首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到19条相似文献,搜索用时 156 毫秒
1.
本文制备了用于费托合成反应的钴改性Fe3O4-MnO2双功能催化剂,并探究了钴负载量对Fe-Co协同效应的影响以及Fe1CoxMn1催化剂的费托合成反应性能. 实验发现,在Fe3O4-Mn催化剂中加入Co可促进铁氧化物的还原、增加反应过程中铁位点的活性. 此外,Co的加入可增强Fe-Co金属间的电子转移,加强两者的协同作用,提高催化性能. Co负载较高的Fe1CoxMn1催化剂可进一步促进加氢反应能力,使产品分布向短链烃方向转移. 在280 °C、2.0 MPa和3000 h-1的最佳工况条件下,Fe1Co1Mn1催化剂的液体燃料收率最高.  相似文献   

2.
用浸渍法制备γ-Al2O3负载的Ni-Mn双金属催化剂.在500~700 oC按照17:17:2的CO2/CH4/N2比例,以36 mL/min的载气流速进行甲烷二氧化碳重整反应, 利用甲烷二氧化碳的转化率、生成的合成气H2/CO比例以及长期稳定性等指标评价了催化剂的催化性能. 实验表明, 添加Mn提高催化性能并使双金属催化剂的稳定性更高, 比单金属催化剂更好地抑制焦炭生成,Mn最合适的添加量0.5wt% .通过BET、CO2-TPD、TGA、XRD、SEM、EDX和FTIR各种技术对催化剂进行了表征.  相似文献   

3.
用水热法得到的钛酸纳米纤维前体,通过不同后处理方法合成了多种纳米结构的TiO2.采用N2等温吸附和BET比表面、X射线衍射、透射电镜和能量分散X射线分析表征了TiO2及负载Ru催化剂的微结构,包括比表面、晶相结构和形貌以及Ru纳米颗粒尺寸分布等.对负载Ru催化剂在富氢条件下CO选择甲烷化反应活性测试表明:金红石相TiO2和TiO2-B为载体负载的Ru催化剂比锐钛矿相TiO2负载的Ru催化剂表现出更高的反应性能.其活性区别说明了不同晶相结构和形貌TiO2载体与Ru纳米颗粒的相互作用存在差异.  相似文献   

4.
采用水热法以HF作为结构调控剂合成了主要暴露(001)面的锐钛矿TiO2纳米片,通过光沉积方法分别合成了负载Ru和RuO2物种的光催化剂。利用X射线衍射、透射电镜和氢气程序升温还原等分析表征了催化剂的结构性质。通过光解水产氧反应来研究催化剂的催化性能,详细考察了Ru含量、负载方式以及氧化和还原处理等因素的影响,光解水产氧速率的差异证明了Ru物种在不同晶面的电荷-空穴分离效应。与负载单一助催化剂的Ru/TiO2和RuO2/TiO2样品相比,活性最优的0.5%Ru-1.0%RuO2/TiO2样品由于负载了双助催化剂,其催化活性得到更大的提高,证实了在锐钛矿TiO2上的晶面电荷-空穴分离效应.  相似文献   

5.
利用ReaxFF分子动力学模拟方法对正庚烷在高温条件下的热解行为进行了研究.细致分析了温度对正庚烷高温裂解过程以及产物分布的影响.结果显示温度对正庚烷的热解过程的影响是分阶段的.高温能加速正庚烷的分解,但是当温度达到一定阶段之后这种影响逐渐变小.正庚烷的热解可以分为三个阶段.主要产物C2H4、C3和C4的质量百分数随转化率的变化规律与实验值符合很好.利用一阶动力学模型得到的正庚烷热解的表观活化能和指前因子分别为53.96 kcal/mol和55.34×1013 s-1,与实验值相符.  相似文献   

6.
本文对纤维素和甲醇在不同金属氧化物改性的ZSM5催化剂作用下共催化快速热解实现一步制备可再生对二甲苯的过程进行了研究. 结果表明,镧改性的ZSM5催化剂是生产生物基对二甲苯的有效催化剂. 对二甲苯的选择性和产率主要由催化剂酸性、反应温度和甲醇含量决定. 在20%La2O3-ZSM5(80)催化剂作用下,纤维素与33wt%甲醇共催化快速热解获得对二甲苯的最高收率和对二甲苯/二甲苯的最高比率分别为14.5 C-mol%和86.8%. 本文详细研究了催化热解过程中催化剂的失活,基于产物的分析和催化剂的表征提出了由纤维素制备对二甲苯的可能反应途径.  相似文献   

