异丙醇和苯液相烷基化反应制备异丙苯

研究MWW结构的有机硅微孔沸石催化剂在苯和异丙醇液相烷基化反应中的性能,考察反应温度、反应压力和空速等对催化剂催化性能的影响。结果表明,反应温度低于150℃时,催化剂活性和稳定性较差,主要反应为烷基化反应及异丙醇的分子内脱水和分子间脱水反应,反应产物为异丙苯、丙烯和异丙醚。反应温度高于170℃时,催化剂活性和稳定性良好,异丙醇接近完全转化,主要反应为烷基化反应,主要产物为异丙苯和多异丙苯。随着原料空速的增大,异丙醇转化率和异丙苯选择性降低,异丙醚和丙烯选择性增大。反应压力(1.5~2.5)MPa时,反应为液相烷基化过程,反应压力的变化对催化剂催化性能影响较小。     

微波热解制备g-Fe2O3催化剂及其SCR脱硝性能

以FeSO₄·7H₂O[Fe(NO₃)₃·9H₂O]为铁源,采用新型微波热解法制备γ-Fe₂O₃[a-Fe₂O₃]催化剂样品,通过XRD、N₂等温吸附-脱附、压汞法等实验手段对催化剂样品晶相、微观孔结构等进行表征;考察两种催化剂样品的NH₃-SCR脱硝性能,通过归一化处理得到两种催化剂在不同温度下的本征脱硝反应速率,同时对比研究了γ-Fe₂O₃与钒系催化剂的脱硝活性;研究氨氮比、氧浓度等运行参数对γ-Fe₂O₃催化剂NH₃-SCR脱硝性能的影响规律,并对其抗硫抗水性能进行考察.结果表明:采用新型微波热解法可得到纯度较高的γ-Fe₂O₃催化剂,其介孔分布合理且大孔数量丰富;同时γ-Fe₂O₃催化剂表现出优于a-Fe₂O₃催化剂的脱硝性能,400℃时最大NO_x转化率达到96%,300、325、350℃下单位面积脱硝速率达到a-Fe₂O₃催化剂的3倍左右;γ-Fe₂O₃催化剂具备优良的抗硫抗水性能,其最佳氨氮比为1、最佳氧体积分数为3.5%.     

后处理方式对2,2′-二氯氢化偶氮苯合成用铂炭催化剂的影响

对2,2′-二氯氢化偶氮苯合成用3%铂炭催化剂分别进行了热处理、微波处理和超声波处理。通过BET测试和SEM表征技术以及催化反应模拟对其性能进行检测与分析。结果表明,热处理导致金属粒子团聚,催化剂的比表面积减小,邻氯硝基苯催化加氢反应性能下降;微波和超声波处理促进了金属粒子的均匀分散,增大了催化剂的比表面积,提高了催化剂在邻氯硝基苯加氢反应中的催化性能。     

裂化装置催化剂跑损分析

针对裂化催化剂使用中磨损和热崩导致细粉增多、易跑损和剂耗高的现状,分析催化剂颗粒单体强度、黏结强度、球形度、表面粗糙度、原料油性能及操作条件对磨损和热崩的影响,探讨影响催化剂使用寿命因素的作用机理,提出减少跑损的相应措施。     

Pd-Cu/γ-Al_2O_3双金属催化剂脱除水中硝酸盐

采用分步浸渍法和共浸渍法制备系列Pd负载质量分数为1%的Pd-Cu/γ-Al2O3双金属催化剂,以氢气为还原剂研究其对水中硝酸盐催化脱除的性能。结果表明,催化剂中Cu与Pd物质的量比以及Cu、Pd的浸渍顺序对催化剂性能有重要影响,硝酸根转化率随着Cu与Pd物质的量比的增大而增大;硝酸根转化活性以Cu与Pd物质的量比为5∶1、先浸渍Pd再浸渍Cu所得催化剂较优;从氨氮选择性方面看,以先浸渍Cu后浸渍Pd制备的催化剂选择性较低,在Cu与Pd物质的量比为1∶1、先浸渍Cu再浸渍Pd所得催化剂较优。     

