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1.
何代平  丁云杰 《催化学报》2005,26(11):961-964
 采用H2和CO吸附、FT-IR和TPR等表征手段对不同Pd含量的Pd-K/MnOx-ZrO2催化剂进行了研究,并考察了其对CO加氢制甲醇和异丁醇反应的催化性能. 结果表明, Pd的加入促进了锰的还原和氧空位的生成,有利于异丁醇的生成; Pd的加入改变了催化剂表面的吸附行为. Pd-K/MnOx-ZrO2催化剂表面有较高的H2和CO吸附量,有利于甲醇与异丁醇合成速率的提高. 当Pd的添加量超过1.5%时, Pd的分散度降低,粒径变大,致使甲醇与异丁醇的合成速率降低.  相似文献   

2.
碱金属助剂对MnOx/ZrO2催化合成   总被引:6,自引:0,他引:6  
 研究了MnOx/ZrO2催化剂中添加的碱金属助剂对以合成气合成甲醇及异丁醇反应的影响,并采用BET,XRD和NH3-TPD等表征技术,考察了碱金属助剂的添加对催化剂结构和表面性质的影响.结果表明,碱金属助剂对MnOx/ZrO2催化剂的催化性能有明显影响.在实验条件下,添加1.0%K(K2CO3作为前驱物)的催化剂,其催化性能最好,醇的选择性高达74.8%,异丁醇选择性达16.3%.添加碱金属助剂也使MnOx/ZrO2催化剂的表面性质发生了很大变化,从而影响催化剂的催化性能.  相似文献   

3.
 采用固定床积分反应器,详细考察了F-T合成反应用Fe-Mn催化剂运行900和1800h后的中后期反应性能.结果表明,该催化剂仍维持着较高的催化活性及稳定性;与初期反应性能相比,运行900h后CH4选择性有明显升高的趋势,运行1800h后CH4选择性进一步升高.运行2200h后,通过降低原料气的H2/CO比和提高反应压力,可明显改善烃产物的选择性.在n(H2)/n(CO)=0.62,GHSV=2300h-1,p=3.02MPa和θ=283℃的条件下,CO转化率可达75.6%,总有效烃(C=2~4+C+5)的选择性可达89.0%,CH4选择性为5.7%.这表明该催化剂具有良好的可操作性,且特别适合于由煤制合成气制液体燃料和C2~4低碳烯烃,在浆态床反应器中有潜在的应用前景.  相似文献   

4.
 在固定床积分反应器中,对Fe-Mn催化剂上F-T合成反应的初期反应性能进行了一系列条件实验,考察了在不同温度、压力、原料气H2/CO比和空速下催化剂的催化性能.结果表明,该催化剂运行200h后,仍显示出较高的催化活性和稳定性,对低碳烯烃和C5+烃具有较高的选择性,且C5+烃的时空收率较高.在n(H2)/n(CO)=1,GHSV=6000h-1,p=2.02MPa和θ=300℃的条件下,CO转化率可达74.1%,总有效烃(C=2~4+C5+)的选择性可达88.6%,甲烷选择性为6.7%,C5+烃的时空收率为0.54g/(ml·h).  相似文献   

5.
 采用CO加氢反应、程序升温还原(TPR)、CO吸附和CO脱附等技术,研究了Fe助剂对Rh-Mn-Li/SiO2催化剂上CO加氢合成二碳含氧化物反应的影响.结果表明,Mn,Li和Fe的加入明显提高了Rh催化剂的活性及选择性,特别是在1%Rh-1%Mn-0.075%Li/SiO2催化剂中加入0.05%Fe后,C2+含氧化物的时空收率由331.6g/(kg·h)提高到457.5g/(kg·h).但当Fe的加入量继续增加时,催化剂的活性及选择性下降,甲醇的选择性上升.TPR实验表明,当加入少量Fe(0.05%~0.5%)时,TPR的峰面积随Fe加入量的增大而增大,Fe的加入使Rh的还原温度向高温移动,Mn的还原温度向低温移动,Fe的还原峰与Rh和Mn的还原峰相重叠,由此推断这些Fe与Rh是处于紧密接触状态的.当Fe含量增加到1%时,样品在522K出现一个新的谱峰,该峰可归属为与Rh非紧密接触的Fe的还原峰.CO的吸附实验表明,当Fe的加入量超过一定值后,CO吸附量下降.CO的脱附实验表明,在Rh基催化剂中加入少量Fe后,强吸附的CO增多,但当Fe的加入量超过一定值时,强吸附的CO量下降.  相似文献   

