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Mo/La-Co-O催化剂上甲烷选择氧化制甲醇反应 总被引:6,自引:0,他引:6
制备了一系列Mo/La-Co-O催化剂,考察了催化剂对甲烷选择氧化制甲醇反应的催化性能,并用BET,XRD,LRS,H2-TPR和XPS等技术研究了催化剂的结构和性质.结果表明,在n(CH4)∶n(O2)∶n(N2)=10∶1∶1,SV=14.4L/(g·h),p=4.2MPa和θ=420℃的反应条件下,7%Mo/La-Co-O催化剂表现出较好的催化性能,甲醇选择性为60%,甲醇收率为6.7%.Mo负载于La-Co-O上以后,Mo-O物种以无定形的状态存在于La-Co-O表面,并与La-Co-O发生相互作用.Mo的负载量影响Mo-O物种的结构及催化剂的性质.催化剂的还原性和表面O-/O2-比影响催化剂上甲烷选择氧化制甲醇反应的性能. 相似文献
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溶胶凝胶包埋吡啶羧酸钴及其对甲醇氧化羰化反应的催化性能 总被引:9,自引:0,他引:9
以正硅酸乙酯为前驱体,采用溶胶-凝胶技术将吡啶羧酸钴包埋进SiO2基体中,于80℃干燥12h后得到钴含量为2.8%(Co/Si摩尔比)的干凝胶催化剂.采用FT-IR和TG-DTA方法对包埋催化剂进行了表征,考察了成胶过程中的pH和水与正硅酸乙酯的摩尔比(R)对包埋催化剂的结构及其对甲醇氧化羰化制碳酸二甲酯反应催化性能的影响.结果表明,干凝胶催化剂有较高的比表面积(320~458m2/g).在酸性条件下,增大pH或减小R值可缩短成胶时间.最佳的包埋条件是pH=4,R=6,在此条件下制备的凝胶包埋催化剂的活性最高,反应3h,甲醇转化率为5.73%,略低于均相催化剂上的甲醇转化率.但凝胶包埋催化剂分离简便,且重复使用6次后活性保持不变. 相似文献
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Cr2O3-Co3O4/SiO2对十八醇氧化生成十八酸反应的催化性能 总被引:2,自引:0,他引:2
制备了一系列不同Cr/Co比例的Cr2O3-Co3O4/SiO2催化剂,并用XRD,FT-IR和BET等手段对催化剂进行了表征;考察了催化剂对十八醇氧化生成十八酸反应的催化性能,及反应条件(反应温度和反应时间)对催化性能的影响,确定了最佳反应条件.结果表明,金属硝酸盐在773K焙烧后转变成相应的氧化物并负载于二氧化硅上.Cr2O3-Co3O4/SiO2催化剂对十八醇氧化反应有很高的催化活性,十八酸选择性最高可达99.93%,收率可达52.44%.Cr2O3-Co3O4/SiO2催化剂的活性明显高于单一的Cr2O3/SiO2或Co3O4/SiO2催化剂 相似文献
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常温常压下光促进烯烃与一氧化碳的羰基化反应 总被引:1,自引:0,他引:1
报道了烯烃(环己烯和1-辛烯)与一氧化碳通过光促进实现常温常压非贵金属(钴配合物)催化的羰基化反应.研究发现,以Co(OAc)2为催化剂时,不需要加入光敏剂丙酮就能发生反应;CoSalen,吡啶-2-羧酸钴和大环配合物[Co(14)4,11-diene-N4]I2是较好的催化剂,其催化活性比Co(OAc)2高.其中,吡啶-2-羧酸钴与Co(OAc)2相同,反应中不需要光敏剂存在,其选择性很高.通过氘代丙酮和氘代甲醇同位素实验,进一步证实了反应中双键异构的存在和副产物的分析结果. 相似文献
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用不同前驱体制备的Co/SiO2催化剂的结构及其CO2/CH4重整反应性能 总被引:1,自引:1,他引:0
分别采用硝酸钴、醋酸钴、硫酸钴和氯化钴为前驱体制备了Co/SiO2催化剂,用XRD,TPR,SEM和H2-TPD等实验技术考察了钴盐前驱体对催化剂结构和二氧化碳重整甲烷反应性能的影响,重点考察了硝酸钴和醋酸钴的作用.结果表明,由醋酸钴制备的Co/SiO2催化剂有最佳的催化活性和稳定性,它在钴物种的存在状态、金属-载体相互作用、钴金属晶粒度及抗烧结、抗积炭能力等方面,均与由硝酸钴制备的Co/SiO2催化剂存在显著的差别.Co/SiO2催化剂的反应活性和稳定性分别与其金属分散度和抗烧结、抗积炭能力密切相关. 相似文献
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Co/γ-Al_2O_3催化剂上肉桂醛的选择加氢──反应性能的考察 总被引:2,自引:0,他引:2
研究了γ-Al2O3负载的Co/γ-Al2O3催化剂上肉桂醛的选择加氢反应.反应结果表明,以CoCl2作为前驱物的Co/γ-Al2O3催化剂的选择性要高于以Co(NO3)2作为前驱物的Co/γ-Al2O3催化剂,而活性则正好相反.当钴的负载量小于9%时,随着钴负载量的增加,催化剂的活性和选择性随之增加,当钴的负载量大于9%时,随着钴负载量的增加,Co/γ-Al2O3催化剂的活性略有增加,而生成肉桂醇的选择性变化也很小,认为9%的钴负载量是催化剂反应活性和选择性的一个阈值.在所选定的范围内,反应温度和压力对肉桂醛加氢的选择性几乎没有影响. 相似文献
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采用简捷高效的方法在交联聚苯乙烯(CPS)微球表面同步合成与固载了N-羟基邻苯二甲酰亚胺(NHPI),制备了非均相催化剂CPS-NHPI微球,我们将其用于分子氧对二苯甲醇的氧化过程,探索研究了其催化性能与催化氧化机理,并考察了主要因素对其催化性能的影响.研究结果表明,将固体催化剂微球CPS-NHPI与过渡金属盐组合形成复合催化剂,可有效地催化分子氧对二苯甲醇的氧化过程.在几种过渡金属盐中,助催化效果的顺序是VO(acac)2Co(OAc)2Co Cl2Mn(OAc)2.显然,乙酰丙酮氧钒盐的助催化效果最好.共催化体系CPS-NHPI+VO(acac)2可在温和条件(75℃、常压的氧气)下高效地将二苯甲醇催化氧化转变为二苯甲酮(二苯甲醇转化率为35.8%,且二苯甲酮是唯一产物),显示出良好的催化活性与优良的催化选择性,催化氧化反应遵循自由基链式反应的机理.体积比为7∶3的乙腈与乙酸乙酯的混合液为适宜的反应溶剂;VO(acac)2与固载NHPI的摩尔比为1∶15时,助催化剂的投加量较为适宜.固体催化剂CPS-NHPI还具有良好的再循环使用性能. 相似文献
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新型钴基介孔分子筛催化剂F-T合成性能和烃分布研究 总被引:6,自引:0,他引:6
