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1.
Binary oxide systems(Cu Cr2O4, Cu Co2O4), deposited onto cordierite monoliths of honeycomb structure with a second support(finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine’s gas exhausts(O2, NOx, H2 O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3 NO2> H2 O > NO > O2> CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively(in the presence of copper chromite based catalyst) even at closing to ambient temperatures.Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem.  相似文献   

2.
Series of mixed metal oxides were synthesized by gel-combustion method and their catalytic activities for soot oxidation were investigated. The catalysts were M-Ce-Zr (M = Mn, Cu, Fe, K, Ba, Sr), and χK-20Mn-Ce-Zr (χ= 0, 5, 10, 20), they were characterized by XRD, SEM, TPR and BET surface area techniques. The results of soot temperature programmed oxidation (TPO) in an O2 oxidizing atmosphere indicate that K-Ce-Zr has the highest catalytic activity for soot oxidation under loose contact condition, due to enhancement of the soot and catalyst contacts. On the other hand, under a tight contact condition, Mn-Ce-Zr and Cu-Ce-Zr nano-composites have high activities for soot oxidation and lower the soot TPO peak temperatures by about 280 and 270℃, respectively, as compared to non-catalytic soot oxidation. Furthermore, the addition of up to 10 wt.% potassium oxides into Mn-Ce-Zr increases its catalytic activity and further reduces the soot TPO peak temperature by about 40℃ under loose contact condition.  相似文献   

3.
In this study, the effects of copper(Cu) additive on the catalytic performance of Ag/SBA-15 in complete soot combustion were investigated. The soot combustion performance of bimetallic Ag–Cu/SBA-15 catalysts was higher than that of monometallic Ag and Cu catalysts. The optimum catalytic performance was acquired with the 5 Ag_1-Cu_(0.1)/SBA-15 catalyst, on which the soot combustion starts at T_(ig)= 225°C with a T_(50)= 285°C. The temperature for 50% of soot combustion was lower than that of conventional Ag-based catalysts to more than 50°C(Aneggi et al., 2009). Physicochemical characterizations of the catalysts indicated that addition of Cu into Ag could form smaller bimetallic Ag–Cu nanolloy particles, downsizing the mean particle size from 3.7 nm in monometallic catalyst to 2.6 nm in bimetallic Ag–Cu catalyst. Further experiments revealed that Ag and Cu species elicited synergistic effects, subsequently increasing the content of surface active oxygen species. As a result, the structure modifications of Ag by the addition of Cu strongly intensified the catalytic performance.  相似文献   

4.
We report the application of a solid lanthanum–ceria–zinc catalyst in the catalytic regeneration of diesel particulate filters(DPF) in diesel engines.We synthesized a CeO_2–ZnO–La_2O_3(Ce–Zn–La) mixed oxide by a lactic acid-mediated sol–gel method,which efficiently coated cordierite substrates for soot capture and combustion.We studied the effects of La loading on the physicochemical and catalytic properties of Ce–Zn mixed oxide during lowtemperature soot combustion processes.We characterized the synthesized catalysts by X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),N2 adsorption,Raman spectroscopy,oxygen storage capacity(OSC),and scanning and transmission electron microscopy(SEM and TEM).Thermogravimetric and differential thermal analysis(TGA/DTA)confirmed that the catalysts effectively reduced the soot oxidation temperature.The ternary Ce–Zn–La mixed oxide catalyst with Ce/Zn/La atomic ratio of 2:1:0.5 had the highest catalytic activity and promoted soot oxidation at temperatures below 390°C.This indicated that the large number of oxygen vacancies in the catalyst structure generated oxygen species at low temperatures.Raman spectroscopy measurements revealed the presence of oxygen vacancies and lattice defects in Ce–Zn–La samples,which were key parameters concerning the stability and redox properties of the prepared catalysts.  相似文献   