7.
采用氨蒸发法、尿素水解法、离子交换法及浸渍法制备HMOR负载的Cu催化剂, 考察其催化二甲醚(DME)羰基化合成乙酸甲酯(MA)性能. 结果表明离子交换法制得Cu/HMOR催化剂在Cu的金属中心和酸性分子筛载体的共同作用下具有较好催化反应活性. 在210 oC、1.5 MPa、空速4883 h-1,DME转化率为95.3%,MA选择性为94.9%. 对催化剂进行N2物理吸附、X射线衍射、NH3程序升温脱附和CO程序升温脱附等表征发现,离子交换法制得Cu/HMOR催化剂具有较高比表面、大量弱酸及一定中强酸、适中的CO吸附强度,提高了CO插入DME羰基化反应活性.  相似文献   

8.
以Na2CO3为沉淀剂,在pH=9时,采用并流沉淀法制备了Ni/CuO-ZrO2-CeO2-Al2O3催化剂,催化剂中活性组分Ni的负载量(质量分数)为10%.采用TPO、SEM和XPS等方法研究了载体焙烧温度对催化剂积炭行为的影响.结果表明,载体焙烧温度为800 oC制备的Ni/CuO-ZrO2-CeO2-Al2O3催化剂不存在高温烧炭峰,可以避免由于积炭而降低反应的活性.反应40 h后,催化剂表面出现表面碳酸盐和非活性丝状积炭,这些物种可能会导致催化剂活性降低.  相似文献   

9.
以传统的浸渍法,在不同焙烧温度下制备了用于CO氧化反应的Co3O4/SiO2催化剂.通过激光拉曼光谱(Raman)、X射线光电子能谱(XPS)、X射线衍射(XRD)、程序升温还原(TPR)和X射线吸收精细结构谱(XAFS)表征了该系列催化剂的结构.在所有的催化剂中,XRD和Raman光谱都只检测到了Co3O4晶相的存在.与Co3O4体相相比,XPS结果表明在200 oC焙烧的(Co3O4(200)/SiO2)催化剂中Co3O4表面上存在着过量的Co2+.与XPS的结果一致,TPR结果表明Co3O4(200)/SiO2催化剂中Co3O4表面上存在氧缺陷, 并且XAFS结果也表明Co3O4(200)/SiO2催化剂中Co3O4具有更多的Co2+.提高焙烧温度使得过量的Co2+进一步氧化为Co3+,同时降低了表面氧缺陷浓度,从而得到计量比的Co3O44/SiO2催化剂.在所有的负载催化剂中Co3O4(200)/SiO2催化剂表现出了最好的CO氧化催化性能,表明过量Co2+和表面氧缺陷的存在能够促进Co3O4催化CO氧化反应的活性.  相似文献   

10.
 对块状TiO2气凝胶的溶胶-凝胶过程及结构进行了实验研究,结果发现:增加催化剂的量,凝胶化时间缩短,湿凝胶的透明度降低,强度提高;增加前驱体的量,凝胶化时间缩短,湿凝胶的透明度变化不大,强度提高;增加水量,凝胶化时间先缩短后增加,湿凝胶透明度先减小后增加,强度先增加后减小。利用扫描电镜对超临界干燥法制备的不同催化剂量和密度的块状TiO2气凝胶的结构进行了表征,并对结构与溶胶-凝胶过程之间的联系进行了分析。结果表明:增加催化剂量,由于缩聚反应进行的程度提高,气凝胶粒子粒径较小且总的孔径较大。减小前驱体量,气凝胶粒子粒径增大且结构逐渐疏松。  相似文献   

11.
选用四种不同的分子筛(SAPO-34, ZSM-5, Y, MCM-41)与CuCoMn(高醇合成组元)构成双功能催化剂,利用N2吸脱附、H2-TPR、XRD、NH3-TPD等表征了催化剂的结构性质. 研究了催化剂在生物质基合成气一段法制取液态烃燃料的应用. 相比于CuCoMn催化剂,加入分子筛的双功能催化剂均不同程度地提高了液体烃燃料的选择性及收率,且收率按顺序递减呈CCM-ZSM-5>CCM-SAPO-34>CCM-Y>CCM-MCM-41. 同时,共沉淀法制备的CuCoMn-ZSM-5 (20wt%, Si/Al=100) 具有最佳的CO转化率(76%)及液体产物收率(30%). 相比于CuCoMn氧化物,双功能催化剂的比表面及孔容均得到提高. CCM-ZSM-5具有适中的微孔尺寸和中等强度的酸性,增加CCM-ZSM-5中ZSM-5含量或降低ZSM-5中的Si/Al比,均有利于提高酸性位的数量,主要是较弱的酸性位. 而共沉淀法制备的CCM-ZSM-5具有更好的金属分散性及还原性能.  相似文献   

