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1.
Ag/Al2O3 is a promising catalyst for the selective catalytic reduction (SCR) by hydrocarbons (HC) of NO
x
in both laboratory and diesel engine bench tests. New developments of the HC-SCR of NO
x
over a Ag/Al2O3 catalyst are reviewed, including the efficiencies and sulfur tolerances of different Ag/Al2O3-reductant systems for the SCR of NO
x
; the low-temperature activity improvement of H2-assisted HC-SCR of NO
x
over Ag/Al2O3; and the application of a Ag/Al2O3-ethanol SCR system with a heavy-duty diesel engine. The discussions are focused on the reaction mechanisms of different Ag/Al2O3-reductant systems and H2-assisted HC-SCR of NO
x
over Ag/Al2O3. A SO2-resistant surface structure in situ synthesized on Ag/Al2O3 by using ethanol as a reductant is proposed based on the study of the sulfate formation. These results provide new insight
into the design of a high-efficiency NO
x
reduction system. The diesel engine bench test results showed that a Ag/Al2O3-ethanol system is promising for catalytic cleaning of NO
x
in diesel exhaust. 相似文献
2.
氮氧化物(NOx)是一种重要的大气污染物, 它造成严重的环境问题, 同时威胁人类健康. 以钢铁烧结烟气为代表的固定源和以柴油机尾气为代表的移动源是氮氧化物的主要来源. 氨气选择性催化还原法(NH3-SCR)是目前最有效且应用最广泛的NOx脱除技术. 然而, 无论是固定源还是移动源上NH3-SCR催化剂, 都不可避免地会被SO2毒化, 造成催化剂失活, 限制了NH3-SCR技术的进一步应用. 因此, 研究NH3-SCR催化剂的SO2中毒机制以及提高催化剂的抗硫性能至关重要. 我们对固定源脱硝的金属氧化物和移动源上脱硝的Cu基分子筛这两类不同催化剂体系的SO2中毒机制的研究进展进行了介绍, 并对这两种催化剂上提高抗硫性能改性方法的研究进展进行了评述, 为未来的研究提供了参考. 相似文献
3.
Metal promoted zirconia-based oxide sorbents, such as Pt–ZrO2/Al2O3 for NO
x
have been investigated. To clarify the role of the catalyst component, sorption of NO and NO2 was compared using the samples with and without Pt. The catalytic oxidation of NO to NO2 and successively to nitrate ions is an important role for the Pt catalyst. The experimental results indicate that a high-temperature calcination is essential to remove residual Cl from Pt–ZrO2–Al2O3 prepared from H2PtCl6 in order to provide more active NO
x
sorption sites. Of M–ZrO2–Al2O3 samples investigated, ruthenium as well as Pt demonstrated relatively good performance as a catalyst component in the sorbent. The FT-IR spectra after sorption of NO and NO2 demonstrated a strong band attributed to stored nitrate ions. The Pt catalyst was more resistant to sulfur poisoning than a base metal catalyst. However, the NO
x
sorptive capacities of the Pt–ZrO2/Al2O3 sorbents were expected to be deteriorated in dilute SO2 as far as observed from FT-IR spectra. 相似文献
4.
Masaharu Hatano 《Catalysis Surveys from Asia》2003,7(4):281-285
Rhodium—alumina-mixed oxides have been investigated as catalysts for selective catalytic reduction of NO
x
by propene, as a part of the R&D Project of Next Generation Catalysts Research Institute. The results indicated that the NO
x
reduction activity increases with a decrease in the reducibility of rhodium, suppressing wasteful consumption of propene by the reaction with oxygen. Coprecipitation method for the preparation of Rh-alumina catalysts was effective for the formation of the less-reducible rhodium sites, and the addition of zirconium and gallium further enhanced the formation of those sites and increased the selectivity of NO
x
reduction. 相似文献
5.
