共查询到20条相似文献,搜索用时 718 毫秒
1.
在340 ℃,5.0 MPa条件下,研究了Fe-Zn-M/HY(M=Cr、Al)复合催化剂上CO2的加氢性能。考察了催化剂中Fe含量对CO2转化率、烃类产物及异构烷烃选择性的影响, 并用CO2-TPD、H2-TPR研究了Fe-Zn-M对CO2的吸附和对H2的还原性能。结果表明, 随着Fe含量的增加, 复合催化剂的活性增强, 烃类产物的选择性降低, 异构烷烃在烃类中的选择性随Fe含量的增加而降低,CO2-TPD、H2-TPR结果表明,随Fe含量的增加,催化剂对CO2的活化吸附量随之增加, 而Fe含量的增加促进了催化剂的还原。 相似文献
2.
Supported Tc catalysts are active in CO hydrogenation, their activity depending on the nature of the support. The reaction proceeds predominantly toward methane formation. All catalysts studied yielded very little C2 and C3 hydrocarbons. The thermal desorption data indicate that the CO strongly bound to the substrate is responsible for CH4 formation.Institute of Physical Chemistry, Russian Academy of Sciences, 117915 Moscow. Translated from Izvestiya Akademii Nauk, Seriya Khimicheskaya, No. 7, pp. 1507–1511, July, 1992. 相似文献
3.
L. A. Zaloznaya I. S. Tkachenko G. V. Egorova S. N. Tkachenko V. V. Lunin 《Moscow University Chemistry Bulletin》2008,63(3):150-152
Cement-containing catalysts of ozone decomposition were synthesized on the basis of iron oxides obtained by ozonation of iron-containing aqueous solutions. X-ray diffraction analysis and Mössbauer spectroscopy showed that α-Fe2O3 occurs in the catalyst as highly dispersed nanoparticles. The catalysts obtained are efficient in the reaction of ozone decomposition and are as active as the best representatives of cement-containing catalysts of the GTT type. 相似文献
4.
Studies on the structural changes and catalytic behavior of iron-manganese catalysts for CO hydrogenation were conducted using Mossbauer spectroscopy, X-ray diffraction, temperature programmed reduction and kinetic measurements. It was observed that the reduction of the mixed oxide catalyst precursors proceeds via the formation of Fe3-xMnxO4,Mn3-xFexO4 mixed spinel and Fe1-zMn2O mixed oxide to α-iron and MnO. After use for CO hydrogenation, catalysts are oxidized as well as carburized. The Mn3-yFeyO4 mixed spinel and Fe1-2MnzO mixed oxide are the most powerful phases for olefin production. The highest attainable 2–4 low carbon olefin selectivity is 41% with an 86% conversion level. Higher manganese content or lower reduction temperatures may change the carbide formed from χ-Fe5C2 to the more unstable ?′-Fe22C. Carbide formation is greatly dependent on manganese content and activation procedure used. 相似文献
5.
Tingzhen Li Yong Yang Chenghua Zhang Zhichao Tao Haijun Wan Xia An Hongwei Xiang Yongwang Li 《天然气化学杂志》2007,16(3):244-251
A systematic study was undertaken to investigate the effects of the manganese incorpo- ration manner on the textural properties,bulk and surface phase compositions,reduction/carburization behaviors,and surface basicity of an iron-based Fischer-Tropsch synthesis(FTS)catalyst.The cata- lyst samples were characterized by N_2 physisorption,X-ray photoelectron spectroscopy(XPS),H_2(or CO)temperature-programmed reduction(TPR),CO_2 temperature-programmed desorption(TPD),and M(?)ssbauer spectroscopy.The FTS performance of the catalysts was studied in a slurry-phase continuously stirred tank reactor(CSTR).The characterization results indicated that the manganese promoter incor- porated by using the coprecipitation method could improve the dispersion of iron oxide,and decrease the size of the iron oxide crystallite.The manganese incorporated with the impregnation method is enriched on the catalyst's surface.The manganese promoter added with the impregnation method suppresses the reduction and carburization of the catalyst in H_2,CO,and syngas because of the excessive enrichment of manganese on the catalyst surface.The catalyst added manganese using the coprecipitation method has the highest CO conversion(51.9%)and the lowest selectivity for heavy hydrocarbons(C_(12 )). 相似文献
6.