12.
Pt-porous glass catalysts have been studied by small-angle X-ray scattering. The catalysts have been prepared by impregnating two micro- or mesoporous glasses with 0.1 wt% of Pt. Two different pore systems of the catalyst supports have been generated and investigated: on the one hand, the mesoporous structure is formed by finely dispersed colloidal silica inside a macroporous glass. On the other hand, micropores are given by the porous glass itself. The pure supports and the supported catalysts have been investigated via chord length analysis for a selected range order, based on the analysis of the scattering intensity for relatively large scattering vectors (up to the upper limit of SAS). The obtained specific structure parameters of both supported catalysts like dispersion, specific metal surface areas, basic arrangement, size distribution and volume fraction of the metal particles basically differ with both pore systems.  相似文献   

13.
Catalysts composed of nickel and promoted with different metal oxides proved to be suitable for H/D isotropic exchange between hydrogen and water vapour. They loss their activity due to water condensation on their surfaces. Several nickel/chromium oxide/zirconium oxide catalysts of different composition were prepared by the coprecipitation technique. The liquid phase activity of these catalysts were followed using the hydrogen peroxide decomposition on their surfaces at different temperatures. The surface characteristics of the examined catalysts were followed by applying the BET method. The results were discussed and lead to the required catalyst composition which resists the water condensation on its surface during operation and has relatively high activity in the vapour phase H/D isotopic exchange reaction between hydrogen and water.  相似文献   

14.
固体核磁共振技术是研究固体催化剂酸碱性的有效工具.本文主要介绍了本课题组利用固体核磁共振技术进行固体酸催化剂酸碱性研究的进展,包括吸附水分子对金属氧化物表面酸性质影响的研究,以及结合酸碱探针分子共吸附表征方法对金属氧化物表面酸碱性的研究,对固体核磁共振技术定性和定量分析固体催化剂的酸碱性提出了一些新的见解.  相似文献   

15.
In situ Mössbauer spectra recorded at 570 and 80 K are reported for Cab-O-Sil supported iron-ruthenium Fischer-Tropsch catalysts with different Ru/Fe ratios. The effect of ruthenium has been revealed in the hinderance of carbide formation and in the improved stability of the catalyst. Spectra obtained in hydrogen and in increased CO/H2 ratio atmospheres are also discussed.  相似文献   

16.
N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NEC/12H-NEC) is one of the most attractive LOHCs, and it is of great significance to develop catalysts with high activity and reduce the hydrogen storage temperature. Layered double hydroxides-carbon nanotubes composites (LDH-CNT) were synthesized by a simple in-situ assembly method. Due to the introduction of CNT, a strong interaction occurred between LDH and CNT, which effectively improved the electron transfer ability of LDH-CNT. Ru/LDH-CNT catalysts were prepared via ultrasound-assisted reduction method without adding reducing agents and stabilizers. Under the cavitation effect of ultrasound, the hydroxyl groups on the surface of LDH were excited to generate hydrogen radicals (•H) with high reducibility, which successfully reduced Ru3+ to Ru NPs. Ru/LDH-3.9CNT-(300-1) catalyst was of 1.63 nm average Ru particle size with CNT amount of 3.9 wt% and the ultrasonic power of 300 W at 1 h, and its electron transfer resistance was less than that of Ru/LDH-(300-1). The synergy of ultrafine Ru NPs and fast electron transfer made it exhibit exceptional catalytic performance in NEC hydrogenation. Even if the reaction temperature was lowered to 80 °C, its hydrogenation performance was better than that of commercial Ru/Al2O3 catalyst at 120 °C. The ultrasound-assisted method is efficient, green and environmentally friendly, and the operation process is simple and economical. It is expected to be used in practical industrial production, which provides a reference for the preparation of high-activity and low-temperature hydrogen storage catalysts.  相似文献   

