Theoretical and experimental study on formation and adsorption of enolic species on Ag-Pd/Al2O3 catalyst

The formation and adsorption of enolic species on a palladium promoted Ag/Al2O3 catalyst (denoted Ag-Pd/Al2O3) during the selective catalytic reduction (SCR) of NOx by C3H6 has been studied by means of DRIFTS and density functional calculations. The structure of the enolic species adsorbed on Ag-Pd/Al2O3 catalyst has been established based on the in situ DRIFTS spectra and simulated results. The reaction mechanism from C3H6 to enolic species on Ag-Pd/Al2O3 catalyst was proposed and the hypothesis about the Pd promotion was discussed.     

Conformational analysis and comparison between theoretical and experimental vibration spectra for isocyanate species on Ag/Al2O3 catalyst

Density functional theory (DFT) calculations were performed to study the structure and vibrational frequencies of the intermediate for the isocyanate (NCO) surface species on Ag/Al(2)O(3) catalyst using the GAUSSIAN 98 suite of programs. Thermal decomposition of adsorbed CH(3)NO(2) species leads to the formation of two types of NCO species (NCO on Ag and NCO on Al(2)O(3)) above 298K. In order to investigate the reaction mechanism, we have designed the calculated models (a-g) for the NCO intermediate. Through the analysis of the vibration mode and the vibration frequency of the calculated models (a-g), we conclude that there is an excellent agreement between the calculated vibration spectrum of the model (e) containing the -AgNCO group or model (g) containing the -AlNCO group and the experimental vibration spectrum.     

氢气对Ag/Al2O3和Cu/Al2O3催化剂选择性催化C3H6还原Nox反应的影响

 添加H2对Ag/Al2O3和Cu/Al2O3催化剂选择性催化C3H6还原NOx反应具有不同的影响. 原位漫反射红外光谱分析表明,在Ag/Al2O3催化剂上, H2的存在促进了C3H6部分氧化产物烯醇式物种(RCH=CH-O-)和乙酸盐等的形成,烯醇式物种和硝酸盐为主要反应中间体,二者间的相互反应性能很强,能形成高浓度的反应关键中间体异氰酸酯(-NCO)表面吸附物种,因此NOx的去除活性提高; 而在Cu/Al2O3催化剂上, H2的存在并没有促进C3H6部分氧化产物的形成,而且抑制了硝酸盐的形成,进而抑制了C3H6部分氧化产物与硝酸盐反应形成表面-NCO 物种,导致NOx的去除活性降低.     

Conformational analysis of sulfate species on Ag/Al2O3 by means of theoretical and experimental vibration spectra

The formation and configuration of sulfate species on Ag/Al2O3 were studied by means of in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. The comparison between theoretical and experimental vibration spectra enable us to draw the following conclusions: Bidentate sulfate species rather than tridentate sulfate species are the predominant surface species on Ag/Al2O3. Moreover, both bidentate and tridentate sulfate species may coexist on the catalyst surface at a lower coverage. The accumulation of surface sulfate species could well explain the blue shift of the sulfate species in IR spectra. In addition, the in situ DRIFTS could distinguish between the sulfate species that linked to Al site and Ag site, which was well supported by temperature-programmed desorption (TPD) results.     