5.
Mo/ZSM-5 catalysts with different Mo content were prepared by impregnation method. The effect of Mo content on the property of Mo/ZSM-5 catalysts and their performance for selective catalytic reduction(SCR) of NO with ammonia was investigated by XRD, ICP,XPS and NO-TPD respectively. The results showed that the catalytic activity of Mo/ZSM-5 for SCR of NO is strongly influenced by the Mo loading in HZSM-5 zeolites. The NOx conversion reached the highest value of 64.2% at 375℃ when Mo content is about 10.9%, and the temperatures at which the maximum of NOx conversion obtained were declined with the increase of Mo content. From XRD results, it can be seen that it exhibits the distinct interaction between Mo and HZSM-5 when Mo content is about 10.9%. This may result in a suitable phase structure in Mo/ZSM-5 catalyst, which is advantageous for NO reduction. XPS and NO-TPD results also showed that the catalytic activity of Mo/ZSM-5 may be related to the Mo percent on the surface.  相似文献   

6.
NOx emission abatement catalysts V2O5 supported on various TiO2 including anatase, rutile and mixture of both were investigated with various physico-chemical measurements such as BET, NH3-TPD, NARP, XRD and so on, and the effect of TiO2 surface properties on the SCR (selective catalytic reduction) activity of V20s/TiO2 catalysts was studied. It was found that the TiO2 surface properties had strong affect on the SCR activity of V2Os/TiO2 catalysts. The stronger acidic property resulted in the higher exposure of active sites as well as the higher SCR activity.  相似文献   

7.
Modified substrates as outer heterogeneous catalysts was employed to reduce the soot generated from incomplete combustion of diesel or diesel/biodiesel blends, a process that harms the environment and public health. The unique storage properties of ceria(CeO2) makes it one of the most efficient catalysts available to date. Here, we proposed that ceria-based catalysts can lower the temperature at which soot combustion occurs; more specifically, from 610℃ to values included in the diesel exhausts operation range(300–450℃). The sol-gel method was used to synthesize mixed oxide-based catalysts(CeO2:ZnO); the resulting catalysts were deposited onto cordierite substrates. In addition, the morphological and structural properties of the material were evaluated by XRD, BET, TPR-H2, and SEM. Thermogravimetric(TG/DTA) analysis revealed that the presence of the catalyst decreased the soot combustion temperature by 200℃ on average, indicating that the oxygen species arise at low temperatures in this situation, promoting highly reactive oxidation reactions. Comparative analysis of soot emission by diffuse reflectance spectroscopy(DRS) showed that catalyst-impregnated cordierite samples efficiently oxidized soot in a diesel/biodiesel stationary motor: soot emission decreased by more than 70%.  相似文献   

8.
Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.  相似文献   

9.
Mn-Ni oxides with different compositions were prepared using standard co-precipitation(CP) and urea hydrolysis-precipitation(UH) methods and optimized for the selective catalytic reduction of nitrogen oxides(NO_x) by NH_3 at low temperature.Mn((2))Ni_((1))O_x-CP and Mn_((2))Ni_((1))O_x-UH(with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction(SCR) catalytic activity,with about 96% NO_x conversion at 750 C and-99%in the temperature range from 100 to 250℃.X-ray diffraction(XRD) results showed that Mn_((2))Ni_((1))O_x-CP and Mn_((2))Ni_((1))O_x-UH catalysts crystallized in the form of Mn_2NiO_4 and MnO_2-Mn_2NiO_4 spinel,respectively.The latter gave relatively good selectivity to N_2,which might be due to the presence of the MnO_2 phase and high metal-O binding energy,resulting in low dehydrogenation ability.According to the results of various characterization methods,it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn_2NiO_4 spinel played important roles in the high-efficiency SCR activity of these catalysts.Mn_((2))Ni_((1))O_x catalysts presented good resistance to H_2O or/and SO_2 with stable activity,which benefited from the Mn_2NiO_4 spinel structure and Eley-Rideal mechanism,with only slight effects from SO_2.  相似文献   

