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1.
采用调节前驱体溶液pH值的方法制备了用于低温NH3-SCR的V2O5-WO3/Ti O2催化剂。通过XPS、Raman光谱、H2-TPR、NH3-TPD、NH3-DRIFT、XRD及物理吸附等手段对催化剂进行了表征分析,并对其脱硝催化活性进行了测试。结果表明,前驱体溶液酸性的增强能够提高催化剂表面聚合态钒物种和V4+(3+)/V5+的比值以及表面酸性,增加活性位数量、降低反应的活化能、提高其脱硝催化性能。因此,通过提高前驱体溶液的酸性,有助于制备出脱硝活性较好的NH3-SCR催化剂。  相似文献   

2.
通过改进液相沉淀法制备纳米Ce O2,在沉淀过程中加入一种可完全燃烧的炭黑微粉,该微粉可将沉淀产生的前驱体粒子吸附在其表面,减小前驱体相互接触面积,大幅降低纳米Ce O2干燥、焙烧过程的团聚程度。实验选择Ce(NO3)3溶液浓度为100 g·L-1,80℃水浴滴加稀释NH3·H2O至p H为9~10,经沉降、洗涤、过滤、干燥可获性能稳定的前驱体。研究了碳黑添加量、煅烧温度与煅烧时间对Ce O2粒径的影响,发现控制制备条件,可获得分散性能良好、结晶完整的不同粒径的微纳米Ce O2粒子。  相似文献   

3.
影响纳米CeO2沉淀法合成的工艺因素研究   总被引:13,自引:1,他引:12  
以Ce(NO3)3·6H2O为铈源, (NH4)2CO3·H2O为沉淀剂, 加入少量表面活性剂作分散剂, 采用液相沉淀法成功合成了纳米CeO2. 研究了反应温度、反应时间、搅拌速率、表面活性剂种类及用量、焙烧温度和焙烧时间等因素对纳米CeO2晶粒尺寸和相对密度的影响, 得出优化工艺条件, 通过XRD, DTA/TG, TEM, BET比表面积、 N2等温吸附与脱附、 BJH脱附孔径分布及杂质含量分析等方法对合成产品性能进行了表征. 结果表明 采用浓度为0.1 mol·L-1的(NH4)2CO3·H2O溶液快速倒入浓度为0.1 mol·L-1 的Ce(NO3)3·6H2O溶液中以化学计量比进行反应, 同时加入0.4% (质量分数) PEG4000, 反应时间为10 min, 反应温度为40 ℃, 搅拌速率为800 r·min-1, 经水洗、醇洗、脱水和真空干燥后所得的前驱体于300 ℃的空气中焙烧1 h, 该条件下合成的CeO2属于立方晶系, 空间群为Fm3m, 原生晶粒粒径为5 nm左右, 颗粒粒径为20 nm以下, 比表面积达140.61 m2·g-1, 孔径分布为5~15 nm, 孔径峰值为9.3 nm, 纯度≥99.97%.  相似文献   

4.
以ZrO(NO3)2·2H2O为前驱体对多壁碳纳米管(MWCNTs)进行了改性并负载MnOx制备了MnOx/ZrO2/MWCNTs催化剂.考察了Zr对催化剂低温选择性催化还原(SCR)反应活性的影响,并通过多种分析手段对催化剂的结构进行了表征.结果表明Zr的添加对催化剂的低温SCR活性具有显著的促进作用,当Zr负载量为30%时,催化剂活性最佳.X射线衍射(XRD)、拉曼(Raman)光谱、透射电镜(TEM)、N2吸附-脱附的表征结果分析表明,适量的Zr改性促进了MnOx在载体表面的分散,增强金属氧化物与MWCNTs之间的作用,也能增加催化剂的比表面积、孔容和孔径.X射线光电子能谱(XPS)、H2程序升温还原(H2-TPR)和NH3程序升温脱附(NH3-TPD)的分析结果则显示,Zr能提高催化剂表面化学吸附氧浓度,促进Mn3+转化为Mn4+,从而使催化剂表面的活性位点增多,氧化还原能力增强,同时还提高了催化剂表面酸性位点的数量和强度,促进了NH3的吸附,是MnOx/ZrO2/MWCNTs催化剂低温SCR活性提高的主要原因.  相似文献   

