有机污染物湿式氧化降解中Cu系列催化剂的稳定性

在 0.5L高压釜中采用自制 Cu系列催化剂在温度 150～ 230℃和氧分压 3.0 MPa反应条件下对染料中间体 H-酸配水进行催化湿式氧化反应 ,着重研究了非均相 Cu催化剂在催化湿式氧化过程中的稳定性问题 ,发现酸性溶出和反应性溶出是导致Cu列系催化剂不稳定的主要原因 .分别针对溶出原因 ,从改变反应条件 ,优化催化剂的设计和制备等方面进行了控制 ²⁺溶出的试验研究 ,指出克服 Cu²⁺溶出问题是规模化实际应用的关键 .     

An inventory of trace element inputs to agricultural soils in China

It is important to understand the status and extent of soil contamination with trace elements to make sustainable management strategies for agricultural soils. The inputs of trace elements to agricultural soils via atmospheric deposition, livestock manures, fertilizers and agrochemicals, sewage irrigation and sewage sludge in China were analyzed and an annual inventory of trace element inputs was developed. The results showed that atmospheric deposition was responsible for 43–85% of the total As, Cr, Hg, Ni and Pb inputs, while livestock manures accounted for approximately 55%, 69% and 51% of the total Cd, Cu and Zn inputs, respectively. Among the elements concerned, Cd was a top priority in agricultural soils in China, with an average input rate of 0.004 mg/kg/yr in the plough layer (0–20 cm). Due to the spatial and temporal heterogeneity of the sources, the inventory as well as the environmental risks of trace elements in soils varies on a regional scale. For example, sewage sludge and fertilizers (mainly organic and phosphate-based inorganic fertilizers) can also be the predominant sources of trace elements where these materials were excessively applied. This work provides baseline information to develop policies to control and reduce toxic element inputs to and accumulation in agricultural soils.     

叶菜类蔬菜对海藻碘的吸收与积累特征

以叶菜类蔬菜菠菜、大白菜、生菜、香菜、芥菜和雪菜为研究对象,利用海藻固体碘肥和海藻液体碘肥作为外源碘,在露天和大棚栽培条件下进行蔬菜植物碘强化的田间试验,通过分析蔬菜对碘吸收量的动态变化和碘在蔬菜各器官的分布和分配状况,研究了叶菜类蔬菜对外源碘的吸收与积累特征.结果表明,供试叶菜可食部分中碘的含量随着外源碘添加量的增加而增加;随着取样时间的延后,叶菜可食部分中碘的含量呈现出下降的趋势;喷施液体碘肥比土施固体碘肥更有利于叶菜对碘的吸收和积累,前者使吸收的碘大部分积累在叶面,后者则大部分积累在根部.     

Enhanced dechlorination of 2,4-dichlorophenol by recoverable Ni/Fe–Fe3O4 nanocomposites

Ni/Fe-Fe_3O_4 nanocomposites were synthesized for dechlorination of 2,4-dichlorophenol(2,4-DCP). The effects of the Ni content in Ni/Fe-Fe_3O_4 nanocomposites, solution pH, and common dissolved ions on the dechlorination efficiency were investigated, in addition to the reusability of the nanocomposites. The results showed that increasing content of Ni in Ni/Fe–Fe_3O_4 nanocomposites, from 1 to 5 wt.%, greatly increased the dechlorination efficiency; the Ni/Fe–Fe_3O_4 nanocomposites had much higher dechlorination efficiency than bare Ni/Fe nanoparticles. Ni content of 5 wt.% and initial p H below 6.0 was found to be the optimal conditions for the catalytic dechlorination of 2,4-DCP. Both 2,4-DCP and the intermediate product 2-chlorophenol(2-CP) were completely removed, and the concentration of the final product phenol was close to the theoretical phenol production from complete dechlorination of 20 mg/L of 2,4-DCP, after 3 hr reaction at initial p H value of 6.0,3 g/L Ni/Fe-Fe_3O_4 , 5 wt.% Ni content in the composite, and temperature of 22℃. 2,4-DCP dechlorination was enhanced by Cl-and inhibited by NO3-and SO_4~(2-). The nanocomposites were easily separated from the solution by an applied magnetic field. When the catalyst was reused, the removal efficiency of 2,4-DCP was almost 100% for the first seven uses, and gradually decreased to 75% in cycles 8–10. Therefore, the Ni/Fe–Fe_3O_4 nanocomposites can be considered as a potentially effective tool for remediation of pollution by 2,4-DCP.     

Use of catalytic wet air oxidation (CWAO) for pretreatment of high-salinity high-organic wastewater

Catalytic wet air oxidation (CWAO) coupled desalination technology provides a possibility for the effective and economic degradation of high salinity and high organic wastewater. Chloride widely occurs in natural and wastewaters, and its high content jeopardizes the efficacy of Advanced oxidation process (AOPs). Thus, a novel chlorine ion resistant catalyst B-site Ru doped LaFe_1-xRu_xO_3-δ in CWAO treatment of chlorine ion wastewater was examined. Especially, LaFe_0.85Ru_0.15O_3-δ was 45.5% better than that of the 6%RuO₂@TiO₂ (commercial carrier) on total organic carbon (TOC) removal. Also, doped catalysts LaFe_1-xRu_xO_3-δ showed better activity than supported catalysts RuO₂@LaFeO₃ and RuO₂@TiO₂ with the same Ru content. Moreover, LaFe_0.85Ru_0.15O_3-δ has novel chlorine ion resistance no matter the concentration of Cl⁻ and no Ru dissolves after the reaction. X-ray diffraction (XRD) refinement, X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), and X-ray absorption fine structure (XAFS) measurements verified the structure of LaFe_0.85Ru_0.15O_3-δ. Kinetic data and density functional theory (DFT) proved that Fe is the site of acetic acid oxidation and adsorption of chloride ions. The existence of Fe in LaFe_0.85Ru_0.15O_3-δ could adsorb chlorine ion (catalytic activity inhibitor), which can protect the Ru site and other active oxygen species to exert catalytic activity. This work is essential for the development of chloride-resistant catalyst in CWAO.

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