O. N. Stavinskaya V. K. Imshennik 《Russian Journal of Physical Chemistry A, Focus on Chemistry》2006,80(12):1925-1928
Mössbauer spectroscopy was used to study size changes of iron-containing particles deposited on carbon and formed in thermal treatment in hydrogen atmosphere under the conditions of iron-catalyzed hydrogenation of carbon. 相似文献
7.
Shuichi Naito 《Catalysis Surveys from Japan》2000,4(1):3-15
The progress in the field of methane conversion into higher hydrocarbons including aromatics and oxygenated compounds in the recent five years will be reviewed shortly, together with a new type of the methane conversion reaction with carbon monoxide at lower temperatures (600–700 K) by supported group VIII metal catalysts. Benzene was formed selectively among hydrocarbons in the CH4–CO reaction over silica-supported Rh, Ru, Pd and Os catalysts under atmospheric pressure. Both CH4 and CO were required for benzene formation, and only ethane and ethylene were formed besides benzene. The amount of C3–C5 hydrocarbons was negligible, which suggests that a completely different mechanism from the CO–H2 reaction may be operating over these catalysts despite of the similarity in the reaction conditions with the CO–H2 reaction. The mechanism of benzene formation was studied deeply by means of kinetical investigation as well as infrared spectroscopy and isotopic tracer method in connection with that of CO hydrogenation. 相似文献
8.
《Electrochemistry communications》2000,2(2):130-134
Radiation effects of energetic heavy ion irradiation in Fe–Zr amorphous alloys were investigated by the help of Mössbauer spectroscopy, X-ray diffraction and electrolytical hydrogenation. The electrolytical hydrogenation of non-irradiated and irradiated samples was carried out by a unique cathodic potential (−1000 mV versus SHE). The combination of electrolytical hydrogenation and Mössbauer analysis gives a very sensitive method for detecting structural changes of these amorphous alloys. It was found that the structural changes in the amorphous state, which are undetectable without hydrogenation by Mössbauer spectroscopy, modify the localization and the concentration of introduced hydrogen, and are reflected in a significant change of magnetic hyperfine interaction. The results can be associated with structural changes due to the effect of energetic heavy ion irradiation. 相似文献
9.
10.
MOFs衍生炭负载的钴基催化剂的廉价制备及其CO加氢催化性能 《燃料化学学报》2019,47(4):428-437
以对苯二甲酸(H2BDC)为配体、乙酸钴为Co源、水作溶剂,通过共沉淀法合成了金属有机框架材料(Co-BDC MOFs);以其为前驱体分别在乙炔和氩气氛下采用化学气相沉积法制备了核壳结构Co@C催化剂。结合XRD、氮吸附、SEM、TEM、XPS、TGA和Raman光谱等手段对Co@C催化剂的结构和组成进行了表征,考察了该催化剂在费托合成反应中的活性及稳定性。结果表明,炭化气氛对炭层结构的石墨化程度有较大影响,而对金属Co核的物相结构和粒径影响较小;乙炔气氛有助于形成多孔的石墨炭壳,从而促进烃链的生长,Co@C-C2H2催化剂上的C5+烃产物选择性高达82.66%,反应过程中催化剂物相由单相金属Co转变为金属Co与Co2C的混合相,且无失活现象发生,表明Co2C具有较高的费托反应催化活性。 相似文献
11.
