以堇青石蜂窝陶瓷为载体的新型钒氧化物脱氮催化剂研究

以TiO₂/Al₂O₃/堇青石蜂窝陶瓷为载体,以V₂O₅-MoO₃-WO₃为活性组分,用于氨法选择性催化还原烟气中NO的新型催化剂,并对该催化剂的活性性能和微观结构进行了评价和表征.同时,将该催化剂的活性性能与其它几种活性组分相同但载体、制备方法、结构不同的催化剂进行了对比.对比结果表明,该新型催化剂能取得最好的选择性催化还原氮氧化物催化性能BET、FT IR、XPS表征实验结果表明,其高催化活性得益于大比表面积及大孔体积,而TiO₂/Al₂O₃/堇青石蜂窝陶瓷载体及其制备方法对获得好的催化剂构型起了至关重要的作用.     

矿物超细颗粒的形成机制、结构特征及其环境行为和效应

矿物超细颗粒在自然环境中普遍存在,具有独特的环境行为和效应,对元素地球化学循环、污染物迁移转化和生态环境演变等有重要影响.矿物超细颗粒的环境行为和效应与其形成过程和结构特征密切相关.综述了物理、化学和生物过程驱动的矿物超细颗粒的形成机制,介绍了用于表征矿物超细颗粒结构特征的显微镜、光谱、质谱和同步辐射技术,分析了矿物超细颗粒在环境中的迁移转化及其与污染物的吸附、氧化还原和催化转化作用,总结了矿物超细颗粒的食物链积累、生物和生态毒性等环境效应,并对颗粒结晶路径、风险管控和微纳界面调控等重要研究方向进行了展望.超细颗粒是连接微观物质与宏观矿物晶体之间的桥梁,全面认识复杂基质中矿物颗粒的环境属性及其与污染物的微观作用机制,有助于指导矿物超细颗粒在环境污染修复中的应用,从而优化功能材料的设计,促进绿色低碳纳米技术的发展.     

Physico-chemical characterization of Residual Household Waste for energy recovery in insular territories: Case study of Reunion Island

Waste-to-energy is a promising approach to face the current challenge of waste overproduction in Reunion Island, a French territory. In this particular context of an isolated and tropical territory, it is essential to study the properties of potential feedstocks to choose the most appropriate conversion process. This article reports on the composition of Residual Household Waste from Reunion Island and its physico-chemical parameters. Twelve representative samples of Residual Household Waste were subjected to thermal and elemental analysis. The results showed that their composition had a significant influence on the physico-chemical properties, including calorific value. Residual Household Waste from the selective sorting (rich in wood, plastic, and sanitary textiles) as well as dry mixed RHW are the most interesting for energy recovery. Due to their high volatile matter and high carbon content, and their low moisture content, these types of waste have a high calorific value exceeding 18 MJ/kg. Furthermore, the RHW sample comply with the environmental and health criteria applied by French regulations concerning halogen and heavy metal. Thus, it seems that Residual Household Waste can be an alternative to conventional fuels used in incineration or pyro-gasification processes. However, the study also points the need for a pre-treatment process for these wastes. Indeed, it is necessary to sort them correctly in order to avoid the risks of pollution and important maintenance. And more importantly, drying beforehand is unavoidable to improve combustibility and obtain optimal energy conversion.     

蜂窝状Ce/Cr掺杂Cu基催化剂用于乙烷的催化燃烧

以蜂窝堇青石陶瓷为载体,采用浸渍法负载氧化铝涂层和活性组分,制备了蜂窝状Ce/Cr掺杂Cu基催化剂。运用BET,XRD,XPS,H₂-TPR技术对催化剂进行了表征,并对其乙烷催化燃烧活性进行了评价。表征结果显示,Ce/Cr掺杂提高了催化剂表面化学吸附氧的含量,提升了催化剂在较低温度下的氧化还原性能。实验结果表明：在入口乙烷质量浓度2 000 mg/m³、反应空速20 000 h^-1的条件下,Cu-Ce催化剂较Cu催化剂的T₅₀和T₉₀（乙烷转化率为50%和90%时的反应温度）分别降低了46 ℃和101 ℃,降幅高于Cu-Cr催化剂的38 ℃和78 ℃;较高反应空速（30 000 h^-1）对催化反应不利,乙烷浓度对催化剂活性的影响不明显;550 ℃下Cu-Ce催化剂对乙烷的转化率100 h内保持在99%以上,表现出良好的稳定性。     

Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive brilliant blue

A study of the decolorization of reactive brilliant blue in an aqueous solution using Fe-Mn-sepiolite as a heterogeneous Fenton-like catalyst has been performed. The Fourier transform infrared (FTIR) spectra of the catalyst showed bending vibrations of the Fe-O. The X-ray diffraction (XRD) patterns of the catalyst showed characteristic diffraction peaks of α-Fe₂O₃, γ-Fe₂O₃ and MnO. A four factor central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables (catalyst addition, hydrogen peroxide dosage, initial pH value and initial dye concentration). When the reaction conditions were catalyst dosage= 0.4 g, [H₂O₂]= 0.3 mL, pH= 2.5, [reactive brilliant blue]_o = 50 mg·L⁻¹, and volume of solution= 500 mL at room temperature, the decolorization efficiency of reactive brilliant blue was 91.98% within 60 min. Moreover, the Fe-Mn-sepiolite catalyst had good stability for the degradation of reactive brilliant blue even after six cycles. Leaching of iron ions (<0.4 mg·L⁻¹) was observed. The decoloring process was reactive brilliant blue specific via a redox reaction. The benzene ring and naphthalene ring were first oxidized to open ring; these were then oxidized to the alcohol and carboxylic acid. The reactive brilliant blue was decomposed mainly by the attack of ·OH radicals including surface-bound ·OH radicals generated on the catalyst surface.     

