汽车尾气净化催化剂Ag/SAPO-34选择性催化还原NO

评价了Ag/SAPO-34分子筛催化剂选择性还原NO的活性,并运用漫反射红外光谱原位研究NO在Ag/SAPO-34催化剂上的选择性催化还原机理.结果表明Ag/SAPO-34有良好的低温活性,在氧气浓度为3.6%和温度为573K～673K时NO还原成N2的转化率达70%;催化剂活性随C3H6浓度的增加而升高,随空速的增加而稍有下降.基于漫反射红外光谱,认为反应机理为:NO、丙烯和氧反应,在Ag/SAPO-34催化剂上生成吸附的有机-氮氧化物,再由这些吸附物种分解成N₂,催化还原的关键是形成有机-氮氧化物中间体.氧的作用是充分促进丙烯活化以及增加NO_x吸附态含量,并且氧的存在是有效产生一系列中间物不可缺少的条件.     

光照对SO2在矿质氧化物表面非均相反应的影响

使用原位漫反射红外傅里叶变换光谱(DRIFTS)研究了SO_2在α-Al_2O_3、TiO_2、CaO和α-Fe_2O_3颗粒物表面的非均相反应,考察了紫外光光照(波长约365 nm)对SO_2在不同氧化物表面反应的影响.结果表明,无紫外光照射条件下,SO_2在TiO_2、α-Al_2O_3、CaO颗粒物表面反应的主要产物为亚硫酸盐;有紫外光照射条件下,SO_2在TiO_2、α-Al_2O_3、CaO颗粒物表面反应的主要产物为硫酸盐;但紫外光照射对SO_2在α-Fe_2O_3表面的反应并没有明显的影响.推测机理可能是光照促进了颗粒物表面的亚硫酸盐向硫酸盐的转化.     

Performance and mechanism study for low-temperature SCR of NO with propylene in excess oxygen over Pt/TiO2 catalyst

A 0.5 wt.% Pt/TiO2 catalyst was prepared and used for the low-temperature selective catalytic reduction(SCR) of NO with C3 H6 in the presence of excess oxygen.The effects of Pt loading and O2 concentration on Pt/TiO2 catalytic performance for low-temperature SCR were investigated.It was found that optimal Pt loading was 0.5 wt.% and excess O2 favored low-temperature SCR of NOx.The mechanism of low-temperature SCR of NO with C3 H6 was investigated with respect to the behavior of adsorbed species over Pt/TiO2 at 150°C using in situ DRIFTS.The results indicated that surface nitrosyl species(Pt δ+-NO and Ti 3+-NO) and Pt 2+-CO are main reaction intermediates during the interactions of NO,C3 H6 and O2.A simplified NO decomposition mechanism for the low-temperature SCR of NO with C3 H6 was proposed.     

In situ DRIFTS study of hygroscopic behavior of mineral aerosol

In situ difflusion reflectance infrared Fourier transform spectroscopy was used to study the water adsorption on mineral oxides(SiO2,α-Al2O3,MgO,Fe2O3,TiO2).The results showed that all the water adsorption isotherms were well fitted with the Brunauer-EmmettTeller(BET)-Ⅲ type equation,with the calculated monolayers occurring at 24%-30% relative humidity.It showed that about 1-5 layers of water adsorbed on oxides surfaces in ambient relative humidity(20%-90%).The measured deliquescence relative humidity of NaCl was(74 ± 1)%,which demonstrated that DRIFTS is a useful method for the study the hygroscopic behavior of mineral dust.In addition,the limits of DRIFTS were also discussed.     

Fe掺杂对MnO_x催化剂结构性质及低温SCR反应机制的影响

采用Fe对MnOx催化剂的低温选择性催化还原（SCR）活性进行改性,并通过N2吸附、X射线衍射（XRD）、X射线光电子能谱（XPS）及原位漫反射傅里叶红外（insituDRIFTS）重点探讨了Fe引入后催化剂结构性质的变化及对低温SCR反应机制的影响.结果表明,Fe的掺杂能显著提高催化剂的低温SCR性能,Fe/（Fe＋...     

