(CeO_2-ZrO_2-Al_2O_3)-(La_2O_3-Al_2O_3)复合氧化物负载的Pd密偶催化剂:载体焙烧温度的影响

采用同时共沉淀法制备了(CeO2-ZrO2-Al2O3)-(La2O3-Al2O3)新型复合氧化物(CZA-LA),考察了焙烧温度对CZA-LA负载的Pd密偶催化剂的影响,并采用N2吸附-脱附法和X射线衍射对其进行了表征.结果表明,随着焙烧温度的升高,尽管CZA-LA样品的比表面积降低,但即使在1000°C焙烧5h后,其比表面积仍能保持在122m2/g左右;另外,CZA-LA样品的孔体积降低幅度不大,当在700℃及更高温度下焙烧后基本上保持稳定.以不同温度焙烧5h后的样品为载体,采用等体积浸渍法制备了一系列整体式Pd/CZA-LA密偶催化剂(Pd含量2.0g/L).催化剂对消除模拟汽油车尾气中C3H8活性测试结果表明,各新鲜催化剂的活性相差不大,均具有较低的起燃温度T50和完全转化温度T90.当催化剂经老化处理后,以1000°C焙烧的载体负载的Pd催化剂活性最高,T50和T90分别为310和341℃,ΔT仅为31℃,仅比新鲜催化剂的高7℃.可见,该催化剂表现出优异的催化活性和抗老化性能,可以满足欧Ⅳ及更高标准的用于汽油车尾气净化的密偶催化剂的性能要求.     

满足欧V排放标准的汽油车中偶催化剂

制备了具有高性能的稀土储氧材料Ce0.65Zr0.25Y0.07La0.03O1.95和镧稳定的氧化铝(La-Al2O3),并以此为基础制备了Pt-Pd-Rh型中偶汽油车尾气净化催化剂.老化前后的性能检测表明,稀土储氧材料具有较大的比表面积和优异的储氧性能,La-Al2O3也具有优越的织构性能和高的热稳定性.催化剂对模拟尾气具有较高的催化活性和稳定性,在捷达-MT型汽油车上的测试结果表明,经该催化剂处理后的尾气排放能够满足欧Ⅴ排放标准.     

满足欧Ⅲ排放标准的压缩天然气汽车中偶催化剂

制备了具有高性能的稀土储氧材料Ce0.45Zr0.45Y0.05La0.05O2和耐高温大比表面积材料La-Al2O3,并以此为基础制备了Pt-Rh型中偶压缩天然气汽车尾气净化催化剂.催化剂对模拟尾气具有较高的催化活性和稳定性,在捷达-MT型压缩天然气汽车上的测试结果表明该催化剂能够满足欧Ⅲ排放标准.     

满足欧Ⅲ排放标准的汽油车中偶催化剂

 制备了高性能稀土储氧材料Ce0.5Zr0.4Y0.1O2和镧稳定的氧化铝(La-Al2O3), 并以此为基础制备了中偶汽油车尾气净化催化剂. 经老化前后的性能检测证实,稀土储氧材料具有优异的织构性能和储氧性能且高温稳定性优良; La-Al2O3具有优异的织构性能及优异的抗高温老化性能. 中偶催化剂对HC, CO和NOx具有优异的低温活性、抗高温老化性能和低的劣化系数. 捷达-MT型汽油车排放检测表明该催化剂能够满足欧Ⅲ排放标准.     

La2O3对Pd密偶催化剂性能的影响

采用浸渍法制备了不同La2O3含量的Pd密偶催化剂.使用低温N2吸附-脱附、X射线衍射、H2程序升温还原、CO化学吸附和X射线光电子能谱等技术考察了La2O3对催化剂性能的影响.模拟汽车尾气条件考察了催化剂上丙烷的转化活性.活性测试结果表明,La2O3的添加能显著提高催化剂对丙烷的转化活性和催化剂的热稳定性.H2-TP...     