以Fe(CO)5为前体采用超声法合成纳米Fe胶体粒子,通过Fe胶体与PdCl2发生金属置换反应制备出活性炭负载Pd-Fe双金属催化剂。研究了表面活性剂聚乙烯吡咯烷酮对制备负载型催化剂的影响。采用XRD、H2程序升温还原(H2-TPR)、TEM、EDX等表征手段对催化剂进行表征,以苯乙炔加氢反应为探针反应考察了Fe含量对于催化剂催化性能的影响。结果表明加氢催化活性较差的金属组分Fe在合适的比例下可以促进Pd基催化剂的加氢催化活性和选择性,然而,过多的Fe也会降低其催化活性。 相似文献
12.
A. Samide I. Bibicu M. S. Rogalski M. Preda 《Journal of Radioanalytical and Nuclear Chemistry》2004,261(3):593-596
The effect of the NO3? anion on the corrosion of carbon steel in a solution of 0.1M NH4Cl (pH 5.5) was studied by galvanostatic polarization and Mössbauer spectrometry. The anion has an inhibiting effect by decreasing the expansion rate of generalized corrosion of carbon steel in a solution of 0.1M NH4Cl. Mössbauer spectroscopy shows that a superficial compound is formed on the electrode surface as a result of corrosion, presenting no magnetic ordering. Its parameters show the initial stage of corrosion. We assume that at this stage the main corrosion product is a mixture of ferrihydrite Fe(III) and FeOOH (α and/or γ). 相似文献
13.
The effect of the addition of a second metals such as Zn and Ni on the calcinaton and reduction of alumina, magnesia and silicasupported iron catalysis with total iron loading of 5wt% is investigated by Mössbauer spectroscopy. It is shown that the reducibility of supported α-Fe2O3 is gradually increased by adding the second metal. The values of the magnetic hyperfine field obtained from Mössbauer spectra for the Zn or Ni-added α-Fe2O3 or Fe catalysts decreased with increasing second metal loading. 相似文献
14.
锰助剂对F-T合成Co/Al2O3催化剂反应性能的影响 总被引:6,自引:0,他引:6
采用程序升温和原位红外技术对锰改性Co/Al2O3催化剂进行了表征,并与CO加氢反应活性和选择性进行关联.结果表明,添加适量锰能够增加反应活性,提高烃选择性,抑制甲烷及低碳烃的生成. XRD和FT IR结果表明锰助剂的添加能够促进活性相的分散,促进桥式CO吸附位数的增加. H2 TPD表明锰的加入可增加低温吸附氢量,但吸附氢量随锰含量的增加而减少.钴基催化剂的费托合成反应性能可以用锰添加导致的CO吸附态物种的变化来解释. 相似文献
15.
Dr. Walter T. Ralston Dr. Gérôme Melaet Tommy Saephan Prof. Gabor A. Somorjai 《Angewandte Chemie (International ed. in English)》2017,56(26):7415-7419
The Fischer–Tropsch process, or the catalytic hydrogenation of carbon monoxide (CO), produces long chain hydrocarbons and offers an alternative to the use of crude oil for chemical feedstocks. The observed size dependence of cobalt (Co) catalysts for the Fischer–Tropsch reaction was studied with colloidally prepared Co nanoparticles and a chemical transient kinetics reactor capable of measurements under non-steady-state conditions. Co nanoparticles of 4.3 nm and 9.5 nm diameters were synthesized and tested under atmospheric pressure conditions and H2/CO=2. Large differences in carbon coverage (ΘC) were observed for the two catalysts: the 4.3 nm Co catalyst has a ΘC less than one while the 9.5 nm Co catalyst supports a ΘC greater than two. The monomer units present on the surface during reaction are identified as single carbon species for both sizes of Co nanoparticles, and the major CO dissociation site is identified as the B5-B geometry. The difference in activity of Co nanoparticles was found to be a result of the structure sensitivity caused by the loss of these specific types of sites at smaller nanoparticle sizes. 相似文献
16.