6.
 研究了不同助剂促进的负载型Pd-Se/H4SiW12O40/SiO2催化剂对乙烯直接氧化制乙酸反应的影响.采用固定床微反装置评价了催化剂的性能,并采用C2H4和O2吸附量测定、吸附C2H4的TPD-MS和TPSR-MS等技术对催化剂进行了表征.结果表明,以SiO2为载体,以硅钨酸为助剂,Pd-Se-Na-Ru组成的催化剂体系其催化性能比文献报道的结果明显提高.在原料气配比n(C2H4)∶n(N2)∶n(O2)∶n(H2O)=55∶14∶9∶22,反应物空速GHSV=3844h-1,反应压力p=1.4MPa,反应温度θ=155℃条件下,乙烯的转化率和乙酸的选择性分别为8.0%和87.4%,乙酸的单程时空产率达372.0g/(L·h).吸附量测定表明,吸附在催化剂表面上的C2H4/O2比值高对于提高乙酸的选择性是有利的.  相似文献   

7.
稀土Sm对于Cu/Zr基合成醇催化剂的改性作用   总被引:6,自引:0,他引:6  
 采用BET,XRD,TPR,H2-TPD和NH3-TPD等表征手段,考察了稀土助剂Sm2O3的添加方式对Cu/Mn/Zr/Ni催化剂结构的影响,并与催化剂催化CO加氢合成醇反应的活性及选择性相关联.结果表明,加入稀土助剂后,催化剂的表面酸性明显增强,催化性能发生了很大变化,副产物烃和CO2的含量明显降低;反应过程中有大量二甲醚生成.此外,稀土助剂Sm2O3对催化剂有一定的电子改性作用,改变了催化剂表面的吸附行为.  相似文献   

8.
Fe/MnO-ZnZSM-5双功能催化剂上合成气直接转化为芳烃的反应   总被引:4,自引:0,他引:4  
 探讨了Fe/MnO-ZnZSM-5(n(SiO2)/n(Al2O3)=50)双功能催化剂上合成气直接转化为芳烃的反应,考察了反应温度和Zn载量对CO转化率及芳烃选择性的影响.结果表明,Fe/MnO-ZnZSM-5具有良好的合成气芳构化性能,在V(CO)∶V(H2)∶V(Ar)=3∶6∶1,SV=1600h-1,p=1.1MPa,T=543K的条件下,CO转化率可达到98.1%,芳烃产物选择性可高达53.1%.催化剂经60h运转后,CO转化率仅降低0.5%,显示了良好的稳定性和应用前景.  相似文献   

9.
在Zr-Mn-K催化剂中添加稀土氧化物助剂Pr6O_(11)、Sm_2O_3可以显著提高合成气合成甲醇、异丁醇的活性,特别是异丁醇的时空产率在400℃、10MPa、5000~(-1)的反应条件下,由原来的5.9分别增加到11.5、9.8ml/h·lcat.。催化剂的XRD、LRS、TPR、TEM图和比表面测定结果一致表明,稀土元素可使催化剂晶粒细化、高度分散,稳定了四方相。XPS结果表明:REO的加入使表面Mn富集,且催化剂表面Mn和K的比例影响其合成甲醇、异丁醇的活性与选择性。  相似文献   

10.
 用等体积浸渍法制备了ZrO2-SiO2(ZrSiO)表面复合氧化物负载的Cu-Ni催化剂,并用IR,TPR,TPD及微反技术考察了K2O助剂对CO2和CH3OH在Cu-Ni/ZrSiO催化剂表面上的吸附及合成碳酸二甲酯(DMC)反应性能的影响.结果表明:加入K2O助剂使CO2在催化剂表面上的吸附增强,当n(K)/n(Cu+Ni)=15%时,CO2在催化剂表面上吸附后生成K2CO3;CH3OH在催化剂表面上的解离吸附态(CH3O-和H+)的吸附减弱;CO2和CH3OH在Cu-Ni/ZrSiO催化剂表面上反应的主要产物为DMC,H2O,CO和CH2O;随着K2O助剂的加入,反应转化率及DMC选择性提高,副产物(CO和CH2O)的选择性下降.根据实验结果,探讨了K2O对催化剂表面活性中心电荷分布的影响.  相似文献   

11.
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   

12.
非那雄胺能抑制5α-还原酶的活性,明显降低二氢睾酮水平,是一种治疗良性前列腺增生的有效药品。该合成工艺以甾烯酮酸为原料,将其与氯化亚砜反应,无须分离即与叔丁胺反应得17β-酰胺化合物,再氧化开环,环合,氢化,脱氢合成了非那雄胺。经元素分析、IR、1HNMR、13CNMR、MS分析表征了其结构。该法无须使用昂贵的2,2-二吡啶二硫化物和剧毒药品苯亚硒酸酐,且以乙酸铵代替氨气,降低了对设备的要求和腐蚀,更适用于工业生产。  相似文献   

