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Shi-hua Wu Xiu-cheng Zheng Wei-ping Huang Shou-min Zhang Wei Wei Department of Chemistry Nankai University Tianjin China 《高分子科学》2001,(5):503-507
Supported An catalysts for low-temperature CO oxidation were prepared by solvated motal atom impregnation(SMAI) and conventional impregnation (CI). X-ray photoelectron spectroscopy (XPS) investigations indicated that theelemental gold in all the samples was in the metallic state. XRD measurements showed that the mean diameters of Auparticles prepared by SMAI were smaller than those prepared by CI with the same gold content. Catalytic tests showed thatthe SMAI catalyst had higher CO oxidation activity than the CI catalyst with the same compositions. Both SMAI and CIcatalysts exhibited high activity in low temperature CO oxidation. Full CO conversion was obtained at 323--383K. 相似文献
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Shi-hua Wu Bao-qing Li Wei-ping Huang Shou-min Zhang Juan Shi Xiu-cheng Zheng 《Reaction Kinetics and Catalysis Letters》2003,78(1):49-58
Supported Au catalysts for low-temperature CO oxidation were prepared by solvated metal atom impregnation (SMAI) and conventional
impregnation (CI). X-ray photoelectron spectroscopy investigations indicated that gold in all the samples was in the metallic
state. TEM and XRD measurements showed that the mean diameter of Au particles prepared by SMAI was smaller than that of those
prepared by CI with the same gold content. Catalytic tests showed that SMAI catalysts had higher CO oxidation activity than
CI catalysts with the same compositions. Both SMAI and CI Au/TiO2catalysts exhibited high activities in low temperature CO oxidation. Full CO conversion was obtained at 323 K for 3.1 wt.%
Au/TiO2 (SMAI) catalyst, which displayed higher activity than the 3.1 wt.% Au/D-72(SMAI) and 3.1 wt.% Au/TiO2(CI). Although the sizes of gold particles prepared by the same method and supported on both TiO2 and resin were comparable, the Au/TiO2 catalysts showed significantly higher activities than the Au/resin catalysts with the same Au contents under the same reaction
conditions. These results prove that not only the gold particle size, but also the support plays a key role in CO oxidation.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
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用元素分析、热脱附和H_2还原脱附等方法分析了Pd/γ-Al_2O_3、Pd/MgO、Pd/TiO_2溶剂化金属原子浸渍(SMAI)催化剂的表面组成和孔结构。结果表明Pd颗粒表面覆盖着一些有机碎片,这些碎片主要由C_1和少量C_2,C_3及C_3以上物种组成。SMAI催化剂的比表面积均高于相应纯载体的比表面积。而平均孔径均小于后者,CO_2甲烷化反应中,SMAI催化剂的活性均高于相应的普通浸渍法(CI)催化剂,而活化能却低于后者。在SMAI催化剂上CO_2甲烷化反应机理与Solymosi机理相同。 相似文献
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Li-hua Yu Shou-min Zhang Xianzhi Guo Da Wang Shu-rong Wang Shi-hua Wu 《Central European Journal of Chemistry》2007,5(1):144-155
The Co-Pd/SiO2 and Co-Cu/SiO2 catalysts were prepared via solvated metal atom impregnation (SMAI) method and investigated for the Fischer-Tropsch (F-T)
synthesis. The catalysts contained 5wt.% Co and a weight ratio of Pd (or Cu) to Co of 1/30. XPS indicated that Co, Pd and
Cu were in metallic state. The results of XPS and magnetic measurements showed that Co and Pd (Cu) were alloyed. The Co particles
on the catalysts were very highly dispersed and they displayed superparamagnetic behavior. FT-IR indicated that the electrons
shifted from Cu and Pd to Co. Catalytic tests showed that CO hydrogenation rates followed the order Pd-Co > Cu-Co > Co.