The activity and stability of aluminum-palladium catalysts in the hydrogenation of aromatic hydrocarbons mixed with thiophene were studied. The catalysts were obtained by impregnation of γ-A2O3 with aqueous solutions of salts of palladium complexes. Preliminary sulfiding followed by oxidative activation of Pd/Al2O3 catalysts were found to favor the formation of such palladium state on the surface at which the hydrogenation of aromatic hydrocarbons in the presence of sulfur-containing impurities proceeds without a noticeable change in the activity with time. IR spectroscopy showed that the palladium metal surface fragments forming CO complexes with a characteristic absorption band at 1998 cm–1 are resistant to poisoning with sulfur-containing compounds in the hydrogenation of aromatic hydrocarbons. 相似文献
17.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(26):7523-7527
The Fischer–Tropsch process, or the catalytic hydrogenation of carbon monoxide (CO), produces long chain hydrocarbons and offers an alternative to the use of crude oil for chemical feedstocks. The observed size dependence of cobalt (Co) catalysts for the Fischer–Tropsch reaction was studied with colloidally prepared Co nanoparticles and a chemical transient kinetics reactor capable of measurements under non‐steady‐state conditions. Co nanoparticles of 4.3 nm and 9.5 nm diameters were synthesized and tested under atmospheric pressure conditions and H2/CO=2. Large differences in carbon coverage (ΘC) were observed for the two catalysts: the 4.3 nm Co catalyst has a ΘC less than one while the 9.5 nm Co catalyst supports a ΘC greater than two. The monomer units present on the surface during reaction are identified as single carbon species for both sizes of Co nanoparticles, and the major CO dissociation site is identified as the B5‐B geometry. The difference in activity of Co nanoparticles was found to be a result of the structure sensitivity caused by the loss of these specific types of sites at smaller nanoparticle sizes. 相似文献
18.
Y. Yamada Y. Minai H. Sato T. Tominaga 《Journal of Radioanalytical and Nuclear Chemistry》1985,96(5):503-511
The UV photolysis of pentacarbonyliron isolated in low temperature nitrogen matrix was studied by the Mössbauer Technique. Besides stable compounds /Fe2/CO/9 and Fe3/CO/12/ unstable species such as Fe/Co/4 and Fe2/CO/8 were produced by UV irradiation. Furthermore, the unstable species were found to react with nitrogen matrix, leading to the formation of Fe/CO/4N2. Mössbauer parameters of the products were obtained. 相似文献
19.
Mössbauer data are presented for FeSbO4 at room temperature (RT) and liquid-nitrogen temperature (LNT). An interpretation of the relaxation phenomena in this compound at LNT is given which differs from previous conclusions (G. M. Bartenev et al. [9]) and shows a correlation with FeSbO4 particle size. The results permit a more accurate evaluation of the phase composition of (Fe, Sb)O catalysts by means of Mössbauer spectroscopy. 相似文献
20.
采用并流共沉淀法在不同焙烧温度下制备K改性Ag-Fe/ZnO-ZrO2催化剂,考察不同焙烧温度对催化剂CO加氢合成低碳混合醇醚反应性能的影响。通过N2物理吸附(N2-adsorption)、X射线衍射(XRD)、氢气程序升温还原(H2-TPR)、一氧化碳程序升温脱附(CO-TPD)等手段对催化剂进行表征。结果表明,250 ℃焙烧的催化剂,由于焙烧温度较低,表面尚未形成足够多的活性位,未能达到最佳的催化性能;300 ℃焙烧的催化剂,其CO转化率最高、醇醚选择性较高,醇醚时空产率达到最大值。随着焙烧温度进一步升高,CO转化率逐渐降低,醇选择性先降低后增大,二甲醚(DME)选择性逐渐增大,醇醚时空产率逐渐降低。催化剂性能主要与其比表面积、还原性能、所含银铁复合物分散度及CO吸脱附性能有关,即比表面积较大、易于被还原、银铁复合物分散度较高以及较多的CO吸脱附活性位,有利于催化剂CO加氢转化。催化剂表面活性位对CO的非解离吸附强度降低,有利于醇醚产物的生成;而对CO的解离吸附强度增强,则不利于烃类产物的生成。 相似文献