采用介孔分子筛MSU-1,SBA-12和HMS为载体,制得含钴质量分数为15%的催化剂。在原料气V(H2)/V(CO)=2.0,T=473-513K,p=2.0MPa,GHSV=500H^-1的F-T合成条件下,反应活性依Co/HMS,Co/SBA-12,Co/MSU-1顺序降低,高碳烃(C19^ )选择性以Co/HMS最低;Co/MSU-1和Co/SBA-12催化剂介孔结构在反应中相对稳定,Co/HMS介孔结构在反应后完全塌陷。 相似文献
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利用手持技术改进测定乙醇分子结构实验 总被引:1,自引:0,他引:1
利用压强传感器代替排水集气法,改进测定乙醇分子结构实验的仪器装置,并探索最佳反应条件。另外,设计两个空白实验,结合压强变化曲线对实验误差进行相关讨论。 相似文献
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Mustafa R. Ibrahim Zacharia A. Fataftah Paul von Ragu Schleyer Peter D. Stout 《Journal of computational chemistry》1987,8(8):1131-1138
Sets of hydrogen molecule equivalents have been developed which permit the calculation of hydrogenation of different types of carbon-carbon bonds from ab initio total energies (3-21G and 6-31G* basis sets, and, to a more limited extent, for MP2/6-31G* data) of reactants and products. The calculated enthalpies of hydrogenation are in good agreement with experiment for unstrained molecules, with average errors on the order of 2 kcal/mol. The 6-31G* equivalents allow the enthalpies for strained molecules to be calculated accurately, but the 3-21G equivalents do not. The equivalents for both basis sets have been tested by calculating the enthalpies of hydrogenation of carbon-carbon bonds in nitrogen- and oxygen-containing organic molecules, free radicals, and classical carbocations. The results are in good agreement with experiment in most cases. 相似文献
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由于石化行业的生产需要,其材质的使用具有多样性和广泛性,经常会出现顾客委托的测试样品的一个或几个元素跨越光谱仪现有测试程序测量范围的情况。本法通过对光谱仪测试原理的认识,根据光谱仪的测试能力及标样的采集,实现了一个或几个元素测量范围的扩展,并对其测量的影响因素进行了研究。 相似文献
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V. I. Bol'shakova L. I. Demenkova É. N. Shmidt V. A. Pentegova 《Chemistry of Natural Compounds》1989,24(6):691-694
The compositions of the neutral diterpenoids of the oleoresins of five species of conifers growing in the Transcarpathia have been studied. It has been found that the oleoresins ofAbies alba M.,Larix decidua M., andPicea excelsa L. contain more than 50% of neutral diterpenoids. The group and qualitative compositions of the oxygen-containing diterpenoids have been determined. In the oleoresins ofAbies alba,Picea excelsa, andPicea abies tertiary alcohols — cis-abienol and isocembrol — predominate, while inLarix decidua the main component is the hydroxy ester larixyl acetate. Primary alcohols related to the resin acids have been found in all the oleoresins investigated. Features of the distribution of diterpenoids according to the species of conifers have been revealed. The results obtained are necessary for the chemotaxonomy of conifers of the family Pinceae.Novosibirsk Institute of Organic Chemistry, Siberian Branch, Academy of Sciences of the USSR. Translated from Khimiya Prirodynkh Soedinenii, No. 6, pp. 812–816, November–December, 1988. 相似文献