银/氧化铝催化乙醇选择性还原氮氧化物过程中典型中间体的吸附态研究

机动车污染物排放是我国大气复合污染形成的重要原因之一.尽管柴油车在我国机动车保有量中所占比例不到20%,但其排放的颗粒污染物(PM)和氮氧化物(NOx)分担率均超过60%.因此,控制柴油车尾气排放成为我国亟待解决的大气污染问题.目前,氨选择性催化还原NOx技术(NH3-SCR)已规模化应用于柴油车污染排放控制,出于安全性考虑,以尿素水溶液作为氨的来源.但NH3-SCR技术应用于柴油车尾气净化存在如下缺点：需要布建庞大的尿素添加基础设施、后处理系统复杂等.与此相反,以车载燃油为还原剂来源的HC-SCR技术可有效规避上述难题,展现了较好的应用前景.但是,直接以柴油为还原剂时, HC-SCR对NOx净化的效率还难以满足日益严格的排放法规的要求,因此需要深入研究HC选择性还原NOx的微观机制与构效关系,并以此为指导,发展以车载燃料为还原剂来源的高效净化NOx的新原理和新方法.已有的研究表明,银/氧化铝(Ag/Al2O3)具有优异的催化乙醇选择性还原NOx的能力,是最有希望应用于柴油车尾气NOx净化的催化剂-还原剂组合体系.鉴于此,本论文以Ag/Al2O3催化剂上乙醇-SCR反应为研究对象,以密度泛函理论计算方法(DFT)搭建了Ag/Al2O3催化剂的理论模型,考察了反应物乙醇(CH3CH2OH)、关键中间体(烯醇式物种CH2=CHO?和?NCO)在Ag/Al2O3催化剂上的吸附特征,采用电子态密度分析(DOS)研究了以上物种被活化的电子机制,以期甄别Ag/Al2O3催化乙醇选择性还原NOx的活性位结构,为高性能的HC-SCR催化剂设计提供指导.
　　依据化学态的不同, Ag/Al2O3催化剂上活性组分银可分为：高度分散的离子态(Ag+、在催化剂表面以Ag?O形式存在)、部分氧化团簇(Agnδ+)和金属颗粒银(Agn0),其中氧化态的银是催化乙醇选择性还原NOx的活性组分. Al2O3载体的主要暴露晶面为(110)和(100),在上述晶面上Al的配位状态存在明显差异,显著影响了银物种的锚定与分散,形成了具有不同键合特征的Ag?O?Al结构.基于对Al2O3暴露晶面上Al配位状态的分析,搭建了6种Ag?O?Al结构模型.结合Al MAS NMR对Ag/Al2O3实际催化剂的表征结果和理论模型吸附能的分析,获得了最为可能的两种Ag?O?Al结构： Ag?O?Altetra(AlO4)和Ag?O?Alocta(AlO6);前者为AgO与Al2O3(110)面Altrip位键合形成的特征结构(Al最终为四配位),后者系AgO锚定于Al2O3(100)面Alpenta位的能量最优结构(Al最终为六配位).
　　在Ag?O?Altetra上, Altetra位具有较强的酸性, Ag、Al原子轨道的杂化融合有利于电子转移;以上特性促进CH3CH2OH、CH2=CHO?、?NCO的吸附活化.在HC-SCR反应中,关键中间体?NCO通过与NOx直接反应可形成最终产物N2和CO2.可见,?NCO中N=C键的拉伸活化、断裂对上述反应的发生至关重要.由电子态密度分析可知, N=Cσ键能向Ag?O?Altetra中Altetra位转移电子,而Ag与Al的轨道融合能反馈电子到N=C π键;在这两种电子转移机制作用下,?NCO中的N=C键被最大程度弱化,有利其断裂,转化为最终产物N2和CO2.而Ag?O?Alocta上,并没有N=C键的活化拉伸,反而呈现出N=C键收缩趋势,不利于N=C键的断裂与最终产物的形成.由此推定, Ag?O?Altetra是Ag/Al2O3催化剂上HC-SCR反应的活性中心.     

Experimental and theoretical studies of surface nitrate species on Ag/Al2O3 using DRIFTS and DFT

Surface nitrate (NO3(-)) species on the Ag/Al2O3 play an important role in the selective catalytic reduction (SCR) of NOx. In this study, the formation and configuration of surface nitrate NO3(-)(ads) species on Ag/Al2O3 and Al2O3 in the oxidation of NO have been studied using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. Different nitrates species (bridging, bidentate and monodentate) were observed by in situ DRIFTS and validated by DFT calculations results. Attention was especially focused on the proposal of two different bidentate nitrates species (a normal bidentate and an isolated bidentate). In addition, the thermal stability of different surface nitrate species was discussed based on the adsorption energies calculations, DRIFTS, and temperature-programmed desorption (TPD) results. It was suggested that the decomposition and desorption of the surface nitrate species could be controlled by kinetics.     