随着稀薄燃烧(lean-burn)发动机的推广使用和环保法规的日趋严格,消除稀燃尾气中的氮氧化物(N O x)已刻不容缓。N O x储存还原技术被认为是最具应用前景的方法之一[1,2]。目前,对Pt/BaA l2O4-A l2O3体系中N O x储存与还原机制的研究较多[1 ̄4],但对该体系中微量铂物种微观结构及其与性能的关系研究较少,这主要是由于Pt含量(0.1w t% ̄0.5wt%)太低,分散度较高,使表征方法受到很大限制。本文采用共沉淀-浸渍法制得具有较高比表面积和热稳定性的N O x储存还原催化剂Pt/BaA l2O4-A l2O3,应用荧光X-射线吸收精细结构方法(Fluores-cence-… 相似文献
6.
我们研究了4种负载型Pt催化剂(1Pt/NiO、1Pt/FeOx、1Pt/Co3O4和Pt/CeO2)上不同反应条件下CO氧化活性及抗H2O和CO2性能.发现反应气氛中CO2的加入与CO形成了竞争吸附,并在催化剂表面形成了碳酸盐物种堵塞了活性位,从而导致催化剂失活.反应气氛中H2O的加入对1Pt/CeO2催化剂的活性有所抑制,但对1Pt/FeOx、1Pt/NiO和1Pt/Co3O4催化剂的活性却有促进作用.在1Pt/FeOx和1Pt/CeO2催化剂上的分步反应实验和动力学研究表明,尽管H2O的加入在两种催化剂上均与CO形成了竞争吸附,但在1Pt/FeOx催化剂上H2O在载体表面解离形成的羟基更易与CO反应,开辟了新的反应途径,从而提高了反应性能.此外,H2O的加入能有效分解该催化剂上的碳酸盐物种,从而保持了其稳定性. 相似文献
7.
研究了以多孔二氧化硅微球和活性炭为载体制备NOx吸附/还原催化剂的方法,摸索了最佳Ce/Co物质的量的比例。采用低温氮吸附方法测定了样品的BET比表面和孔容,利用XRD方法表征了样品中所掺杂的金属元素的晶型。研究发现:当nCe/nCo=75/25时,材料获得最佳NOx吸附能力,当以多孔二氧化硅微球作载体时,材料对于NOx的吸附主要来自CoOx和CeO2的二元氧化物;当以活性炭作为载体时,活性炭参与了NOx的吸附,因此其吸附容量大大提高。对NOx的吸附机理进行了探讨,并研究了样品的NH3还原性质。 相似文献
8.
9.
本文采用溶胶凝胶法制备了一系列不同Ca含量的钙钛矿型氧化物La1-xCaxMnO3(x=0~0.4)纳米颗粒, X射线粉末衍射及精修、扫描电镜表征显示其相纯度和结晶度高, 颗粒平均粒径约40 nm。在0.1 mol·L-1 KOH水溶液中进行的氧还原电催化性能测试显示, La0.7Ca0.3MnO3样品催化活性最高, 表观电子转移数接近4, 还原电流密度与Pt/C催化剂相当, 而催化稳定性优于Pt/C。进一步研究了La1-xCaxMnO3样品中Mn价态、晶胞参数的改变对氧还原催化活性的影响, 结果表明当x=0.3时, 催化剂中Mn处于混合价态, Mn-O键长适中, 最有利于电催化反应。 相似文献
10.
Xiaoying Bao Muhammad Arif Malik Daniel G. Norton Vasile B. Neculaes Karl H. Schoenbach Richard Heller Oltea P. Siclovan Susan E. Corah Antonio Caiafa Louis P. Inzinna Kenneth R. Conway 《Plasma Chemistry and Plasma Processing》2014,34(4):825-836
The nonthermal plasma generated in a shielded sliding discharge reactor was used to reform diesel for the hydrocarbon-selective catalytic reduction (HC-SCR) of NOx on Ag/Al2O3 catalysts. Compared with raw diesel, the reformed diesel enhanced the NOx reduction efficiency, mitigated hydrocarbon poisoning of the catalyst and reduced the fuel penalty for the HC-SCR reaction. The NOx conversion values obtained with a commercial Ag/Al2O3 catalyst exceeded that of a 2.0 wt% Ag/Al2O3 catalyst prepared by wet impregnation. A significant amount of NH3 was produced as a by-product during the HC-SCR reaction, which suggests that further NOx conversion enhancement can be achieved by placing a second NH3-SCR catalyst in series with the Ag/Al2O3 catalyst. 相似文献
11.