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V. I. Bol'shakova L. I. Demenkova É. N. Shmidt V. A. Pentegova 《Chemistry of Natural Compounds》1988,24(6):691-694
The compositions of the neutral diterpenoids of the oleoresins of five species of conifers growing in the Transcarpathia have been studied. It has been found that the oleoresins ofAbies alba M.,Larix decidua M., andPicea excelsa L. contain more than 50% of neutral diterpenoids. The group and qualitative compositions of the oxygen-containing diterpenoids have been determined. In the oleoresins ofAbies alba,Picea excelsa, andPicea abies tertiary alcohols — cis-abienol and isocembrol — predominate, while inLarix decidua the main component is the hydroxy ester larixyl acetate. Primary alcohols related to the resin acids have been found in all the oleoresins investigated. Features of the distribution of diterpenoids according to the species of conifers have been revealed. The results obtained are necessary for the chemotaxonomy of conifers of the family Pinceae. 相似文献
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Influence of viscosity of medium on processes of oxygen quenching of excited states of mesoporphyrin
E. I. Kapinus V. A. Ganzha B. M. Dzhagarov E. I. Sagun V. B. Pavlenko 《Theoretical and Experimental Chemistry》1989,25(2):146-151
The oxygen quenching rate constants for singlet and triplet excited states of the dimethyl ester of mesoporphyrin IX increase with decreasing viscosity of the medium and reach a maximum at a viscosity of approximately 0.4 mPa·sec, after which the rate constants begin to decrease. The drop in rate constant with increasing fluidity of the medium may be related to a nonequilibrium character of the elementary act in the interaction of the reactants in the solvent cage. In viscous media such as isopropyl alcohol, isobutyl alcohol, and isoamyl alcohol, the reaction radius is greater than the sum of the radii of the reacting particles. The long-range character of these processes is due to the relatively weak dependence of the quenching probability on distance.Translated from Teoreticheskaya i Éksperimental'naya Khimiya, Vol. 25, No. 2, pp. 161–167, March–April, 1989. 相似文献
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The spectral-polarization characteristics of absorption and phosphorescence of molecules of the initial form of nitro-substituted
indolinospirobenzothiopyran were studied in oriented polyethylene films and in solutions with different polarity. An oscillator
model of the electron transitions responsible for the formation of absorption and luminescence spectra was suggested. It was
established that the principal differences in the spectral and photophysical properties of the compound studied and its oxygen-containing
analog are associated with the fact that the electronegativity of the S atom is lower than that of the O atom.
Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 6, pp. 1143–1146, June, 1997. 相似文献