H3PW12O40/Y-β催化氯乙酸异戊酯的绿色合成

采用Y-β复合分子筛负载H₃PW₁₂O₄₀为催化剂,对氯乙酸与异戊醇酯化反应合成氯乙酸异戊酯进行研究,考察催化剂用量、异戊醇与氯乙酸物质的量比、反应时间及催化剂重复使用次数等对酯收率的影响。结果表明,H₃PW₁₂O₄₀/Y-β催化剂具有催化性能高、易回收及较好的重复使用性能等优点。在氯乙酸0.1 mol、异戊醇与氯乙酸物质的量比1.2、催化剂用量0.8 g和反应时间45 min最佳反应条件下,氯乙酸异戊酯收率为93.5％     

超声法制备Ni/HKUST-1催化剂

HKUST-1催化剂作为当今纳米材料研究的热点之一,具有优良的表面性能。而在催化领域方面,使用金属-有机骨架(MOFs)材料作为催化剂的催化效果不是很明显,利用不同金属之间的协同作用有望提高该材料的催化性能,有必要对MOFs的表面进行修饰。采用超声法、过量浸渍法和溶胶-凝胶法在HKUST-1催化剂表面负载金属Ni,并利用原子分光光度计检测3种方法的负载性能,结果表明,超声法的负载性能最好。     

不同载体对Pt-Sn催化剂丙烷催化脱氢性能影响

分别以Hβ分子筛和γ-Al₂O₃为载体,采用浸渍法制备不同Sn含量的负载型Pt-Sn双组分丙烷催化脱氢催化剂。在固定床微反装置上对制备的催化剂进行活性评价,并采用NH₃-TPD方法测定催化剂表面酸量和酸强度分布。结果表明,负载型Pt-Sn/Hβ和Pt-Sn/γ-Al₂O₃催化剂对丙烷催化脱氢反应性能与Sn含量密切相关,弱酸中心的存在对丙烷催化脱氢反应有利,对于特定的Pt-Sn体系,γ-Al₂O₃为载体的催化剂性能优于Hβ分子筛为载体的催化剂,当负载Sn质量分数为0.9时,Pt-Sn/γ-Al₂O₃催化剂性能最好。     

Ir/C催化剂氯代硝基苯选择性催化加氢反应性能

采用浸渍法制备Ir/C和Pd/C催化剂,并用于氯代硝基苯选择性催化加氢反应,采用ICP-MS、XRD、XPS和TEM等手段对催化剂进行表征。结果表明,在相同负载量条件下,Ir在活性炭表面的分散与Pd有显著差异,Ir颗粒粒径更小且更均匀。在氯代硝基苯液相催化加氢反应中,Ir催化剂的催化活性较低,对氢解脱氯副反应有较好的抑制作用,这些性能与Ir的特殊性能有关。     

碱土金属修饰的Co/RPSA催化剂催化分解N2O

以RPSA分子筛为载体,采用浸渍法制备了一系列以Co为主活性组分和碱土金属为助剂的CoM/RPSA（M=Mg、Ca、Sr和Ba）催化剂,考察了含硫和含氧条件下直接催化分解N2O的性能。采用X射线衍射、热重-质谱联用系统、NH3-TPD和N2O-TPD等方法对催化剂进行了表征。XRD结果表明,Co物种主要以Co3O4尖晶石形态存在。NH3-TPD和N2O-TPD结果表明,碱土金属的种类影响催化剂酸性和对反应物N2O的吸附-脱附性能,催化剂活性与催化剂酸性及其对反应物N2O的吸附-脱附性能有关。催化剂活性评价结果显示,CoSr/RPSA催化剂的N2O分解活性较好,N2O转化率达到95%时的反应温度为471 ℃。     

Catalytic combustion technology to achieve ultra low NOx, emissions: Catalyst design and performance characteristics

A catalytic combustion system has been developed which feeds full fuel and air to the catalyst but avoids exposure of the catalyst to the high temperatures responsible for deactivation and thermal shock fracture of the supporting substrate. The combustion process is initiated by the catalyst and is completed by homogeneous combustion in the post catalyst region where the highest temperatures are obtained. Catalysts have been demonstrated that operate at inlet temperatures as low as 320°C at 11 atm total pressure and conditions typical of high performance industrial gas turbines. The ignition temperature is shown to correlate with the specific catalytic activity of the washcoat layer over a rather broad range of activities. A reaction model has been developed that can predict ignition behavior from the measured catalytic activity.     