10.
Binary oxide systems (CuCr2O4, CuCo2O4), deposited onto cordierite monoliths of honeycomb structure with a second support (finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine's gas exhausts (O2, NOx, H2O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3 >> NO2 > H2O > NO > O2 > CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively (in the presence of copper chromite based catalyst) even at closing to ambient temperatures. Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem.  相似文献   

11.
采用低温燃烧法制备了Na+部分取代La3+的La1-xNaxCo0.5Mn0.5O3系钙钛矿型复合氧化物催化剂。利用程序升温反应(TPR)技术,对催化剂应用于柴油机常规排放物中的碳微粒(soot)和氮氧化合物(NOx)的同时催化脱除性能进行了研究。  相似文献   

12.
用柠檬酸法制备了不同贵金属取代的钙钛矿LaCo0.96X0.04O3(X为Pt、Pd、Rh、Au、Ag)催化剂,用热重法测试了催化剂对碳烟的催化活性,采用程序升温还原法(H2-TPR)、X-射线衍射仪(XRD)、能量谱仪(EDS)和红外光谱(FTIR)对催化剂进行了测试.结果表明,催化剂LaCo0.96Ag0.04O3催化活性最高,起燃温度为449℃,远低于LaCoO3的504℃;各贵金属取代的钙钛矿LaCoO3的TPR还原峰变化各异;XRD特征峰的衍射角向高角度偏移,说明各贵金属进入了钙钛矿结构相;能谱图显示各贵金属进入钙钛矿相的量不同.  相似文献   

13.
综述了柴油机排放碳颗粒催化燃烧中运用的贵金属催化剂、过渡金属催化剂、(类)钙钛矿催化剂以及催化技术与低温等离子体技术协同作用的最新研究进展,介绍了上述催化剂和催化技术的作用机理,并探讨了它们在实际应用中存在的问题和应用前景。  相似文献   

14.
复合氧化物催化材料上碳颗粒物的催化燃烧   总被引:3,自引:1,他引:3  
针对柴油车排放碳颗粒物的控制 ,研制可应用于柴油车排放碳颗粒物催化再生复合氧化物催化材料 .通过运用热分析仪 (TGA)和程序升温氧化反应装置 (TPO)对复合氧化物催化材料的活性进行评价 ,研究了催化材料的组成、原子配比、催化材料与碳颗粒物质量比、H2O的加入、焙烧温度对催化活性的影响 .实验结果表明 :双组分金属氧化物催化剂中 ,Cu-Mo-O有较好的活性 ;多组分金属氧化物催化剂中 ,Cu-K-Mo-O在原子比Cu∶K∶Mo =1∶1∶2 ,催化剂与碳颗粒物质量比为 5∶1时活性最好 ,其碳颗粒物起燃温度为 32.7℃ ,同时H2O和焙烧温度对该催化剂的影响较小 ,是能够应用于柴油车排放碳颗粒物控制催化再生的良好催化材料 .  相似文献   

15.
柴油车的排气污染受到了越来越多的关注。文章分别介绍了柴油机排气中氮氧化物的还原、碳烟颗粒物的氧化以及同时去除氮氧化物和颗粒物的各种催化净化技术及其最新研究进展,并对该研究方向存在的主要问题和应用前景进行了探讨。  相似文献   

16.
Manganese oxide-loaded and -doped ceria as well as the corresponding barium-modified oxide catalysts were prepared for soot oxidation in the presence of NOx, and were characterized by using X-ray diffraction, Brunauer-Emmett-Teller and NO temperatureprogrammed oxidation measurements. The activity of catalyst depended strongly on the NO2 production capacity, and the importance of surface nitrates was weakened without heat transfer limitations. The formation of perovskite-type oxides after the high-temperature calcination caused the loss of NOx storage capacity for the Ba-modified catalysts, but did not seem to affect the NO oxidation activity obviously. The addition of barium did not prevent the phase separation of MnOx-CeO2 solid solutions, whereas it inhibited the sintering of oxide crystallites effectively. This, as well as the relatively high surface area, resulted in a small increase in soot oxidation temperature for the thermally aged Ba/Mn-Ce catalyst.  相似文献   