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为避免有机聚合物因热稳定性差而不能用高温氢气还原金属制备聚合物负载催化剂的弱点,采用溶剂化金属原子浸渍法在温和的条件下直接把零价金属负载在聚合物上,制备了几种不同金属含量的CoAg催化剂,用X- 射线衍射,X- 射线光电子能谱和磁测定对催化剂进行表征并和普通浸渍法制得的相同金属含量的催化剂进行比较,表明溶剂化金属原子浸渍法制得催化剂的金属粒度小于普通浸渍法制得的催化剂,而且前者的零价金属含量也高于后者。溶剂化金属原子浸渍法制得的催化剂Co 在表面上,而普通浸渍法制得催化剂Co 在表面和体相的金属含量基本相同。 相似文献
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用溶剂化金属原子浸渍(SMAI)法和普通浸渍(CI)法两种不同的方法制备了组成相同的K-Fe/硅沸石催化剂。TEM,XRD,XPS和磁测定结果表明,SMAI K-Fe/硅沸有催化剂中铁的分散度和还原度都大于CI催化剂,SMAI催化剂中金属颗粒直径小于4nm,具有超顺磁性,而CI催化剂中金属颗粒较大,表现铁磁性。两种方法制备的催化剂反应前后金属的状态发生明显的改变,对CO+H_2反应的催化性质不同。 相似文献
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采用柠檬酸法制备了Ce-Zr-O2固溶体, 并负载了过渡金属和贵金属Pt, 其中, 以Cu作为活性组分, 在CO氧化反应中表现出最高的活性, CO完全转化的温度约为120 ℃, 明显高于负载1%Pt(质量分数)催化剂的活性. 掺杂少量Zr到CeO2(Ce0.8Zr0.2O2)中对Cu基催化剂有非常好的促进作用. 分别采用等体积浸渍法(IW)、 沉淀沉积法(DP)、 水热法(HT)以及柠檬酸法(CA)制备了Cu负载质量分数为20%的Cu/Ce0.8Zr0.2O2催化剂. 结果表明, 由沉淀沉积法制备的Cu/Ce0.8Zr0.2O2催化剂的活性最高, 在100 ℃时, CO可完全转化. TEM结果表明, CuO物种很好地分散在Ce0.8Zr0.2O2上. 吸附实验数据表明, Cu基催化剂上CO与O2之间较弱的竞争吸附是其活性高于Pt催化剂的主要原因. Cu基催化剂上的氧空位对促进O2的吸附具有重要作用, 也是影响CO低温氧化的重要因素之一. 相似文献
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聚合物固载Co-Pd 催化剂的结构与活性 总被引:3,自引:0,他引:3
采用溶剂化金属原子浸渍(SMAI)法制备了几种不同金属含量的Co Pd催化剂,用X射线衍射、X射线光电子能谱和磁测定对催化剂进行表征,并与普通浸渍法(CI)制得的相同金属含量的催化剂进行比较.结果表明SMAI法制备的催化剂金属粒度小于CI法制备的催化剂,且前者零价金属含量高于后者.SMAI法制备的催化剂Co在表面上富集,而CI法制备的催化剂Co在表面和体相的金属含量基本相同.在二丙酮醇加氢及电催化反应中, SMAI法催化剂比相同组成的CI法催化剂具有更高的催化活性. 相似文献
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Effect of pretreatment methods on the performance of Cu-Zr-Ce-O catalyst for CO selective oxidation
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The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu+/Cu^2+ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation. 相似文献
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以硝酸铜、 正硅酸乙酯和硝酸铈为原料, 利用溶胶-凝胶-超临界流体干燥技术制备了不同n(Cu)/n(Si)的用于CO催化氧化的Cu/SiO2系列气凝胶催化剂. 利用TEM、 XRD、 物理吸附、 微型反应器和气相色谱等对试样进行了表征. TEM观察结果显示, 试样中含有介孔的气凝胶结构, 5 nm左右的Cu粒子均匀地分布在SiO2的网络组织中. BET分析结果表明, 试样的比表面积均在140 m2/g以上. XRD分析结果显示, 添加铈前后, 试样的物相发生了从Cu 2+ →Cu+ →Cu的转变, 使试样的催化活性进一步提高. 试样的催化氧化CO活性表明, 组分中铜含量的不同及铜的不同物种直接影响试样的催化氧化CO的活性, 当组分中n(Cu)/n(Si)=2时, Cu/SiO2试样上CO完全氧化的温度降为210 ℃; 于400 ℃低温焙烧, 可使试样中有效活性组分全部转变成纳米晶CuO, 并进一步降低了CO完全转变成CO2的温度; 添加少量铈组分, 使试样催化氧化CO的tstart, t50及t90温度提前20 ℃以上, Cu/SiO2试样催化氧化CO动力学研究结果显示, 试样降低CO氧化温度的实质是降低了CO氧化的反应活化能. 相似文献
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以凹凸棒土(APT)作载体,采用等体积浸渍法制备了Pd-Cu/APT催化剂,以CO氧化为探针反应,在连续流动微反装置上,考察了焙烧温度对催化剂CO常温催化氧化性能的影响。通过N2-物理吸附、XRD、TG、FT-IR和H2-TPR等手段对催化剂的结构和性质进行了表征。结果表明,随焙烧温度升高,Pd-Cu/APT中载体逐步脱水,进而引起催化剂结构和织构变化,其中,Cu物种由Cu(OH)Cl逐渐向CuO转变,同时,高分散的Pd物种与Cu物种间相互作用先增强后减弱。经300℃焙烧的催化剂比表面积大,Cu物种以Cu(OH)Cl形式存在,且具有良好的分散状态,与Pd物种之间产生较强的相互作用,显著提高了其还原性能。在空速6 000 h-1、CO体积分数0.5%、水蒸气体积分数3.3%的反应条件下,常温可将CO完全转化800 min以上。焙烧温度高于或低于300℃均引起CO常温催化氧化性能的下降。 相似文献