稀土在机动车尾气催化净化中的应用与研究进展

随着我国机动车尾气排放法规日趋严格,对机动车尾气净化催化剂性能提出了更高的要求.稀土元素由于独特的4f电子层结构和储放氧性能等特性,在机动车尾气催化剂中得到广泛应用.本文综述了稀土元素在机动车尾气催化剂中的应用及相关机理研究现状,并依据京V排放法规要求探讨了最新排放限值对尾气净化催化剂性能的要求,分析了稀土在开发高性能催化剂中的作用,并对稀土在机动车尾气净化催化剂中的应用前景进行了展望.     

钾掺杂三维有序大孔结构Mn0.5Ce0.5Oδ催化剂合成及其催化燃烧炭烟性能

柴油发动机是一种高效耐用的发动机,具有广阔的应用前景.但柴油车尾气中的炭烟颗粒吸附了许多有毒有害物质,也是城市PM2.5的主要来源之一,对人类生命安全造成极大威胁.因此,降低和消除柴油车尾气中的炭烟颗粒是柴油车尾气净化的重要任务.尾气后处理是炭烟颗粒进入大气环境前的最后一道程序,可有效控制柴油车尾气中炭烟颗粒排放.其中,催化净化催化剂是尾气后处理技术的核心.研究表明,炭烟颗粒催化燃烧是一个气-固-固三相深度氧化反应,因此开发新型催化剂体系,改善催化剂与炭烟颗粒的接触,提高催化剂的本征活性,对于研制高活性炭烟燃烧催化剂具有重要的实际意义. 对于三维有序大孔(3DOM)结构催化剂,大孔有利于炭烟颗粒进入催化剂内部并与活性位点接触,而有序的孔道结构可以促进炭烟颗粒在催化剂孔道内传输.因此,将催化炭烟颗粒燃烧催化剂设计成3DOM结构,可促进炭烟颗粒催化燃烧,提高催化剂活性.研究表明,锰铈复合氧化物材料在炭烟颗粒催化燃烧中表现出比单一的锰氧化物和铈氧化物更好的性能.而将K与Ce和Mn形成复合氧化物,利用三者之间的协同作用,将可使K掺杂3DOM结构Mn0.5Ce0.5Oδ催化剂具有更高的催化活性.本文利用胶体晶体模板法成功制备了3DOM结构的Mn0.5Ce0.5Oδ复合氧化物,并采用简单的等体积浸渍方法成功制备了不同K担载量的K掺杂3DOM结构Mn0.5Ce0.5Oδ催化剂(K-MCO).表征结果表明, K-MCO催化剂具有贯通有序的大孔结构,但焙烧温度和焙烧时间会对大孔结构的规整性有一定影响;催化剂中K含量、焙烧温度和焙烧时间对K-MCO的晶型影响较大,催化剂中出现了一个新的晶相K2Mn4O8.另外, K含量、焙烧温度和焙烧时间对催化剂的氧化还原性能也有较大影响.评价结果表明,所制催化剂对炭烟催化燃烧均具有较高活性,其中20% K-MCO-4h催化剂活性最高,催化燃烧炭烟的T50(炭烟的最大燃烧峰值)为331oC, CO2选择性为95.3%.催化剂的大孔结构效应以及K, Mn和Ce三者间的协同作用有利于提高催化剂催化燃烧炭烟的活性.另外,由于柴油车尾气排气口温度范围为175–400 oC,而本文所制催化剂催化燃烧炭烟的温度低于400 oC,因此该催化剂可以在柴油车尾气排气口温度范围内进行炭烟催化燃烧.由于具有合成步骤简单、活性高以及成本低等优点,该催化剂在实际应用方面具有广阔前景.     

柴油机尾气净化催化剂的最新研究进展

柴油机尾气排放的污染物已经引起了严重的环境污染问题,催化净化技术是柴油机尾气污染治理必不可少和最有效的处理技术之一,而高效催化剂的研制和开发是催化净化技术的核心.本文以柴油机尾气中最难处理的两种污染物NOx和碳烟颗粒(PM)的催化处理技术为主线,综述了NOx的催化还原(选择性催化还原(SCR)和贮存还原(NSR))催化剂、碳烟的催化燃烧催化剂、NOx和碳烟颗粒同时消除的催化剂及柴油机尾气四效催化剂的最新研究进展,并总结性地提出了目前该研究方向存在的主要问题和发展方向.     

