碳氮结构空心管材料及其对钍离子的吸附性能研究

目的合成碳氮结构空心管材料,用于稀土矿山开采中放射性钍离子的吸附去除,方法通过三聚氰胺和三聚氰酸超分子自组装,经水热碳化及高温热解,制备碳氮结构空心管材料.采用SEM、XRD等对材料进行表征.在不同热解温度和pH值下进行钍离子吸附实验,比较不同钍离子的初始浓度和吸附时间下吸附容量的差异.结果600℃时,材料形貌为均匀的中空管状结构;pH=3.5,热解温度为800℃时,材料最大吸附容量达到133.87 mg/g,吸附过程符合Langmuir等温吸附模型且遵从准二级动力学规律.结论碳氮结构空心管材料对钍离子具有良好的吸附效果,有望用于稀土开采过程中产生的放射性废钍离子的去除.     

Significance of platinum group metals emitted from automobile exhaust gas converters for the biosphere

Intention, Goal, Scope, Background  Following the introduction of automobile catalytic converters the platinum group metals (PGM) platinum (Pt), palladium (Pd) and rhodium (Rh) gain on increasing interest in environmental research as these metals are emitted with exhaust fumes into the environment. Consequently, elevated PGM levels were found in different environmental matrices uch as road dusts, soils along heavily frequented roads, sediments of urban rivers etc. Accordingly, the effects of increasing PGM emissions on the biosphere are controversially discussed. Objective  This paper summarizes the present knowledge on the biological availability of PGM to plants and animals. As biological availability is one of the most decisive factors determining the toxicologi-cal potential of xenobiotics, this information is very important to evaluate the possible threat of the noble metals to ecosystems. Results and Discussion  The availability of soluble as well as particle bound PGM to terrestrial plants was demonstrated in several studies. Experimental investigations revealed uptake of Pt, Pd and Rh also by aquatic plants. Additionally, the biological availability of the noble metals for animals has been verified in experimental studies using soluble metal salts, catalytic converter model substances, sediments of urban rivers, road dust or tunnel dust as metal sources. These studies refer mainly to aquatic animals. Beside of free living organisms, in particular worms parasitizing fish demonstrated a high potential to accumulate PGM. This could be of great interest in respect of biomonitoring purposes. Generally, for plants as well as for animals Pd turns out to be the best available metal among the PGM. Compared to other heavy metals, the biological availability of PGM from road dust to zebra mussels(Dreissena polymorpha) ranged between that of Cd and Pb. Conclusion  Especially chronic effects of PGM on the biosphere can not be excluded due to (1) their cumulative increase in the environment, (2) their unexpected high biological availability and bioaccumulation and (3) their unknown toxicological and ecotoxicological potential. However, it appears that acute effects on ecosystems due to anthropogenic PGM emission are not likely. Recommendation and Outlook  Research on environmental PGM contamination of the biosphere, especially the fauna, and on long-term toxiciry of low PGM concentrations is highly appreciated. These studies require very sensitive analytical techniques to determine PGM even in low sample amounts. Research has to be done in particular on reliable determination of (ultra) trace levels of Pd and Rh as the lack of data on these two metals is mainly due to analytical problems.     

制备方法对MgAl水滑石衍生氧化物负载钯催化剂丙烷完全氧化活性的影响

以沉积沉淀法(DP)、浸渍法(IM)和共沉淀法(CP)制备MgAl水滑石衍生氧化物负载钯催化剂,用ICP、XRD、SEM、TEM、EDS、TPR以及比表面测定等手段对催化剂进行了表征.ICP和XRD数据表明用上述3种方法均可成功制备水滑石为前体载钯催化剂.SEM、TEM、EDS数据表明不同方法制备的样品具有不同的形貌以及钯在其中的分散度.综合各类表征数据可知Pd在催化剂中暴露的活性位是影响其活性的主要因素.     

CeO2负载型双金属Pd/Fe催化还原四氯化碳的实验研究

实验采用共沉淀法制得CeO_2负载型双金属Pd/Fe催化剂,并对催化剂的结构特征进行了X射线衍射(XRD)和扫描电子显微镜(SEM)分析.使用负载型双金属催化剂对四氯化碳进行还原脱氯研究,探究了温度、溶液初始pH值、催化剂投加量及不同钯载率对四氯化碳脱氯的影响;对比了不同催化剂包括纳米零价铁、纳米钯铁双金属和CeO_2负载型双金属Pd/Fe对四氯化碳的脱氯效果.实验结果表明负载型双金属催化剂在温度为40℃,溶液初始pH为6.5,催化剂投加量为0.4 g·L-1,钯载率为0.5%的条件下,对初始浓度为5 mg·L-1的四氯化碳的去除率高达99.88%.在相同的反应条件下,纳米零价铁和纳米钯铁双金属对四氯化碳的脱氯率分别为58.25%、87.94%.此外,对四氯化碳的脱氯机制进行了探讨.     