Ag/Al2O3 催化剂催化含氧烃类选择性还原氮氧化物的基础与应用研究进展

 Ag/Al2O3 催化含氧烃类选择性还原 (SCR) 氮氧化物 (NOx) 是有望实际应用于柴油机尾气治理的技术之一. 从 Ag/Al2O3 的基本属性、还原剂的筛选与匹配、NOx 还原低温活性改进、催化体系耐硫性的调变和 Ag/Al2O3-乙醇体系的实用化开拓等方面, 对我们近年来的工作进行了综述, 阐明了该组合体系高效 SCR 特性的微观机制. 发动机台架实验表明, 结合柴油机机内调整, 应用 Ag/Al2O3-乙醇的 SCR 体系能够满足我国重型柴油车国 Ⅳ 排放标准.     

富氧条件下Cu/Al2O3催化剂上C3H6选择性还原NO的研究

以Cu/Al2O3为催化剂,对富氧条件下C3H6为还原剂选择性催化还原NO反应进行了研究.活性评价结果表明,与高活性的Ag/Al2O3催化剂相比,Cu/Al2O3催化剂选择性还原NO的活性较低,NO的最高转化率仅为40%.在所考察的温度范围(473～723K)内,红外谱图中不存在有机含氮化合物(R—ONO和R—NO2)的特征振动吸收峰.作为反应中间体—NCO的前驱体,有机含氮化合物在Cu/Al2O3催化剂表面难以生成是造成催化剂选择性还原NO活性低的直接原因.在Cu/Al2O3催化剂上,NO2吸附能够优先发生,并以NO3-物种的形式覆盖在大部分催化剂表面.动态原位红外光谱实验发现,这种NO3-表面物种与C3H6的反应性较差,使生成有机含氮化合物的关键反应难以发生,但此时的催化剂表面有利于C3H6和O2的完全氧化反应,这是导致Cu/Al2O3催化剂选择性较低的根本原因.     

Bactericidal mechanism of Ag/Al2O3 against Escherichia coli

The bactericidal process of Ag/Al2O3 to Escherichia coli has been investigated to clarify the bactericidal mechanism. In SEM images, the configuration of E. coli cells contacting with the catalyst surface was quite different from that contacting with AgNO3 solution, which indicated that the Ag+ eluted from the catalyst did not play an important role in the bactericidal process. The bactericidal experiments strongly confirmed the contribution of multiform reactive oxygen species (ROS) (super oxide dismutase (SOD) and catalase as the scavengers for O2*- and H2O2, respectively) to bactericidal effect on the catalyst surface. Furthermore, the surface modification of Ag/Al2O3 by ultraviolet and formaldehyde influenced the bactericidal effect obviously, which not only confirmed the bactericidal mechanism of catalytic oxidation but also provided evidence for the synergistic effect between Ag and Al2O3 on the catalyst surface.     

Brönsted and Lewis acidity of the BF3/gamma-Al2O3 alkylation catalyst as revealed by solid-state NMR spectroscopy and DFT quantum chemical calculations

Multinuclear solid-state NMR techniques and DFT quantum chemical calculations were employed to investigate the detailed structure of acid sites on the BF3/gamma-Al2O3 alkylation catalyst. The NMR experiment results indicate that gaseous BF3 is able to react with the hydroxyl groups present on the surface of gamma-Al2O3, leading to the formation of new Br?nsted and Lewis acid sites. The 1H/11B and 1H/27Al TRAPDOR (TRAnsfer of Population in DOuble Resonance) experiments suggest that the 3.7 ppm signal in 1H NMR spectra of the BF3/gamma-Al2O3 catalyst is due to a bridging B-OH-Al group that acts as a Br?nsted acid site of the catalyst. On the other hand, a Lewis acid site on the surface of the catalysts, as revealed by 31P MAS and 31P/27Al TRAPDOR NMR of adsorbed trimethylphosphine, is associated with three-coordinate -OBF2 species. 13C NMR of adsorbed 2-13C-acetone indicates that the Br?nsted acid strength of the catalyst is slightly stronger than that of zeolite HZSM-5 but still weaker than that of 100% H2SO4, which is in good agreement with theoretical prediction. In addition, DFT calculations also reveal the detailed structure of various acid sites formed on the BF3/gamma-Al2O3 catalyst and the interaction of probe molecules with these sites.     