本文采用溶胶凝胶法制备了一系列不同Ca含量的钙钛矿型氧化物La1-xCaxMnO3(x=0~0.4)纳米颗粒,X射线粉末衍射及精修、扫描电镜表征显示其相纯度和结晶度高,颗粒平均粒径约40 nm。在0.1 mol.L-1KOH水溶液中进行的氧还原电催化性能测试显示,La0.7Ca0.3MnO3样品催化活性最高,表观电子转移数接近4,还原电流密度与Pt/C催化剂相当,而催化稳定性优于Pt/C。进一步研究了La1-xCaxMnO3样品中Mn价态、晶胞参数的改变对氧还原催化活性的影响,结果表明当x=0.3时,催化剂中Mn处于混合价态,Mn-O键长适中,最有利于电催化反应。 相似文献
12.
Xia J. F. Gao X. X. Kong J. Y. Hui H. X. Cui M. Yan K. P. 《Plasma Chemistry and Plasma Processing》2000,20(2):225-233
NOx are main toxic by-products in the effluent gas whendecomposing volatile organic compounds in air by a packed-bed plasmareactor. Several types of materials such as 13X zeolite, BaTiO3and Pd/Pt catalysts have been selected to be packed in the reactor, andmethane decomposition and NOx by-products in discharged gases areinvestigated at different range of reaction temperature and dischargeenergy density at atmospheric pressure. The ratios of methane decompositionpercentage/NOx concentration are used to assess these packed bedmaterials and reaction conditions. The results show that usingPd/-Al2O3 with lower percentage Pd as packedbed, and discharging with lower discharge density at higher reactiontemperature can reduce NOx output effectively and greatly improveperformance of the reactor. 相似文献
13.
Lingchao Jiang Huizi Gu Xingzhong Xu Xinhuan Yan 《Journal of molecular catalysis. A, Chemical》2009,310(1-2):144-149
Carbon nanotubes (CNTs), γ-alumina (γ-Al2O3) and silica (SiO2) supported Pt and Pd catalysts were produced by laser vaporization deposition of respective bulk metals. The catalysts were characterized by inductive coupled plasma emission spectrometer (ICP), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The catalytic properties of the catalysts were investigated in the liquid phase hydrogenation of o-chloronitrobenzene (o-CNB) to o-chloroaniline (o-CAN) under 333 K and 1.0 MPa hydrogen pressure. The results show that the catalytic properties are greatly affected by the supports. Pt/CNTs catalyst exhibits the best catalytic performance among the Pt-based catalysts, producing o-CAN with 99.6% selectivity at complete conversion. Pd/CNTs catalyst exhibits the best catalytic performance among the Pd-based catalysts, giving o-CAN with 95.2% selectivity at complete conversion. For Pt-based catalysts, geometric effect and the textures and properties of the supports play important roles on catalytic properties. On the other hand, geometric effect, electronic effect and the textures and properties of the supports simultaneously influence the catalytic properties of the Pd-based catalysts. In addition, hydrogenolysis of the C–Cl bond can be well inhibited over all catalysts prepared by laser vaporization deposition. 相似文献
14.