17.
A novel four-way combining catalysts containing double layers was applied to simultaneously remove four kinds of exhaust pollutants(NOx,CO,HC and PM) emitted from diesel engine.The four-way catalysts were characterized using scanning electron microscope(SEM) and Ultraviolet visible diffuse reflectance spectroscopy(UV-Vis DRS).Their catalytic performances were evaluated by temperature-programmed reaction technology.The double layer catalysts could effectively remove the four main pollutants.The highest catalytic activity was given by the two-layered catalysts of La0.6K0.4CoO3/Al2O3 and W/HZSM-5.Under the simulated exhaust gases conditions,the peak temperature of the soot combustion was 421°C,the maximal conversion of NO to N2 was 74%,the temperature of the HC total conversion was 357°C,and the maximum conversion ratio of CO was 99%.  相似文献   

18.
文章介绍了NH3选择性催化还原NOx技术(SCR)的基本原理,主要讨论了TiO2和分子筛型催化剂的优缺点,以及这两种催化剂应用于柴油车尾气NOx净化的主要问题和相应的解决措施,为开发车用SCR催化剂提供必要的支持。  相似文献   

19.
采用溶剂热法制备La1-xKxMnO3(x=0, 0.10, 0.15, 0.20, 0.25)钙钛矿型复合金属氧化物催化剂;通过XRD、FT-IR、SEM、H2-TPR、XPS、NO-TPD等手段对催化剂的物相组成、表面形貌、氧化还原性能等进行了表征;在常压固定床微型反应装置中评价催化剂同时消除NO和碳烟催化性能.结果表明,制备的La1-xKxMnO3催化剂均具有钙钛矿结构;K部分取代La-Mn钙钛矿结构中La后,颗粒结构得以改善,部分Mn3+价态升高为Mn4+,形成较多氧空位和Mn4+,提高氧化还原性能和吸附NO性能.活性评价结果表明,La0.80K0.20MnO3催化剂表现出较好的同时消除NO和碳烟催化性能,NO最大转化率(Xmax NO)和对应反应温度(Tmax NO)分别为46.5%和436℃,碳烟起燃温度(Tig)、CO2浓度峰值温度(Tmax CO2)和生成CO2选择性(Smax CO2)分别为341℃、454℃和98.8%.  相似文献   

20.
SO2气氛下Cu-Ce-O催化剂氧化柴油车排气碳烟的性能   总被引:5,自引:1,他引:4       下载免费PDF全文
陈瑜  叶代启  付名利  梁红 《环境科学学报》2008,28(11):2167-2174
运用程序升温氧化(TPO)对共沉淀法合成的Cu-Ce-O催化剂进行了活性评价,考察了在不同浓度的S0,气氛下cu-Ce-O催化剂氧化模拟碳黑的性能,并用BET、XRD、TPR和FT-IR对催化剂进行了表征.BET和XRD测试显示,cu和ce的结合使催化剂比表面积增大,晶体结构发生变化,形成了复合氧化物;TPO活性测试结果表明,Cu-Ce-O复合催化剂比单一组分的CuO或CeO2具有更好的低温催化活性.复合氧化物cu-Ce-O中Cu原子含量越高,对应硫化后的催化剂氧化碳烟的能力越低,同时催化剂表面生成的硫酸盐越多,即催化剂抗硫中毒能力也降低.浓度低于0.03%的SO2对Cu-Ce-O的催化性能有一定的促进作用,但SO2的体积分数超过0.03%后碳黑燃烧速率变慢;FT-IR初步证实了高体积分数的SO2所产生的大量SO24-可能是抑制催化剂活性的原因.  相似文献   

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