Fe(Ⅲ)掺杂Mg/Al-LDO作为氮磷吸附剂的研究

针对污水厂尾水脱氮除磷问题,采用共沉淀法制备了镁铝铁类水滑石（Mg/Al/Fe–LDHs）,在450℃下焙烧3h得到焙烧态类水滑石（Mg/Al/Fe–LDO）.研究了Fe（Ⅲ）掺杂对Mg/Al-LDO吸附氮磷的影响及吸附特性.结果表明,当Mg/Al/Fe物质的量比为3：0.6：0.4时,Mg/Al/Fe-LDO对氮磷吸附性能较好,最大吸附容量分别为28.57mg/g和231.46mg/g.吸附过程均符合Langmuir吸附等温模型,拟合相关系数（R²）达到0.99以上.根据XRD、FTIR的表征结果可以推断,Mg/Al/Fe–LDO是通过“记忆效应”、静电引力作用完成对氮磷的吸附,对磷的吸附还包括离子交换作用.     

掺钴水钠锰矿对铅的吸附及对砷的氧化

为了研究过渡金属离子掺杂对锰氧化物作为环境友好材料物理化学性质的影响,在浓盐酸还原高锰酸钾制备水钠锰矿过程中添加氯化钴,在常压回流条件下一步合成了三维纳米微球状水钠锰矿,考察了其铅吸附和砷氧化能力.应用粉晶X射线衍射、化学分析、N2物理吸附、场发射扫描电镜（FE-SEM）、X射线光电子能谱（XPS）等手段表征产物晶体结...     

城市环境铂族金属分布特性及生态健康风险研究进展

随着铂族金属铂（Pt）、钯（Pd）、铑（Rh）被广泛应用于汽车尾气催化净化器中,这三种金属在自然界中的含量逐渐升高。越来越多的研究表明,这几种曾被认为对环境影响较小的金属的确会带来潜在的生态健康风险。本文概括了国内外城市各种环境介质的含量分布,重点分析了铂族金属的源解析方法、粒径分布特性、影响其排放的因素和其潜在的生态健康风险。就全世界的城市来看,灰尘、空气、土壤、沉积物等各种环境介质中铂族金属的含量均有显著提高,主要来源于汽车三元催化净化器。这三种金属倾向于富集在细颗粒中,行车模式是影响其排放量的重要因素,自然界的共存物质可增强它们的溶解性和迁移性,从而使它们的生物可利用性大大提高。生物体吸收这类金属后,可与体内的物质发生反应,形态发生变化,毒性增强。在以后的研究中,除了持续跟踪调查这三种金属在环境中的含量水平以外,还应加强研究这三种金属在环境中的颗粒分布、迁移转化、形态变换、生物可利用性以及生物毒性等,使我们能够更好地评估其生态健康风险,并为与之相关的应用研发、防范措施、政策制订提供引导和支持。     

负载型纳米Fe-Pd降解水溶性偶氮染料

采用阳离子交换树脂表面为载体,合成了负载型纳米Fe-Pd二元复合金属材料,采用扫描电子显微镜(SEM)和能谱分析对该材料进行表征,研究了其对一些水溶性偶氮染料的降解效果.实验表明,该材料对0.05 g.L-1甲基橙、日落黄、酸性橙8、金橙G和活性红2等偶氮染料有较好的降解效果,纳米双金属中Pd含量的增加有利于染料的降解;反应体系初始pH值对染料的降解率影响较大,本研究中,pH 4酸性条件下降解效果最佳;制备的材料在第10次活化后,仍有较好的降解效果;为环境中偶氮染料的降解提供了一种有效的方法.     

Semi-closed synthesis of nitrogen and oxygen Co-doped mesoporous carbon for selective aqueous oxidation

Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors, hard/soft templates, and heteroatom-containing agents. Herein, we report a facile synthesis of N and O co-doped meso/micro-porous carbon (NOMC) by template-free carbonization of a small-molecule precursor in a semi-closed system. The semi-closed carbonizaiton process yields hydrophilic NOMCs with large surface area in a high yield. The porous structure as well as the elemental composition of NOMCs can be modulated by changing the holding time at a particular temperature. NOMCs as metal-free heterogeneous catalysts can selectively oxidize benzyl alcohol and its derivatives into aldehydes/ketones with>85％conversion in aqueous solution, which is much higher than that of the control sample obtained in tube furnace (21％conversion), mainly due to their high N content, high percentage of pyridinic N, and large surface area. The presence of O-containing moieties also helps to improve the hydrophilicity and dispersion ability of catalysts and thus facilitates the mass transfer process during aqueous oxidation. The NOMC catalysts also dispayed excellent activity for a wide range of substrates with a selectivity of>99％.     

Propane oxidation and steam reforming over Pd/LaFe(0.8) Co(0.2) O3 catalyst: effects of the reactant composition and steam

The effects of reactant composition and steam on propane combustion over Pd/LaFe0.8Co0.2O3 catalyst were investigated.Propane conversion and the oxidation state of palladium were strongly affected by the redox ration of reactants.Higher propane conversion could be obtained under rich conditions and explained as a complex balance between oxidation and steam reforming.Water produced in the oxidation could promote the propane conversion by steam reforming.However,the presence of excess steam would bring about inhibition.