17.
The electronic state of ruthenium in the supported Ru/EOx (EOx = MgO, Al2O3 or SiO2) catalysts prepared by with the use of Ru(OH)Cl3 or Ru(acac)3 (acac = acetylacetonate) and reduced with H2 at 723 K is characterized by X-ray photoelectron spectroscopy (XPS) in the Ru 3d, Cl 2p and O 1s regions. The influence of the final state effects (the differential charging and variation of the relaxation energy) on the binding energy (BE) of Ru 3d5/2 core level measured for supported Ru nanoparticles is estimated by comparison of the Fermi levels and the modified Auger parameters determined for the Ru/EOx samples with the corresponding characteristics of the bulk Ru metal. It is found that the negative shift of the Ru 3d5/2 peak which is observed in the spectrum of ruthenium deposited onto MgO (BE = 279.5-279.7 eV) with respect to that of Ru black (BE = 280.2 eV) or ruthenium supported on γ-Al2O3 and SiO2 (BE = 280.4 eV) is caused not by the transfer of electron density from basic sites of MgO, as considered earlier, but by the differential charging of the supported Ru particles compared with the support surface. Correction for the differential charging value reveals that the initial state energies of ruthenium in the Ru/EOx systems are almost identical (BE = 280.5 ± 0.1 eV) irrespectively of acid-base properties of the support, the mean size of supported Ru crystallites (within the range of 2-10 nm) and the surface Cl content. The results obtained suggest that the difference in ammonia synthesis activity between the Ru catalysts supported on MgO and on the acidic supports is accounted for by not different electronic state of ruthenium on the surface of these oxides but by some other reasons.  相似文献   

18.
Over the past two decades, advanced materials with hollow interiors have received significant attention in materials research owing to their great application potential across a vast number of technological fields. Though with great difficulty, multi-shelled hollow metal–organic frameworks (MSHMs) have also been successfully synthesized in recent years. Herein, a rational shell-by-shell soft-templating protocol has been devised to fabricate highly uniform multi-shelled hollow cobalt-imidazole-based MOF (ZIF-67). For the first time, it has become possible to endow mesoporosity to this new type of functional material (i.e., mesoporous MOFs). When used as carrier materials in catalytic reactions, in principle, these mesoporous MSHMs with high surface area not only improve the dispersity of metal nanoparticles (NPs), but also efficiently facilitate the mass diffusion of the reactions, resulting in enhanced catalyst activity. Moreover, the obtained MSHMs/M nanocomposites serve as base-metal bifunctional catalysts for one-pot oxidation-Knoevenagel condensation cascade reaction, in which the MSHMs itself serves as a pristine active catalyst in addition to its role of catalyst support. The results demonstrate that excellent multifunctional catalysts can be achieved via preparing intrinsically microporous bulk MOFs into extrinsically mesoporous MSHMs which possess many structural merits that conventional bulk MOFs do not have.  相似文献   

19.
Yu F  Ji J  Xu Z  Liu H 《Ultrasonics》2006,44(Z1):e389-e392
Ruthenium-based materials are the second-generation catalysts for ammonia synthesis. Ruthenium is less inhibited by ammonia, less sensitive to poisons, and more active than the traditional iron-based catalyst. The relatively high cost of Ru compared to that of iron requires a high dispersion of the metal on a suitable support. Carbon-supported Ru catalysts with promoters have been reported to be active for ammonia synthesis. The ultrasonic technique has been proven to be beneficial to the preparation of supported catalysts. In this paper, the effects of ultrasonic treatment on the surface texture, oxygen groups of activated carbon (AC) as well as ruthenium dispersion were investigated by the employments of N(2) physisorption, TPD-MS and CO chemisorption respectively. It have been shown that ash content in AC can be effectively eliminated by ultrasonic pretreatment, at the same time, the BET surface area and total pore volume are reduced, and the amount of the decomposable surface oxygen groups are decreased. Furthermore the ash content decrease and the mesopore surface area increase with the ultrasonic power increasing. The activities of a series of barium-potassium-promoted Ru/AC catalysts for ammonia synthesis were tested at 10,000 h(-1), 10.0 MPa and 400 degrees C. The results show that the activities of Ru/AC catalysts which were prepared by ultrasonic treatment are greatly increased, and the optimum pretreatment power is 100 W. The ash content of this carbon support is decreased from 1.39% to 1.15%. As a result, the catalytic activity is improved from 65.3 to 83.8 mmol g(-1) h(-1).  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号