Theoretical study on silver- and gold-loaded zeolite catalysts: thermodynamics and IR spectroscopy

Density functional calculations have been carried out to determine geometries, adsorption energies and vibrational frequencies of NO, N(2)O, CO, O(2), and H(2)O, on a model for Ag(I) and Au(I) ion-exchanged ZSM-5 catalysts. Using statistical mechanics, the DeltaH and DeltaG values were calculated in order to evaluate the stability of the adsorbates on Ag(I) and Au(I) sites. The calculated vibrational frequencies are in reasonable agreement with the reported experimental values. The analysis of the results shows that at 475 degrees C the adsorption of two NO molecules and the direct N(2)O decomposition on AgZSM-5 are thermodynamically unfavorable. The adsorption of one NO molecule presents a small positive DeltaG value. On the contrary, in the case of AuZSM-5, the adsorption of one NO molecule and the direct N(2)O decomposition to produce N(2) are thermodynamically favorable. For both models, the N(2)O decomposition by AgO and AuO species is thermodynamically very favorable. The analysis of the interaction with H(2)O shows that water displaces the adsorbed NO on AgZSM-5 but not on AuZSM-5 which indicates that the AuZSM-5 catalyst is less sensitive to deactivation by H(2)O than the AgZSM-5 catalyst.     

Cl–改性对Ag/Al2O3催化剂结构及其催化C3H6-SCR和H2/C3H6-SCR反应性能的影响

以烯烃为还原剂的NOx选择性催化还原(HC-SCR)是重要的环境催化反应之一.Ag/Al2O3催化剂(SA)因在HC-SCR反应中表现高活性、高N2选择性及中等H2O和SO2耐受性等优点,而被广泛研究.SA催化剂中存在不同的Ag物种,包括孤立Ag+离子,带部分正电荷Agnδ+团簇和金属态Agn0团簇.文献研究结果表明,SA催化剂中Agnδ+团簇是催化HC-SCR反应的活性Ag物种,而Ag物种类型与Ag的负载量密切相关.因此文献中研究SA催化HC-SCR反应的结构-性能关系主要是通过改变Ag负载量来开展的,最优Ag负载量约为1％～2％.本文以Cl–改性的γ-Al2O3作为载体,采用传统的浸渍法制备了Ag/Al2O3-Cl催化剂(SA-Cl),通过XRD、TEM、H2-TPR、UV-Vis DRS以及XPS对催化剂进行了结构表征,并结合C3H6-SCR和H2/C3H6-SCR活性测试,建立催化剂结构-催化性能关系;同时利用原位傅里叶变换红外光谱(DRIFTS)和在线同步辐射单光子电离质谱(SVUV-PIMS)研究了SA催化HC-SCR的反应机理.结构表征结果表明,在SA催化剂中,Ag负载量的提高主要是增加了Agn0物种,而在SA-Cl催化剂中,Ag负载量的提高主要是增加了Agnδ+物种,因此Cl?改性能促进SA催化剂中Agnδ+物种的形成.活性测试结果表明,在相同Ag负载量下,SA-Cl催化剂表现出比SA催化剂更好的HC-SCR催化性能.Cl?改性对SA催化剂中Ag物种的调控作用和HC-SCR催化性能的促进作用随Ag负载量的增加变得更为明显.原位DRIFTS结果表明,γ-Al2O3载体(Al位点)是NO氧化形成硝酸盐物种的主要活性位点;Agnδ+物种催化丙烯适度氧化主要生成乙酸盐类物种,可以还原表面硝酸盐物种;而Agn0催化丙烯过度氧化主要生成羧酸盐类物种,进而生成CO2,不能还原表面硝酸盐物种.由此可见,Agnδ+是催化HC-SCR反应的活性Ag物种,而Agn0是催化烃类完全氧化反应的活性Ag物种;Cl–改性能有效促进Agnδ+的形成,进而提高HC-SCR催化反应活性.在线SVUV-PIMS结果检测到H2/C3H6-SCR反应中存在气态中间物种丙烯腈(CH2=CHCN).–CN和–NCO物种被认为是HC-SCR反应的关键中间物种,能够直接与气相NO+O2反应生成N2.因此,CH2=CHCN的存在说明HC-SCR反应涉及到气相反应机理.基于SA和SA-Cl催化剂,进一步研究了H2对C3H6-SCR低温活性的促进作用.结果表明,H2的促进作用是通过作用于Agnδ+物种,而不是通过Agn0物种来实现的;H2的引入有利于低温下强吸附硝酸盐物种的脱附或分解以及中间体向–NCO和–CN物种的转化,从而提高HC-SCR低温催化活性.综上,基于Cl–改性的Ag/Al2O3-Cl催化剂,本文成功证实了Agnδ+物种是催化HC-SCR反应的活性Ag物种,并结合原位DRIFTS在线SVUV-PIMS谱分别鉴定了催化反应表面中间物种和气相中间物种.这些结果加深了对SA催化HC-SCR反应构-效关系和反应机理的基础理解.     