5.
粒径可控球形TiO2的制备   总被引:3,自引:1,他引:2  
在正丙醇与水的混合溶剂体系中以Ti(SO4)2为前驱物制备得到了粒径分布窄,分散性好的球形TiO2.对表面活性剂种类及用量,反应物浓度及焙烧温度和时间等影响因素进行了研究,结果表明,在正丙醇与水的体积比为1∶1的条件下,以聚乙烯吡咯烷酮(PVP)为表面活性剂,温度为70-90℃时可制得粒径分布窄、分散性好的高质量的球形TiO2颗粒.通过TG-DSC、SEM、XRD等分析表明,颗粒粒度大小及粒径分布受表面活性剂浓度和反应前驱物浓度影响大;物相间的转化主要由焙烧温度和时间来决定.并引入LaMer模型对颗粒形核、长大的过程进行理论说明.  相似文献   

6.
氮氧化物(NOx)作为主要的大气污染物之一,给环境和人类带来一定危害,其主要源于汽车、轮船以及工厂中液态(汽油和柴油)或固态(煤)化石原料的燃烧.目前,选择性催化还原法(SCR)因技术相对成熟且经济有效,被广泛应用于氮氧化物脱除.催化剂是该技术的关键,而典型的商业钒系催化剂(V2O5-WO3/TiO2和V2O5-MoO3/TiO2)存在工作窗口温度窄(300–400 ℃)、V2O5的生物毒性以及较高的SO2氧化性能等缺点,因此开展高效且环境友好催化剂的研究工作迫在眉睫.近年来,锰基催化剂因其丰富的价态变化以及氧化形态而受到科研工作者的广泛关注.研究者已经对锰前驱体做了大量研究,但是关于不同锰前驱体制备得到的催化剂的活性物种组成以及催化活性往往存在着不同观点.因此进一步开展对锰前驱体研究仍有必要.同时,二氧化钛载体比表面积较小,并不是制备锰基催化剂的理想载体.分子筛载体因其比表面积大、特殊的孔道结构以及丰富的酸位等特点引起了研究者的关注.用于制备锰基催化剂的分子筛载体主要有ZSM-5,Beta,USY和SAPO等,其中ZSM-5系列催化剂是研究热点.另一方面,研究发现Beta分子筛具有良好的水热稳定性,被认为是理想的NH3-SCR催化剂载体.研究者对比了不同金属负载的Beta分子筛与ZSM-5分子筛的催化活性,结果表明,Fe/beta的催化活性高于Fe/ZSM-5和Fe/ZSM-11; Cu/beta的催化活性与Cu/ZSM-5相当,均表现出较高的活性.而关于Mn/ZSM-5的研究已有大量文献报道,但关于Mn/beta的研究相对较少.另外,关于不同锰前驱体在Beta以及ZSM-5分子筛载体表面的物化性质差异也少有报道.本文以H/beta和H/ZSM-5分子筛作为载体,采用硝酸锰、乙酸锰和氯化锰三种前驱体,通过湿法浸渍制备了Mn/beta和Mn/ZSM-5两类NH3-SCR催化剂,并在固定床管式反应器中对比评价了两类催化剂的催化活性.凭借氮气等温吸附/脱附(BET)、X射线衍射(XRD)、X射线荧光(XRF)、氢气程序升温还原(H2-TPR)、氨气程序升温脱附(NH3-TPD)以及X射线光电子能谱(XPS)等技术对催化剂进行了表征,系统分析了不同前驱体在两种载体表面形成的活性组分以及理化性质对催化性能的影响.催化剂活性评价结果表明,对于Mn/beta和Mn/ZSM-5催化剂,在220–350 ℃反应温度区间内,乙酸锰和硝酸锰制备的催化剂NO脱除率均在80%以上.其中Mn/beta-Ac在240 °C时达到最高的NO脱除率97.5%,并且在220–350 ℃温度区间内保持着90%以上的活性,具有最宽的活性温度窗口.同时,在两系列锰基催化剂中,乙酸锰制备的催化剂均表现出最佳的催化活性,且对于同一种前驱体制备的催化剂,Mn/beta催化剂的NH3-SCR活性优于Mn/ZSM-5.BET数据显示,负载锰物种之后,催化剂的比表面积和孔体积均明显减小,但相对于Mn/ZSM-5催化剂,Mn/beta催化剂仍保持着优良的织构性质.XRD、XRF及H2-TPR结果表明,氯化锰前驱体主要产生少量的结晶Mn3O4并且大部分保持以MnCl2的形式存在,这也是此类催化剂表现出较差的低温催化活性的原因.结合XPS表征分析了催化剂的表面性质.结果表明,硝酸锰前驱体主要产生结晶MnO2和少量未分解的硝酸锰,乙酸锰前驱体主要产生高度分散的无定形MnO2和Mn2O3混合物以及结晶Mn3O4.进一步结合NH3-TPD分析结果以及活性评价结果可以得出: 丰富的无定形MnOx(MnO2和Mn2O3)物种、较高的表面锰含量和表面活性氧基团以及适当含量的弱酸位有利于提升催化剂的低温NH3-SCR催化活性.  相似文献   