Highly active recyclable SBA-15-EDTA-Pd catalyst for Mizoroki-Heck,Stille and Kumada C–C coupling reactions

Highly efficient SBA-15-EDTA-Pd(11) heterogeneous catalyst was synthesized by covalent anchoring Pd-EDTA complex over organo-modified surface of SBA-15. SBA-15-EDTA-Pd(11) catalyst was found to exhibit excellent catalytic activity in appreciable yield for Heck, Stille and Kumada cross-coupling reactions. Catalytic system exhibited excellent activity for completion of reaction, isolation, Pd loading (0.87 mmol%) and yields of products as compared to earlier reported heterogeneous supported Pd catalysts. Covalently anchored heterogeneous SBA-15-EDTA-Pd(11) catalyst can be recycled for more than five times without noticeable loss in activity and selectivity.     

预处理温度对SAPO-11催化丁烯骨架异构化性能的影响

采用水热合成法合成的SAPO-11分子筛，经酸洗、干燥和焙烧处理得H-SAPO-11分子筛，考察了预处理温度对催化剂物化性能的影响，采用XRD、XRF、IR和NH₃-TPD等手段对催化剂进行表征。实验证明，500 ℃预处理后H-SAPO-11分子筛的结构缺陷较少，B酸位较多，骨架更完美；将其成型制成催化剂，对丁烯骨架异构化反应显示更优良的催化活性、选择性和稳定性。     

SAPO-11分子筛催化丁烯异构化反应的研究

在连续流动固定床反应装置上,考察了温度、空速及添加水蒸汽对混合丁烯在SAPO-11分子筛催化剂上骨架异构化的影响。结合催化剂的NH₃-TPD表征与Al₂O₃催化剂的评价结果,对催化剂酸性能和孔结构与丁烯骨架异构化进行了关联。结果表明,对于丁烯骨架异构,分子筛催化剂优于Al₂O₃催化剂,显示出催化剂孔结构的重要作用。SAPO-11分子筛酸量越小,转化率越低,酸量过小时催化剂基本没有活性,说明丁烯异构转化与表面酸量有密切关系。分子筛催化剂上,添加少量的水蒸汽使转化率有所降低,但异丁烯选择性明显增加。     

Sr_xCa_（1-x）NiAl_（11）O_（19）催化剂的制备及其催化甲烷燃烧活性研究

用异丙醇盐水解法制备SrxCa1-xNiAl11O19（x=1.0,0.75,0.5,0.25,0）催化剂,通过X射线衍射、比表面积分析等实验技术及甲烷燃烧,对催化剂的结构和性质进行了考察。研究了掺杂不同量的钙离子对催化剂的结构以及对甲烷催化燃烧活性的影响。结果表明,催化剂在1 200℃焙烧后可以形成完整的六铝酸盐晶型,同时具有较高的催化性能和高温稳定性,不同量的Ca离子掺杂对于催化剂的比表面积有较大的影响。Sr0.25Ca0.75NiAl11O19催化剂具有较好活性,其起燃温度（T10%/℃）为590℃,完全转化温度（T90%/℃）为730℃。     

SrxCa1-xNiAl11O19催化剂的制备及其催化甲烷燃烧活性研究

用异丙醇盐水解法制备SrxCa1-xNiAl11O19(x=1.0,0.75,0.5,0.25,0)催化剂,通过X射线衍射、比表面积分析等实验技术及甲烷燃烧,对催化剂的结构和性质进行了考察。研究了掺杂不同量的钙离子对催化剂的结构以及对甲烷催化燃烧活性的影响。结果表明,催化剂在1 200℃焙烧后可以形成完整的六铝酸盐晶型,同时具有较高的催化性能和高温稳定性,不同量的Ca离子掺杂对于催化剂的比表面积有较大的影响。Sr0.25Ca0.75NiAl11O19催化剂具有较好活性,其起燃温度(T10%/℃)为590℃,完全转化温度(T90%/℃)为730℃。     