FTIR spectroscopy combined with quantum chemical calculations to investigate adsorbed nitrate on aluminium oxide surfaces in the presence and absence of co-adsorbed water

Surface reactions of nitrogen oxides with aluminium oxide particles result in the formation of adsorbed nitrate. Specifically, when alpha-Al(2)O(3) and gamma-Al(2)O(3) particles are exposed to gas-phase NO(2) and HNO(3) adsorbed nitrate forms on the surface. In this study, Fourier transform infrared (FTIR) spectroscopy is combined with quantum chemical calculations to further our understanding of the adsorbed nitrate product on aluminium oxide particle surfaces in the presence and absence of co-adsorbed water at 296 K. FTIR spectra of adsorbed nitrate on alpha-Al(2)O(3) and gamma-Al(2)O(3) particles are interpreted using calculated vibrational frequencies of nitrate coordinated to binuclear Al oxide cluster models. Comparison of the calculated and experimental vibrational frequencies of adsorbed nitrate establishes different modes of coordination (monodentate, bidentate and bridging) of the nitrate ion to the surface in the absence of adsorbed water. In the presence of co-adsorbed water, the nitrate ion becomes fully solvated, as shown by a comparison of the experimental nitrate infrared spectra as a function of relative humidity with the calculated nitrate vibrational frequencies for binuclear Al cluster compounds which contain both coordinated nitrate ions and water molecules. These calculations also suggest that adsorbed water can displace nitrate from direct coordination to the surface, leading to an outer-sphere nitrate adsorption complex as well as an inner-sphere complex. Furthermore, the relative humidity dependence of the spectra suggest that water does not evenly wet the surface even at high relative humidity, as there are open or bare surface sites where nitrate ions are not solvated. Besides adsorbed mondendate, bidendate, bridging and solvated nitrate, the presence of ion bound nitrate ion, partially solvated nitrate, molecular nitric acid, hydronium ion and H(3)O(+):NO(3)(-) ion pairs on the oxide surface are also discussed.     

Characterization of O2-CeO2 interactions using in situ Raman spectroscopy and first-principle calculations.

Interactions between O(2) and CeO(2) are examined experimentally using in situ Raman spectroscopy and theoretically using density-functional slab-model calculations. Two distinct oxygen bands appear at 825 and 1131 cm(-1), corresponding to peroxo- and superoxo-like species, respectively, when partially reduced CeO(2) is exposed to 10 % O(2). Periodic density-functional theory (DFT) calculations aid the interpretation of spectroscopic observations and provide energetic and geometric information for the dioxygen species adsorbed on CeO(2). The O(2) adsorption energies on unreduced CeO(2) surfaces are endothermic (0.91相似文献   