7.
粒径可控球形TiO2的制备   总被引:2,自引:0,他引:2  
在正丙醇与水的混合溶剂体系中以Ti(SO4)2为前驱物制备得到了粒径分布窄, 分散性好的球形TiO2. 对表面活性剂种类及用量, 反应物浓度及焙烧温度和时间等影响因素进行了研究, 结果表明, 在正丙醇与水的体积比为1:1的条件下, 以聚乙烯吡咯烷酮(PVP)为表面活性剂, 温度为70-90 ℃时可制得粒径分布窄、分散性好的高质量的球形TiO2颗粒. 通过TG-DSC、SEM、XRD等分析表明, 颗粒粒度大小及粒径分布受表面活性剂浓度和反应前驱物浓度影响大; 物相间的转化主要由焙烧温度和时间来决定. 并引入LaMer模型对颗粒形核、长大的过程进行理论说明.  相似文献   

8.
王晖  段连运  谢有畅 《催化学报》2007,28(8):730-736
分别以Ba(NO3)2和Ba(CH3COO)2为Ba的前驱体,利用浸渍法制备了两个系列不同Ba含量的NOx存储还原催化剂Ba/(Pt/γ-Al2O3).采用X射线衍射、X射线光电子能谱、程序升温反应脱附和差热-热重等分析技术对样品进行了表征,并考察了催化剂的NOx存储性能.结果表明,不同前驱体在Pt/γ-Al2O3载体表面的分散能力不同.前驱体为Ba(NO3)2时,Ba的分散阈值为0.047 g/g(Ba/(Pt/γ-Al2O3)质量比),而前驱体为Ba(CH3COO)2时,Ba的分散阈值为0.149 g/g(Ba/(Pt/γ-Al2O3)质量比).经高温焙烧后,前驱体的分散容量决定催化剂中Ba物种的分散容量.在NOx存储性能评价实验中,以Ba(CH3COO)2为前驱体时,催化剂的NOx等温吸附穿透时间最长为23 min,而以Ba(NO3)2为前驱体时,具有相同Ba含量的催化剂的穿透时间为13 min.因此,在制备NOx存储还原催化剂时,选择易分散的前驱体Ba(CH3COO)2可以获得较高的NOx存储活性的催化剂.  相似文献   