Yi-Fan Zheng Hua-Zhang Liu Zong-Jian Liu Xiao-Nian Li 《Journal of solid state chemistry》2009,182(9):2385-2391
The temperature-programmed reduction process of two types of industrial ammonia-synthesis catalysts, A110 and ZA-5, which are, respectively, based on Fe3O4 and Fe1−xO precursors, were studied by in situ X-ray power diffraction (XRD). It has been found that the ZA-5 has lower reduction temperature and faster reduction rate, and its active phase α-Fe possesses a higher value of lattice microstrain than A110. The simulation based on Rietveld refinement has also shown that the shape of α-Fe grain of ZA-5 has a mixed shape of cube and sphere with more exposing (111) and (211) planes, while that of A110 looks like a concave cube with more exposing (110) planes. Based on the results obtained, a growth model of α-Fe during the reduction of Fe3O4- and Fe1−xO-based ammonia-synthesis catalysts is proposed, and the origins for the activity difference has been also discussed. 相似文献
15.
采用多种物理化学手段研究了在模拟的轻型柴油车尾气中不同Co担载量及Cu掺杂的Co/ZSM-5催化剂的Co组分分散状态、可还原性、NO吸附脱附性质对C3H8选择性催化还原NOx性能的影响。结果表明,浸渍法制备的Co/ZSM-5催化剂上既有外表面上的Co3+和Co2+物种,也有孔内的Co2+离子。富氧条件下Co/ZSM-5催化剂上C3H8选择性催化还原NOx的活性主要与ZSM-5载体孔外表面分散的CoOx物种中的钴离子可还原能力和NO吸附脱附性能密切相关。Co/ZSM-5催化剂上适宜的Co担载量约为4.0wt%,低担载量时随Co担载量增加,表面CoOx物种中钴离子可还原能力增强,C3H8选择性催化还原NOx的低温转化活性增加;高担载量时,随Co担载量增加,单位Co离子的NO吸附量的减少以及催化剂表面活性中心数的减少,导致了Co/ZSM-5催化剂NOx的转化率和催化剂比速率(k)的下降。孔外表面Co3O4晶体的存在使催化剂表面产生较强的NO吸附,并在高温时有利于C3H8的氧化燃烧,使C3H8选择性催化还原NOx的活性降低。 相似文献
16.
采用多种物理化学手段研究了在模拟的轻型柴油车尾气中不同Co担载量及Cu掺杂的Co/ZSM-5催化剂的Co组分分散状态、可还原性、NO吸附脱附性质对C3H8选择性催化还原NOx性能的影响。结果表明,浸渍法制备的Co/ZSM-5催化剂上既有外表面上的Co3+和Co2+物种,也有孔内的Co2+离子。富氧条件下Co/ZSM-5催化剂上C3H8选择性催化还原NOx的活性主要与ZSM-5载体孔外表面分散的CoOx物种中的钴离子可还原能力和NO吸附脱附性能密切相关。Co/ZSM-5催化剂上适宜的Co担载量约为4.0wt%,低担载量时随Co担载量增加,表面CoOx物种中钴离子可还原能力增强,C3H8选择性催化还原NOx的低温转化活性增加;高担载量时,随Co担载量增加,单位Co离子的NO吸附量的减少以及催化剂表面活性中心数的减少,导致了Co/ZSM-5催化剂NOx的转化率和催化剂比速率(k)的下降。孔外表面Co3O4晶体的存在使催化剂表面产生较强的NO吸附,并在高温时有利于C3H8的氧化燃烧,使C3H8选择性催化还原NOx的活性降低。 相似文献
17.
以四丁基氢氧化铵作为相转移剂,以硼氢化钠为还原剂,利用相转移法在二氯甲烷中制备了一系列不同比例的Pd_xMo/C(Pd/Mo的原子比x=1、2、3、4、5)催化剂。透射电镜(TEM)图像显示,Pd_x Mo/C是呈2~4 nm的圆形颗粒,尺寸均匀、分散性良好。X射线衍射(XRD)结果表明,加入第二组元Mo后,Pd的晶格发生扩张,调节了 Pd的几何结构。此外,X射线光电子能谱(XPS)结果表明,相对于Pd/C,Pd_4Mo/C的Pd3d_(5/)2结合能负移了 0.50 eV,说明电负性较大的Pd从Mo吸电子,电子结构发生改变。氧还原反应(ORR)结果表明,不同比例的Pd_xMo/C催化剂活性均优于Pd/C,其中当x=4时,ORR活性最佳,其起始电位和半波电位分别为0.876和0.813 V,高于商业Pt/C的0.870和0.810 V。此外,在经过3 h的运行之后电流密度仍保留82.9%,与商业Pt/C相比具有明显的优势。 相似文献
18.