大气化学非均相反应摄取系数的测定

摄取系数是表征大气非均相反应的重要物理化学参数,也是大气颗粒物表面摄取气体能力的重要量化指标.本文综述了摄取系数的主要概念、主要测定方法和影响因素,以NaCl与NO2非均相反应为例,讨论了用漫反射傅立叶转换红外原位反应器扩散实验方式测定反应摄取系数的方法和误差,分析了气体扩散深度与红外穿透厚度对测定结果的影响,并测定了初始反应摄取系数.     

Heterogeneous reaction of NO2 on the surface of montmorillonite particles

The studies on heterogeneous reactions over montmorillonite, which is a typical 2:1 layered aluminosilicate, will benefit to the understanding of heterogeneous reactions on clay minerals. Montmorillonite can be classified as sodium montmorillonite or calcium montmorillonite depending on the cation presented between the different layers. Using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), the heterogeneous reaction mechanism of NO₂ on the surface of montmorillonite was firstly investigated. Results showed that the reaction of NO₂ on the surface of sodium and calcium montmorillonite fit a first-order kinetics, and the reaction duration of calcium montmorillonite was longer than that of sodium montmorillonite under the dry condition. For either sodium or calcium montmorillonite, the uptake coefficient decreased as humidity increased.     

Elimination of formaldehyde over Cu-Al2O3 catalyst at room temperature

Catalytic elimination of formaldehyde (HCHO) was investigated over Cu-Al2O3 catalyst at room temperature. The results indicated that no oxidation of HCHO into CO2 occurs at room temperature, but the adsorption of HCHO occurs on the catalyst surface.With the increase of gas hourly space velocity(GHSV) and inlet HCHO concentration, the time to reach saturation was shortened proportionally. The results of the in situ DRIFTS, Density functional theory calculations and temperature programmed desorption(TPD) showed that HCHO was completely oxidized into HCOOH over Cu-Al2O3 at room temperature. With increasing the temperature in a flow of helium, HCOOH was completely decomposed into CO2 over the catalyst surface, and the deactivated Cu-Al2O3 is regenerated at the same time. In addition, although Cu had no obvious influence on the adsorption of HCHO on Al2O3, Cu dramatically lowered the decomposition temperature of HCOOH into CO2. It was shown that Cu-Al2O3 catalyst had a good ability for the removal of HCHO, and appeared to be promising for its application in destroying HCHO at room temperature.     

MnOx／Al-SBA-15催化剂低温NH3选择性催化还原NO的原位红外研究

用原位红外分别进行了MnOx／Al-SBA-15催化剂上NH3和NO＋O2的吸附态和瞬态实验以及NH3＋NO＋02反应的稳态实验。结果表明,催化剂上存在着L酸位和B酸位,NH3吸附在催化剂上形成配位态的NH3和NH4＋,配位态的NH3能脱氢形成-NH2活性中间态。NO＋O2在催化剂上吸附形成硝酸盐类、硝基类和亚硝酸盐类。将NO＋O2通入预吸附NH3的催化剂中时,表面的配位态的NH3、NH4＋和-NH2都会减少直至消失,SCR反应显著。而将NH3通人预吸附NO＋O2的催化剂中时,只有硝基类和亚硝酸盐类减少,硝酸盐类基本不发生变化,SCR反应微弱。NH3＋NO＋O2稳态反应中,催化剂表面稳定存在着NH4＋和硝酸盐类,SCR反应显著。     

A case study of Asian dust storm particles: Chemical composition, reactivity to SO2 and hygroscopic properties

Mineral dust comprises a great fraction of the global aerosol loading, but remains the largest uncertainty in predictions of the future climate due to its complexity in composition and physico-chemical properties. In this work, a case study characterizing Asian dust storm particles was conducted by multiple analysis methods, including SEM-EDS, XPS, FT-IR, BET, TPD/mass and Knudsen cell/mass. The morphology, elemental fraction, source distribution, true uptake coefficient for SO₂, and hygroscopic behavior were studied. The major components of Asian dust storm particles are aluminosilicate, SiO₂ and CaCO₃, with organic compounds and inorganic nitrate coated on the surface. It has a low reactivity towards SO₂ with a true uptake coefficient, 5.767×10^-6, which limits the conversion of SO₂ to sulfate during dust storm periods. The low reactivity also means that the heterogeneous reactions of SO₂ in both dry and humid air conditions have little effect on the hygroscopic behavior of the dust particles.