9.
朱学成  沈如伟  张利雄 《催化学报》2014,35(10):1716-1726
采用一步法将原硅酸四乙酯与3-氨丙基三乙氧基硅烷在表面活性剂P123作用下,酸性共水解制备出氨基功能化的介孔分子筛SBA-15(NH2-SBA-15),再利用其中氨基与水杨醛的缩合反应制备SBA-15固载的席夫碱,该席夫碱与Cu(NO3)2溶液反应最终制成固定于SBA-15的Cu(II)席夫碱配合物多相催化剂Cu-SBA-15.采用X射线衍射、红外光谱仪、紫外可见分光光度计、场发射电镜、透射电镜、N2吸附-脱附、元素分析、原子发射光谱和热重分析对催化剂进行了表征,并将此催化剂用于无有机溶剂条件下催化氧化苯乙烯制备苯甲醛,考察了反应时间、反应温度、H2O2用量、水的用量、催化剂用量对反应的影响.当反应温度为100°C,反应时间8 h,H2O2与苯乙烯的摩尔比为2:1,不额外添加溶剂,且催化剂用量为3.8 wt%时,苯乙烯的转化率最高为84.4%,苯甲醛选择性为83.9%,催化剂的TOF值为261.1 h–1,并且重复使用3次后活性没有明显下降.规则的孔道、较大的比表面积以及分布均匀的活性中心可能是催化剂活性提高的原因.  相似文献   

10.
Na2WO4·2H2O-H2O2催化氧化苯甲醛制备苯甲酸   总被引:4,自引:0,他引:4  
以30%H2O2为氧源,Na2WO4·2H2O催化氧化苯甲醛制备苯甲酸.考察了H2O2用量,反应时间,催化剂和酸性添加物(硫酸氢钠)对苯甲酸收率的影响和在非酸性环境下,表面活性剂对苯甲酸收率的影响.结果表明,加入非离子表面活性剂能有效的提高苯甲酸的收率,特别是添加β-环糊精,苯甲酸的收率达90.03%.  相似文献   

11.
The effect of vinyltriethoxysilane (VTES) addition on the pyrolytic conversion of tetraethoxysilane (TEOS) based silica gel had been studied. Thermogravimetric analysis coupled with mass spectroscopy was carried out to study the thermal decomposition behavior of precursor gels. The ceramic yield of precursor gels was decreased with the increase of the VTES content. 29Si magic angle spinning nuclear magnetic resonance indicated that the incorporation of VTES into TEOS not only changed the composition and structure of precursor gels, but also increased carbon-enriched SiO x C4?x units of silicon oxycarbide ceramics during the pyrolysis conversion. The carbon content of SiOC ceramic was almost unchanged between 1,000 and 1,500 °C. However, the O/Si ratio of the silicon oxycarbide ceramic was reduced and the free carbon content was increased with the increasing molar ratios of VTES/TEOS. Moreover, the carbothermal reduction reaction led to the free carbon content decreased with the increase of the sintering temperature.  相似文献   

12.
Stable emulsions of a core–shell acrylic copolymer (non-crosslinkable V0, and crosslinkable V2, V4, V6, and V8, where the numbers indicate the wt% of crosslinking agent based on the total acrylate monomer content) containing butyl acrylate (BA, 45 wt%), glycidyl methacrylate (GMA, 45 wt%), heptadecafluorodecyl methacrylate (PFA, 10 wt%), and various contents of crosslinking agent (vinyltriethoxysilane, VTES) were synthesized using a three-stage seeded emulsion polymerization process with a small amount of surfactant. The average particle size and viscosity of emulsions increased significantly with increasing VTES content. This study examined the effects of the VTES content on the surface/mechanical properties of self-crosslinked copolymer film samples containing a fixed acrylate monomer content to find the optimum VTES content. XPS showed that the film–air surface of the copolymer samples had a higher fluorine/silicone content than the film–dish interface. The tensile strength/modulus, thermal stability, and two Tgs (α and β Tgs) of the film samples increased significantly with increasing VTES content. The contact angle of the film samples increased with increasing VTES content up to approximately 6 wt%, and then decreased slightly. The optimum VTES content was approximately 6 wt% based on the total acrylate monomer content to obtain a high water/oil repellent coating material (V6) with the highest water/methylene iodide-contact angles (118.2°/81.8°) and lowest surface energy (18.4 mN/m).  相似文献   