A density functional theory study of vibrational coupling in the amide I band of beta-sheet models

We report the first molecular orbital/density functional theory (DFT) calculations on the vibrational frequencies involved in the amide I band of completely geometrically optimized models for beta-sheet peptides based upon (up to 16) glycine residues. These calculations use the B3LYP/D95** level of DFT. The primary means of vibrational coupling occurs through H bond, rather than through space, interactions, which is consistent with a previous report on alpha-helical polyalanines and H-bonding chains of both formamides and 4-pyridones. We decoupled the C=O stretching vibrations using selected 14C substitutions to probe the coupling mechanism and to determine "natural" frequencies for individual 14C=Os. The intermolecular H-bonding interactions affect the geometries of the amide groups. Those near the center of H-bonding chains have long C=O bonds. The C=O bond lengths correlate with these "natural" frequencies, The frequencies obtained from the DFT calculations are generally more coupled, and the most intense are more red shifted than those calculated by transition dipole coupling (TDC). TDC inverts the order of the shifted frequencies compared to DFT in several cases.     

Vibrational frequencies and infrared intensities of the hydrogen-bonded complexes of nitrous acid with ethers: ab initio and DFT studies

The vibrational spectra of the binary complexes formed by HONO-trans and HONO-cis with dimethyl and diethyl ethers have been investigated using ab initio calculations at the SCF and MP2 levels with 6-311++G(d,p) basis set and B3LYP calculations with 6-31G(d,p) and 6-31+G(d,p) basis sets. Full geometry optimisation was made for the complexes studied. The accuracy of the ab initio calculations have been estimated by comparison between the predicted values of the vibrational characteristics (vibrational frequencies and infrared intensities) and the available experimental data. It was established, that the methods, used in this study are well adapted to the problem under examination. The predicted values with the B3LYP calculations are very near to the results, obtained with 6-311++G(d,p)/MP2. The ab initio and DFT calculations show that the changes in the vibrational characteristics (vibrational frequencies and infrared intensities) upon hydrogen bonding for the hydrogen-bonded complex (CH3)2O...HONO-trans are larger than for the complex (CH3)2O...HONO-cis.     

富氧条件下Ag/Al2O3-Cu/Al2O3组合催化剂催化乙醇选择性还原NOx

 在富氧条件下,以乙醇为还原剂,考察了不同金属负载量的Ag/Al2O3和Cu/Al2O3催化剂选择性还原NOx的活性. 结果表明,4%Ag/Al2O3和10%Cu/Al2O3分别为各自体系中的最佳催化剂. 4%Ag/Al2O3具有很高的选择性催化还原NOx的活性,但同时会产生一定量的副产物CO. 10%Cu/Al2O3选择性催化还原NOx的活性不高,但却具有很好的消除CO的活性. 将4%Ag/Al2O3和10%Cu/Al2O3以不同方式组合,其评价结果表明,4%Ag/Al2O3-10%Cu/Al2O3组合催化剂具有与单纯4%Ag/Al2O3相似的NOx脱除活性,同时能够完全消除反应过程中产生的CO,并且能大大降低尾气中乙醇和乙醛的浓度.     

Ab initio prediction of the potential energy surface and vibrational-rotational energy levels of dialuminum monoxide, Al2O

The equilibrium structure and potential energy surface of dialuminum monoxide, Al(2)O, have been determined from large-scale ab initio calculations using the coupled-cluster method, CCSD(T), in conjunction with basis sets of triple- through quintuple-zeta quality. The effects of core-electron correlation on the calculated molecular parameters were investigated. The vibrational-rotational energy levels of the Al(2) (16)O and Al(2) (18)O isotopic species were calculated by a variational approach. The predicted energy levels are in remarkably good agreement with the available experimental spectroscopic data (from laser-induced fluorescence), demonstrating that the Al(2)O molecule is linear at equilibrium in its ground electronic state. The reported theoretical data settle controversies between the experimental studies about the equilibrium structure and assignment of vibrational fundamentals of the Al(2)O molecule.     

TiO2-Al2O3作为Mo催化剂担体的研究

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