13.
翟宗玺  刘树深  夏树屏 《化学学报》1990,48(10):946-950
用氧化镁氯化镁水溶液制备了8水合氯氧化镁[nMg(OH)2·MgCl2·8H2O], 并测定了其在盐酸中的溶解热, 实验结果表明, 氯氧化镁溶解热与n值呈线性关系, 根据溶解热求出5Mg(OH)2·MgCl2·8H2O和3Mg(OH)2·MgCl2·8H2O的生成热分别为-7727.1和5888.1kJ·mol^1^-。  相似文献   

14.
Two vanilloids, (5E)-8-(4-hydroxy-3-methoxyphenyl)oct-5-en-4-one (1) and 4-[3-hydroxydecyl]-2-methoxyphenol (2), isolated from the dried seeds of Grains of Paradise (Aframomum melegueta), were synthesized; the latter compound was made as the S-enantiomer and the material derived from the seeds was found to be a 1:1.7 mixture of the R and S isomers. The synthetic route used should allow the preparation of analogs having extended alkyl chains and consequently different lipophilicity, and 3, a homolog of 2, was also prepared.  相似文献   

15.

The heats of detonation of 20 simple high explosives and explosive mixtures were determined by means of an adiabatic detonation calorimeter designed by the authors. The results indicated that the performance of the instrument was reliable and the experimental data were very accurate. For explosive mixtures, there was a linear accumulative relationship between the heats of detonation of the explosive mixture and its components. Accordingly, the heats of detonation of explosive mixtures could be calculated directly from the heats of detonation of simple explosives and the characteristic heats of other components. The experiments showed that the gold or brass shell of the cylindrical charge could be substituted by a thick-walled porcelain shell, which had the advantage of cheapness.

  相似文献   

16.
Cotton cellulose was swollen in a sodium hydroxide solution and carboxymethylated by a two-bath method for different periods of time for each process. The kinetics of acid hydrolysis and the crystallinity of the swollen and carboxymethylated samples were measured. The proportion of broken bonds, rate constants for hydrolysis, and permeability of cellulose to hydrolyzing agents were calculated. The susceptibility of glycosidic linkages to acid hydrolysis was improved by carboxymethylation more than by swelling in alkali. The increased accessibility of carboxymethylcellulose to acid was regarded as a consequence of increased intra-and intercrystalline swelling and of the glycosidic bonds' weakness caused by the electron-attracting carboxymethyl group on the C-6 position.  相似文献   

17.
Main hydration products of two cement pastes, i.e. CSH-gel, portlandite (P) (and specific surface S) were studied by static heating, and by SEM, TEM and XRD, as a function of cement strength (C-33 and C-43) hydration time (th) and subsequent hydration in water vapour.Total change in mass on hydration and air drying, Mo, increased with strength of cement paste and with hydration time. Content of water escaping at 110 to 220°C, defined as water bound with low energy, mainly interlayer and hydrate water, was independent on cement strength but its content increased with (th). Content of chemically bound (zeolitic) water in CSH-gel, escaping at 220-400°C, was slightly dependent on strength and increased with (th). It was possibly derived from the dehydroxylation of CSH-gel and AFm phase. Portlandite water, escaping at 400-500°C, was independent on cement strength and was higher on longer hydration. Large P crystals were formed in the weaker cement paste C-33. Smaller crystals were formed in C-43 but they increased with (th). Carbonate formated on contact with air (calcite, vaterite and aragonite), decomposed in cement at 600-700oC. It was high in pastes C-33(1 month) and C-43(1 month), i.e. 5.7 and 3.3%, respectively; it was less than 1% after 6 hydration months (low sensitivity to carbonation) in agreement with the XRD study showing carbonates in the air dry paste (1month), and its absence on prolonged hydration (6 months) and on acetone treatment. Water vapour treatment of (6 months) pastes or wetting-drying increased this sensitivity.Nanosized P-crystals, detected by TEM, could contribute to the cement strength; carbonate was observed on the rims of gel clusters.This revised version was published online in November 2005 with corrections to the Cover Date.  相似文献   

18.
In this review, the research of the author in the field of colloidal systems is summarized. The factors influencing colloidal stability are systematized and analyzed. Examples are presented to illustrate the practical utilization of the theory of stability of colloids and thin films.This review was prepared on the basis of the works of the author, which were awarded the State Premium for 1991 in the field of science and technology, chemistry section.Institute of Physical Chemistry, Russian Academy of Sciences, 117915 Moscow. Translated from Izvestiya Akademii Nauk, Seriya Khimicheskaya, No. 8, pp. 1708–1717, August, 1992.  相似文献   

19.
20.
The aim of the presented work was the investigation of thermal oxidation of ilmenite in static air atmosphere. The investigations were carried out by use of a derivatograph (MOM, Hungary). The changes of crystallographic structure of investigated samples were identified by X-ray diffractometry on Philips PW-1710 diffractometer. In temperature above 500°C appears structure of hematite Fe2O3. On the basis of the thermogravimetric measurements, the contracting area and contracting volume models were found as the best fitting experimental data. This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

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