13.
Monodispersed ??-Fe2O3 nanoparticles modified by sodium dodecylbenzene sulfonate (SDBS) surfactant and assisted by glycerol have been successfully synthesized via a hydrothermal process using FeCl3·6H2O as the starting precursor. These nanoparticles possess good crystallinity and have an average particle size of 100 nm. The as-prepared products are characterized by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, and a superconducting quantum interference device magnetometer. SDBS and glycerol played an important role in controlling the final morphology of the products. Magnetic hysteresis measurements reveal that monodispersed ??-Fe2O3 nanoparticles exhibit normal ferromagnetic behaviors with the remanent magnetization and coercivity of 0.2389 emu/g and 2339.0 Oe at room temperature.  相似文献   

14.
In studying 2,2,6,6‐tetramethy‐1‐piperidinyloxy (TEMPO)‐mediated styrene miniemulsions, we have observed that the surfactant sodium dodecylbenzenesulfonate (SDBS) not only provides colloidal stability but also influences the rate of polymerization. Increasing the SDBS concentration results in higher polymerization rates, although the molecular weight distribution and particle size distribution are not significantly impacted. We have also examined another common sulfonate surfactant, DOWFAX 8390. In contrast to SDBS, DOWFAX 8390 does not affect the polymerization rate. Furthermore, DOWFAX‐stabilized polymerizations are slower than SDBS‐stabilized polymerizations. TEMPO‐mediated bulk styrene polymerizations are also accelerated significantly in the presence of SDBS. Although the mechanism for the rate acceleration is unknown, the experimental evidence suggests that SDBS is participating in the generation of radicals capable of propagating, thereby reducing the TEMPO concentration within the particles. © 2006 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 44: 5974–5986, 2006  相似文献   

15.
The droplet size distribution (DSD) of emulsions is the result of two competitive effects that take place during emulsification process, i.e., drop breakup and drop coalescence, and it is influenced by the formulation and composition variables, i.e., nature and amount of emulsifier, mixing characteristics, and emulsion preparation, all of which affect the emulsion stability. The aim of this study is to characterize oil-in-water (O/W) emulsions (droplet size and stability) in terms of surfactant concentration and surfactant composition (sodium dodecyl benzene sulphonate (SDBS)/Tween 80 mixture). Ultraviolet-visible (UV-vis) transmission spectroscopy has been applied to obtain droplet size and stability of the emulsions and the verification of emulsion stability with the relative cleared volume technique (time required for a certain amount of emulsion to separate as a cleared phase). It is demonstrated that the DSD of the emulsions is a function of the oil concentration and the surfactant composition with higher stability for emulsions prepared with higher SDBS ratio and lower relative cleared volume with the time. Results also show that smaller oil droplets are generated with increasing Tween 80 ratio and emulsifier concentration.  相似文献   

16.
Gadolinium doped ceria (Gd–CeO2) nanoparticles have been synthesized by an reverse microemulsion system using cyclohexane as the oil phase, a non-ionic surfactant Igepal CO 520 and their mixed aqueous solutions of gadolinium III nitrate hexahydrate and cerium III nitrate hexahydrate as the water phase. The control of particle size was achieved by varying the water to surfactant molar ratio. The synthesized and calcined powders were characterized by thermogravimetry-differential thermal analysis (TGA-DTA), X-ray diffraction analysis (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), Fourier transform infrared spectroscopy (FTIR) and Raman spectroscopy. The XRD results show that all the samples calcined at 700 °C were single phase cubic fluorite structure. The average size of the particle was found to increase with increase in water to surfactant molar ratio (R). The mean diameter of the particle for various value of R varies between 8–15 nm (SEM) and 7.5–11 nm (TEM), respectively. EDS confirm the presence of gadolinia and ceria phase in the nanopowder calcined at 700 °C. FTIR analysis was carried to monitor the elimination of residual oil and surfactant phases from the microemulsion-derived precursor and calcined powder. Raman spectroscopy and DTA evidenced the formation of a solid solution of gadolinium doped ceria at room temperature.  相似文献   

