区域风速最高降幅达92.8%. 抑尘网和料堆迎风面之间区域,从地面至网顶高度,不同孔隙率抑尘网工况下的风速均较无网工况小,最小处为无网工况风速的18.5%;抑尘网以上区域的风速较无网工况的大,最大处为无网工况风速的128.0%,并且差距随抑尘网孔隙率的减小而增大. 料堆剪切力分布显示,其迎风面和平顶面为主要散尘面,背风面被涡旋卷起的扬尘量较前两者小得多. 防风抑尘网的设置改变了料堆周围空气的流动结构和受力分布,对不同孔隙率的抑尘网数值模拟结果可知,0.2和0.3为最佳孔隙率.      

聚烯丙基氯化铵调控的中空多孔磷酸八钙超结构及其对Pb(Ⅱ)的吸附特性

环境友好、价格低廉且易于批量化生产的矿物基吸附剂在环境污染物去除方面越来越显现出其优越性,但以往的研究多集中于晶相的矿物吸附剂,有关亚稳相的研究相对较少.因此,本文通过仿生矿化的方法,以聚烯丙基氯化铵（PAH）作为生长调节剂,在气相扩散过程中成功制备了由超薄纳米片构筑的中空、多孔磷酸八钙（Octacalcium Phosphate,OCP）微球.结果发现,制备的吸附剂具有较高的比表面积和孔隙率,且高分辨电镜图片显示其具有一定的非晶纳米区域,并对重金属离子Pb（II）表现出优越的吸附特性.吸附实验证明,OCP/PAH对Pb（Ⅱ）的吸附符合Langmuir等温吸附模型和准二级吸附动力学模型,最高吸附量可达1644.74 mg·g^-1.该亚稳相矿物吸附剂出色的重金属吸附性能,为开发新型矿物吸附剂提供了新思路.     

泡沫强化多孔介质中纳米零价铁迁移试验

通过批量模拟试验考察了纳米零价铁(NZVI)在水、十二烷基硫酸钠(SDS)溶液与SDS泡沫3种流体中的沉降性能,以及3种流体输送作用下NZVI在多孔介质中的迁移分布特性.结果表明:NZVI在SDS溶液中的稳定性远大于其在水中的稳定性;搅拌速度为3000r/ min时,NZVI在泡沫中的分布较均匀且泡沫对NZVI携带量较大;NZVI对泡沫稳定性影响不大.水、SDS溶液、SDS泡沫分别作为输送流体时,NZVI迁移的最大距离分别为0.8m,7.9m和2.1m,SDS溶液和泡沫均显著促进了其在多孔介质中的运移.当NZVI由SDS溶液和泡沫输送时,其在介质中的分布范围(33.5%和42.5%)大于水(12.8%);由于重力作用,SDS溶液携带NZVI的迁移主要集中在垂向上,水平迁移能力有限;而泡沫受重力影响较小,其携带的NZVI在水平和垂直方向上的分布更为均匀.可见泡沫作为NZVI的输送流体具有明显优势.     

Tetracycline removal via adsorption and metal-free catalysis with 3D macroscopic N-doped porous carbon nanosheets: Non-radical mechanism and degradation pathway

Recently, metal-based carbon materials have been verified to be an effective persulfate activator, but secondary pollution caused by metal leaching is inevitable. Hence, a green metalfree 3D macroscopic N-doped porous carbon nanosheets（NPCN） was synthesized successfully. The obtained NPCN showed high adsorption capacity of tetracycline（TC） and excellent persulfate（PS） activation ability, especially when calcined at 700 °C（NPCN-700）. The maximum adsorption capacity of NPCN-700 was 121.51 mg/g by ...