Chemical poison and regeneration of SCR catalysts for NOx removal from stationary sources

Selective catalytic reduction (SCR) of NO_x with NH₃ is an effective technique to remove NO_x from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V₂O₅-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO₂ and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.     

复合金属氧化物Cu-Co-Al低温催化水解HCN

采用共沉淀法制备了Cu-Al、Co-Al和Cu-Co-Al复合金属氧化物催化剂,考察了3种催化剂对HCN的催化水解性能,并通过XRD、BET、XPS和H2-TPR等对催化剂的结构和性能进行表征.结果表明, Cu-Co-Al催化剂展示最高的催化活性. 反应温度200℃,反应180min后, Cu-Co-Al、Cu-Al和Co-Al催化剂对HCN的转化率分别为95%,90%,10%;NH3生成量分别为122,118,18mg/m3.低结晶度、高分散性、高比表面积的催化剂有利于低温HCN水解.适量的表面分子氧含量、较高的Cu2+和Co3+含量、较低的还原温度是Cu-Co-Al催化剂具有较高的HCN低温水解活性的主要原因.     

DOC+CDPF对生物柴油燃烧颗粒排放特性的影响

以一台满足国五排放法规的车用柴油机为样机,研究加装氧化催化转化器DOC与催化型颗粒捕集器CDPF(DOC+CDPF后处理装置)前后,柴油机燃用B20燃料(燃料含20%体积掺混比的生物柴油)的颗粒排放特性.结果表明,在未加装该后处理装置时,该机排气颗粒数量浓度的粒径分布呈双峰形态,B20燃料的排气颗粒数量浓度的峰值粒径在10nm和50nm附近,纯柴油的排气颗粒数量浓度的峰值粒径在50nm和200nm附近.在颗粒粒径小于120nm的区域,该机燃用B20燃料的排气颗粒数量浓度大于纯柴油.加装该后处理装置后,该机排气颗粒数量浓度的粒径分布呈多峰形态,峰值粒径在10nm、20nm和60nm附近.加装DOC+CDPF后,不论是柴油还是B20燃料,与原机相比,柴油机排气颗粒总数量下降明显,其中60~200nm粒径范围的颗粒数量浓度降幅更为显著.在相同工况下,DOC+CDPF对柴油机燃用B20燃料的颗粒总数量净化效率高于纯柴油.     

Optimizing synthesis conditions of nanoscale zero-valent iron (nZVI) through aqueous reactivity assessment

Nanoscale iron particles (nZVI) is one of the most important engineered nanomaterials applied to environmental pollution control and abatement. Although a multitude of synthesis approaches have been proposed, a facile method to screen the reactivity of candidate nZVI materials produced using different methods or under varying synthesis conditions has yet been established. In this study, four reaction parameters were adjusted in the preparation of borohydride-reduced nZVI. The reductive properties of the resultant nanoparticles were assayed independently using two model aqueous contaminants, Cu(II) and nitrate. The results confirm that the reductive reactivity of nZVI is most sensitive to the initial concentration of iron precursor, borohydride feed rate, and the loading ratio of borohydride to ferric ion during particle synthesis. Solution mixing speed, in contrast, carries a relative small weight on the reactivity of nZVI. The two probing reactions (i.e., Cu(II) and nitrate reduction) are able to generate consistent and quantitative inference about the mass-normalized surface activity of nZVI. However, the nitrate assay is valid in dilute aqueous solutions only (50 mg·L⁻¹ or lower) due to accelerated deactivation of iron surface at elevated nitrate concentrations. Additional insights including the structural and chemical makeup of nZVI can be garnered from Cu(II) reduction assessments. The reactivity assays investigated in this study can facilitate screening of candidate materials or optimization of nZVI production parameters, which complement some of the more sophisticated but less chemically specific material characterization methods used in the nZVI research.     

铁基催化剂的微波水热处理对其SCR脱硝性能的影响

利用微波对共沉淀制备的铁铈钛复合氧化物催化剂前驱体进行水热处理,探讨了微波水热处理对铁基催化剂低温SCR脱硝性能的优化;并对微波水热处理条件的影响进行了正交分析.结果表明:对铁基催化剂前驱体进行微波水热处理,可提高其低温SCR脱硝性能,使其脱硝温度窗口向低温偏移;且微波水热处理的低温优化效果与催化剂中Fe/Ti摩尔比密切相关,Fe/Ti摩尔比越小,微波水热处理的低温优化越强;微波加热方式和微波辐射时间会影响微波水热处理对铁基催化剂SCR脱硝性能的低温优化;在相同微波辐射时间条件下,当P30逐渐变为P80,微波水热处理对铁基催化剂低温SCR脱硝的促进作用降低;在P30条件下,微波辐射15min使铁基催化剂具有最佳低温SCR脱硝活性.