17.
Fe-doped TiO2 catalyst was prepared by wet impregnation, using TiO2 P25 Degussa as a precursor and Fe(NO3)3 as a dopant, followed by irradiation with an electron beam or γ-rays. Surface properties of Fe/TiO2 samples were examined by BET, XRD, ToF-SIMS, and TPR methods. The photocatalytic activity towards destruction of the anionic surfactant, sodium dodecylbenzenesulfonate (SDBS), in aqueous solutions was higher for the irradiated Fe/TiO2 catalysts than for bare TiO2 P25 or that calcined at 500 °C. The results show that irradiated catalysts exhibit a more uniform texture with high dispersion of iron species. An enhancement of the activity of irradiated Fe/TiO2 systems can be attributed to the synergetic effects of small crystallite size and homogenous distribution of iron species including FeTiO3 phase.  相似文献   

18.
New natural polymer-based aerogels, cross-linked chitosan aerogels, were prepared by the sol-gel route with glutaradehyde, glyoxal, and formaldehyde as cross-linkers. The alcogels were dried by supercritical carbon dioxide (CO2) fluid extraction. The resulting materials were characterized using scanning electron microscopy (SEM), nitrogen adsorption/desorption analysis, and Fourier transform infrared (FT-IR) spectroscopy. Furthermore, the adsorption of the anionic surfactant sodium dodecylbenzene-sulfonate (SDBS) from aqueous solution by the materials was investigated. The aerogels exhibit high adsorption capability, can remove SDBS from acidic aqueous solutions, and have potential applications in controlling SDBS pollution.  相似文献   

19.
Mesoporous platinum–palladium alloy films with different compositional ratios have been successfully synthesized by electrochemical plating in aqueous surfactant solutions. Scanning electron micrographs and transmission electron micrographs reveal that all of the platinum–palladium alloy films possess uniform mesopores with a narrow size distribution (around 7 nm). The alloy compositions in the pore walls can be controlled by changing the compositional ratios in the precursor solutions, as confirmed by inductively coupled plasma mass spectroscopy analysis and X‐ray photoelectron spectroscopy measurements. Due to large surface areas, the prepared mesoporous platinum–palladium films show distinctly enhanced electrocatalytic activity for methanol oxidation reactions, compared with the commercially available platinum black catalyst. Furthermore, compared with mesoporous platinum film, the alloying of platinum with palladium has a critical effect on the enhanced electrocatalytic activity. In particular, a mesoporous Pt82–Pd18 film exhibits highly enhanced electrocatalytic activity.  相似文献   

20.
杨智  沈亚云  周娥  魏成玲  秦好丽  田娟 《电化学》2020,26(1):130-135
采用热解法制备FeN/C催化剂,考察催化剂前驱体中氮含量对其氧还原活性的影响. 使用X射线衍射、比表面积和孔径分布测试、透射电子显微镜以及热重分析等方法对催化剂的结构、形貌及催化剂前驱体的热性质等进行表征,使用线性扫描伏安法对催化剂的氧还原活性进行测试. 结果表明,以1,10-菲啰啉为氮源,FeCl3为铁源,Black Pearl 2000为载体,催化剂前驱体中1,10-菲啰啉含量为20wt%,Fe含量为1wt %时,热处理制备所得催化剂粒子分布均匀,比表面积为824.48 m 2·g -1,平均孔隙为10.58 nm,表面的氮元素含量为0.31wt%;并具有最好的氧还原催化活性.催化剂前驱体中氮源含量在热解过程中导致催化剂的比表面积、孔径结构及表面氮元素含量的变化是影响催化剂活性的关键因素.  相似文献   

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