研究了低于300 ℃时两种氧化铈对稀燃阶段NOx存储性能的影响,催化剂由2%(w)Pt/Al2O3(PA)与CeO2-X(X=S,I)机械混合制备. X射线衍射(XRD),BET表面积和扫描电子显微镜(SEM)用于表征材料的物理结构. X射线光电子能谱(XPS)和H2程序升温还原(H2-TPR)用于表面Ce3+和活性氧定量. 原位漫反射傅里叶变换红外光谱(in-situ DRIFTS)用于分析表面NOx吸附物种. 相比于CeO2-I,CeO2-S 具有优良的物理化学性能,包括高比表面积、丰富的空隙结构、较高的抗老化能力及表面Ce3+浓度. 因而,Pt/Al2O3+CeO2-S 表现出优异的NOx存储能力. 此外,PA+CeO2-X(X=S,I)上存在Pt 与CeO2之间的相互作用,可提高表面氧物种的活性进而促进NO氧化及NOx存储. PA+CeO2-S上的这种相互作用要强于PA+CeO2-I. 研究表明,表面Ce3+浓度和活性氧含量对NOx存储起到重要作用. 然而经过水热处理后,Pt 与老化的氧化铈(ACS,ACI)之间的相互作用降低,并且两种氧化铈NOx存储性能显著下降. 另外,与PA+ACS(ACI)相比,PA+PACS(PACI)样品NOx存储能力得到改善,这归因于表面氧物种活性增加能促进硝酸盐的形成. 相似文献
19.
Lee Ju-No Lee Jin-Suk Shin Chul-Seung Park Soon-Chul Kim Seung-Wook 《Applied biochemistry and biotechnology》2000,84(1-9):329-342
Possible methods to minimize the toxic effects of SO
x
and NO
x
on the growth of a highly CO2 tolerant and fast-growing microalga, Chlorella sp. KR-1, were investigated. Maintaining the pH of the culturing media at an adequate value was quite important to enhancing
the tolerances of the microalgae to SO
x
and NO
x
. Controlling the pH by adding an alkaline solution, using a low flow rate of gas fed to the culture, and using a high concentration
of inoculating cells were effective methods to maintaining the proper pH of the culture. Controlling the pH was the most effective
method but could be applied only for some specific microalgae. 相似文献
20.
M. Yu. Smirnov A. V. Kalinkin V. I. Bukhtiyarov 《Journal of Structural Chemistry》2007,48(6):1053-1060
The reactions of the platinum and rhodium model catalysts applied to aluminum oxide with NOx (10 Torr NO + 10 Torr O2) were studied by X-ray photoelectron spectroscopy. The reaction conducted at room temperature formed on the surface of the oxide support the NO 3,s ? nitrate ions characterized by the N1s line at 407.4 eV and O1s line at 533.1 eV and the NO 2,s ? nitrite ions characterized by the N1s line with a binding energy of 404.7 eV. At the same time, the Pt4f and Rh3d lines of the supported platinum particles are shifted toward higher binding energies by 0.5–1.0 eV and 0.7–1.2 eV, respectively. It is assumed that the binding energies increase due to changes in the chemical state of the platinum metal in which oxygen is dissolved. The reaction of NOx with Pt/Al2O3 at 200°C forms platinum oxide defined by the Pt4f 7/2 line with a binding energy of 72.3 eV. 相似文献