Selective catalytic reduction of NO with propene over CuMFI zeolites: dependence on Si/Al ratio and copper loading

Selective catalytic reduction of nitrogen oxide by propene in an oxidising atmosphere was studied on several CuMFI catalysts with different Si/Al ratios (11 Si/Al 100) and different copper loadings (between 0 and 5.5 wt.-%). From the results it was observed that the influence of zeolite Si/Al ratio on CuMFI catalytic activity for NO SCR by propene is dependent on the catalyst copper loading. Furthermore, the effect of catalyst copper loading on catalytic performance depended on the catalyst Si/Al ratio. The results also demonstrated that CuMFI catalysts with different Si/Al ratios and copper loadings, but with the same Cu/Al ratio and, therefore, the same copper exchange level have similar catalytic activity profiles for NO SCR.

It was further observed that not all Cu cations exchanged into MFI catalysts have equivalent catalytic activity for NO SCR, which made the existence of different copper environments on CuMFI catalysts evident, isolated Cu²⁺ ions being the most active species for NO SCR by propene.

Moreover, the results showed an improvement of the CuMFI catalytic activity at low temperatures by increasing the catalyst copper exchange level and, consequently, decreasing the number of Brönsted acid sites, which can be performed either by increasing the zeolite Si/Al ratio or copper loading.     

TiO2对乙苯脱氢制苯乙烯催化剂中KFe11O17活性相结构的影响

采用穆斯堡尔谱,X-射线衍射和程序升温还原等方法,研究了乙苯脱氢铁钾系催化剂中氧化钛对铁钾活性相KFe_(11)O_(17)结构形成的影响。发现添加适量的氧化钛对形成KFe_(11)O_(17)物相有利,当催化剂中Fe_2O_3,K_2O,CeO_2和Mo_2O_3的质量比固定为75.0:12.0:7.0:3.0,而Fe_2O_3与TiO_2质量比为75.0:0.1时,TiO_2对铁钾尖晶石结构形成的促进作用最明显,催化剂的活性也最高。但当TiO_2添加的质量比继续提高,会抑制铁钾尖晶石的形成,从而使催化剂的活性下降。当Fe_2O_3与TiO_2的质量比为75.0:1.0时,催化剂内的铁钾尖晶石结构遭到破坏。     

Coke burning behavior of a catalyst of ZSM-5/ZSM-11 co-crystallized zeolite in the alkylation of benzene with FCC off-gas to ethylbenzene

Since the commercialization of ethylbenzene production via alkylation of benzene with the dilute ethene in FCC off-gas over a ZSM-5/ZSM-11 co-crystallized zeolite catalyst in China, the catalyst has been regenerated several times and showed good regeneration performance. During the alkylation process, the catalytic activity decreases, some of the catalyst pores are blocked and the acid centers are partly covered by coke deposition. Influence of the factors such as catalyst particle size, temperature, etc. on the burning rate of the coke was investigated by the TG technique, and a rate equation for coke burning on the ZSM-5/ZSM-11 co-crystallized catalyst was established.     

CeMn_xAl_（12-x）O_（19-δ）催化剂的制备及甲烷燃烧性能研究

采用共沉淀法制备了一系列CeMnxAl12-xO19-δ（x=1,2,3）催化剂,通过甲烷活性测试对其催化性能进行表征。结果表明：以NH4HCO3为沉淀剂的CeMnAl11O19-δ的催化活性比以氨水为沉淀剂的高,起燃温度T10为480℃,氨水为沉淀剂的起燃温度T10高达669℃;Mn掺杂量对催化剂的活性有很大的影响,其中CeMn2Al10O19-δ的催化活性最高,起燃温度T10为445℃,完全转化温度T为728℃。