Cu／A1-Ce-PILC在丙烯选择性催化还原NO反应中的失活研究

采用聚合羟基复合阳离子合成交联黏土A1-Ce-PILC，经SO4^2-改性后，以浸渍法制备了铜基交联黏土催化剂Cu／A1-Ce-PILC，并将其应用于C3H6选择性催化还原NO的反应，350℃时NO转化率达到最大值56％，700℃时下降至22％．为探究催化剂高温失活的原因，采用XPS、TPR、TGA、Py-IR和DSC对反应前后催化剂的物化性能进行了表征．结果表明，经过H2预处理活化后活性组分Cu物种以Cu^＋形式存在，而高温反应后Cu物种除以Cu^＋和Cu^2＋ 2种形式存在外，还出现了少量CuO物种；高温反应过程中A1-Ce-PILC上结构羟基和SO4^2-流失导致催化剂表面酸性减弱；此外，还存在表面积炭覆盖了部分活性中心并堵塞了催化剂孔道的现象．这三者的共同影响促进了C3H6深度氧化，抑制了NO还原，从而导致催化剂的失活．     

Promotional effect of cobalt doping on catalytic performance of cryptomelane-type manganese oxide in toluene oxidation

The cryptomelane-type manganese oxide (OMS-2)-supported Co (xCo/OMS-2; x = 5, 10, and 15 wt.%) catalysts were prepared via a pre-incorporation route. The as-prepared materials were used as catalysts for catalytic oxidation of toluene (2000 ppmV). Physical and chemical properties of the catalysts were measured using the X-ray diffraction (XRD), Fourier transform infrared spectroscopic (FT-IR), scanning electron microscopic (SEM), X-ray photoelectron spectroscopy (XPS), and hydrogen temperature-programmed reduction (H₂-TPR) techniques. Among all of the catalysts, 10Co/OMS-2 performed the best, with the T_90%, specific reaction rate at 245°C, and turnover frequency at 245°C (TOF_Co) being 245°C, 1.23 × 10⁻³ mol_toluene/(g_cat·sec), and 11.58 × 10⁻³ sec⁻¹ for toluene oxidation at a space velocity of 60,000 mL/(g·hr), respectively. The excellent catalytic performance of 10Co/OMS-2 were due to more oxygen vacancies, enhanced redox ability and oxygen mobility, and strong synergistic effect between Co species and OMS-2 support. Moreover, in the presence of poisoning gases CO₂, SO₂ or NH₃, the activity of 10Co/OMS-2 decreased for the carbonate, sulfate and ammonia species covered the active sites and oxygen vacancies, respectively. After the activation treatment, the catalytic activity was partly recovered. The good low-temperature reducibility of 10Co/OMS-2 could also facilitate the redox process accompanied by the consecutive electron transfer between the adsorbed O₂ and the cobalt or manganese ions. In the oxidation process of toluene, the benzoic and aldehydic intermediates were first generated, which were further oxidized to the benzoate intermediate that were eventually converted into H₂O and CO₂.     

南昌市环境空气质量分析和控制

利用多年的环境监测数据,分析南昌市环境空气中主要污染物尘类、二氧化硫和氮氧化物产生的原因,并提出有效控制上述污染物的具体措施。     

A new approach for modelling potential effects in cation adsorption onto binary (hydr) oxides

The current approach for modelling ion adsorption onto binary (hydr)oxides using homogeneous surface complexation models involves the assumption of either an ideal mixture of the two surfaces (i.e. two surface sites on one surface) or a patchwise surface (i.e. two surfaces with one surface site on each surface). As the physical truth should be between these two limiting cases, a model which assumes a patchwise surface constituted of three patches is proposed. Two patches represent the distinct (hydr)oxides, and the third one a mixture of these distinct (hydr)oxides. Using the diffuse layer model, the three approaches are applied to literature data for Cd adsorption onto binary mixtures of alumina-coated silica at total constant Cd concentration and varying amounts of alumina coatings. For Cd adsorption onto these binary (hydr)oxide systems, the new approach explains the observed potential effects. The proposed model, which contains two additional adjustable parameters in terms of site concentrations or one adjustable parameter in terms of specific surface area, is more successful than the two limiting cases. The new model is then validated by predicting Ca and Zn behaviour on the same binary (hydr)oxide system.     

生物法处理NOx废气的研究进展

氮氧化物 (NOx)是主要的大气污染物之一 ,是治理大气污染的一大难题。对当前国内外生物处理NOx 的研究现状进行了系统的论述 ,介绍了生物过滤法处理氮氧化物的基本原理 ,分析了生物过滤法处理氮氧化物存在的问题 ,并预测该技术的未来发展趋势     

烟气脱硫过程锰催化氧化亚硫酸钙的研究

利用直径280 mm、高320 mm的间歇式搅拌槽,在MnSO4加入浓度为0～0.05 mol/L的情况下,对亚硫酸钙悬浮液进行了催化氧化实验研究.实验结果表明,锰离子的加入会改变亚硫酸钙的氧化机理及氧化过程,表现为终点氧化率和氧化速率的变化.当Mn2 浓度为0.05 mol/L时,亚硫酸钙的终点氧化率比未加入Mn2 时高30%;此外,与非催化反应过程相比,Mn2 的加入能使亚硫酸钙在一个更宽的浓度范围内(0.02～0.073 mol/L)和一个更宽的时间范围内(20～100 min)均保持较高的氧化速率水平.     

Pt/Mg-Ce-O catalyst for NO/H<Subscript>2</Subscript>/O<Subscript>2</Subscript> lean de-No<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> reaction

The NO/H₂/O₂ reaction was studied under oxidizing conditions in the 100-400 °C range over 0.1 wt% Pt supported on various metal oxides such as MgO, CeO₂, SiO₂, La₂O₃, CaO, Y₂O₃ and TiO₂. The Pt/MgO and Pt/CeO₂ catalysts showed good catalytic behaviours. Here, we find that the Pt/Mg-Ce-O catalyst, prepared from MgO and CeO₂ by the sol-gel method, is a very active and selective catalyst towards N₂ formation in the whole 100–400 °C range. This catalyst appears to be the most active, selective and stable one ever reported in the literature for the NO/H₂/O₂ reaction, even in the presence of 5%v H₂O or 20 ppmv of SO₂ in the feed stream.Selected article from the Regional Symposium on Chemistry and Environment, Krusevac, Serbia, June 2003, organised by Dr. Branimir Jovancicevic.     

低污染、高效转式垃圾焚烧技术

通过在本课题组自行设计的中空水冷转式垃圾焚烧炉上的实验研究，论文从工艺流程和NOx生成特性方面探讨了该新型焚烧炉的稳定燃烧和低污染排放技术特点；并与固定床焚烧炉作了实验研究比较，可知中空水冷转式垃圾焚烧炉在降低NOx浓度与提高燃尽率方面具有良好的性能。     

超重力技术治理火炸药行业氮氧化物的初步研究

火炸药行业排放氮氧化物(NOX)具有浓度高、排放点不集中和间歇排放的特点,采用超重力技术对尾气中高浓度的NOX进行湿法吸收.以清水为吸收剂,研究了进气量、液气比和超重力因子等因素对NOX吸收率的影响.结果表明,单级NOX吸收率可达64.69%(β＝90).超重力旋转填料床具有占地面积小、投资低和操作方便等优点,适宜于火炸药行业吸收NOX.     

络合吸收结合生物转化去除氮氧化物技术

介绍了络合吸收结合生物转化处理NOx 技术的基本原理和目前的研究进展情况 ,并分析了该技术处理氮氧化物存在的问题和未来发展方向