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BEHAVIOR OF SUPPORTED NANO-COPPER CATALYST IN CO OXIDATION 总被引:1,自引:0,他引:1
IntroductionNanomaterialisanewkindofmaterialwithparticlesizebetWeenIurnand100urn.Becauseofthesmallparticlesizeandthelargespecificsufficearea,nanomaterialpossessesmanyparticularproperties,suchashighersufficeenergyandhighersurfaceactivity.t.[l]Thehigheracti… 相似文献
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采用非晶态多核配合的方法合成了La1-xCuxMnO3(x=0、0.05、0.1、0.2、0.3、0.4、0.5)系列催化剂, 并用X射线衍射(XRD)、透射电镜(TEM)、比表面测定仪(BET)等手段对催化剂的微观结构进行了表征. 研究了Cu掺杂对钙钛矿结构及其对CO催化氧化发光性能及催化氧化CO、CH4性能的影响规律. 结果表明, 当x≤0.1 时, Cu掺杂仍可形成单相的钙钛矿结构; 当x>0.1时, 过量掺杂的Cu以CuO杂相存在. Cu掺杂可改善La1-xCuxMnO3催化剂对CO和CH4的催化氧化活性. 经700 ℃焙烧3 h制备的La0.9Cu0.1MnO3催化剂具有最高CO催化氧化活性(T100%=170 ℃), 该结果与CO催化氧化发光结果一致.而La0.95Cu0.05MnO3催化剂对CH4的催化氧化活性最高(T95%=705 ℃). 相似文献
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The effects of particle composition on heterogeneous catalysis were studied using dendrimer-encapsulated nanoparticles (DENs) as precursors to supported Pt-Cu catalysts. Bimetallic Pt-Cu DENs with varying Pt/Cu ratios were prepared in an anaerobic aqueous solution and deposited onto a high-purity commercial alumina support. The dendrimer template was then thermally removed to yield supported nanoparticle catalysts, which were studied with toluene hydrogenation and CO oxidation catalysis as well as infrared spectroscopy of adsorbed CO. Incorporating Cu into Pt nanoparticles had opposite effects on the two test reactions. Cu acted as a mild promoter for CO oxidation catalysis, and the promoting effect was independent of the amount of Cu present. Conversely, Cu acted as a strong poison for toluene hydrogenation catalysis, and the normalized rate tracked inversely with Cu content. Infrared spectroscopy of the supported nanoparticles indicated that electronic effects (electron donation from Cu to Pt) were minimal for these materials. Consequently, the catalysis results are interpreted in terms of potential structural differences as a function of Cu incorporation and reaction conditions. 相似文献
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以环氧丙烷为凝胶剂,采用简便低廉的无表面活性剂的溶胶-凝胶法制备了一系列不同Cu/Fe摩尔比的高比表面积介孔Fe-Cu复合氧化物纳米粉末。运用微反应器-色谱体系考察了它们在低温CO氧化反应中的催化性能。采用X射线衍射、N2吸附-脱附、热重-差热分析、程序升温还原、傅里叶变换红外光谱和透射电镜对所制样品进行了表征。结果表明,这些介孔Fe-Cu复合氧化物催化剂具有纳米晶结构、窄的孔径分布和高的比表面积,在低温CO氧化反应中表现出高的活性和稳定性。 CuO的添加影响了Fe2O3的结构和催化性能。当CuO含量为15 mol%时,催化剂具有最高的比表面积和催化活性,在低温CO氧化反应中表现出较高的催化稳定性。 相似文献
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SMAI和CI法制备的Ni—Ag/SiO2催化剂的结构与催化性质研究 总被引:1,自引:0,他引:1
应用溶剂化金属原子浸渍(SMAI)法和普通浸渍(CI)法制备了金属含量相同的SiO2负载Ni-Ag双金属催化剂。XRD和磁测定结果表明SMAI催化剂中Ni和Ag的粒度均小于金属含量相同的CI催化剂,SMAI催化剂中Ni和Ag未形成合金,而CI催化剂中Ni和Ag形成了合金。SMAI和CI催化剂都具有超顺磁性。研究了这些催化剂在甲苯加氢反应的催化性质,结果表明与组成相同的普通浸渍法催化相比,SMAI催 相似文献