柴油车排放碳黑颗粒消除催化剂的研究进展

 柴油车尾气排放的碳黑颗粒已引起严重的环境污染问题. 对于柴油车尾气碳黑颗粒的处理必须使用高活性的催化剂来加快碳黑颗粒在低温下的氧化速率. 本文总结了柴油车排放碳黑颗粒催化燃烧用几种不同类型的催化剂,即碱金属或碱土金属催化剂、贵金属催化剂、过渡金属催化剂以及复合型催化剂,归纳了它们的催化作用机理,比较了它们在松散接触与紧密接触时的不同催化活性,概括了这些催化剂的最新研究进展,并对它们在实际应用中存在的问题和应用前景进行了探讨.     

性能优异的Rh改性的Pd/Al2O3密偶催化剂

采用等体积浸渍法制备了Pd/Al2O3和Rh-Pd/Al2O3密偶催化剂,运用H2程序升温还原、CO化学吸附和X射线光电子能谱等手段对催化剂进行了表征,并考察了催化剂对丙烷总包反应和单反应的转化活性.总包反应结果表明, Rh的添加使起燃温度和完全转化温度分别降低了23和18oC.单反应结果证明,添加Rh能提高各单反应丙烷的转化活性,尤其是有NO参与的反应.表征结果证明,掺杂Rh不仅可以抑制活性组分PdOx的烧结,提高PdOx的分散度,而且可以改变其电子状态.     

Pd Close Coupled Catalyst

Europe III standards require significantly higher emissions reduction, especially for hydrocarbon (HC). For a typical vehicle, a large portion (up to 80 %) of the HC emissions occurs during cold start. A variety of technologies are under development to reduce cold start HC emissions, including close coupled catalysts1; electrically heated catalysts2 and hydrocarbon absorbers3. Among them, the close coupled catalyst gradually dominated the technologies4. A high performance close coupled cat…     

Au/SBA-15 的制备及其催化 CO 氧化反应性能

 以 SBA-15 为载体, 采用沉积沉淀法制备了纳米 Au 催化剂, 研究了不同预处理条件对 Au 在载体表面状态的影响, 考察了催化剂样品催化 CO 氧化性能. 以高分辨率透射电子显微镜、N2 吸附、X 射线衍射、紫外-可见漫反射吸收谱、X 射线光电子能谱和电感耦合等离子体发射光谱等手段对催化剂的结构和表面性质进行了表征. 结果表明, 经还原焙烧处理后的 Au/SBA-15 催化剂热稳定性较好, Au 在 SBA-15 孔道表面呈高分散状态, 样品在 CO 氧化反应中表现出优异的低温催化活性和高温稳定性, 同时具有优异的抗烧结性能和良好的循环稳定性.     

新型CeO2/HBEA催化剂上NH3低温还原NO活性及抗毒性能研究

采用等体积浸渍法制备了CeO2/HBEA催化剂,用于NH3选择性催化还原NO.考察了CeO2负载量、焙烧温度、氧浓度、空速、以及SO2和水蒸气等因素对催化剂活性的影响,并运用BET、X射线衍射(XRD)、扫描电镜(SEM)、热重分析(TGA)、傅里叶红外(FTIR)等手段对该催化剂进行表征,研究了催化剂的晶相、微观形貌与抗毒机制.结果显示:CeO2/HBEA催化剂具有良好的脱硝活性,高活性温度窗口在220～400℃,当反应温度为220℃、空速为12 000 h-1时,NO的转化率达96.49%.H2O的存在对催化剂的脱硝活性无明显影响.SO2一定程度抑制该催化剂的低温脱硝活性,但随着温度的升高,其脱硝活性得到一定恢复.所制备的CeO2/HBEA催化剂有良好的低温活性,能适应较高的空速,且具有较强的抗硫性和抗水中毒性能,有一定的应用前景.     

二维M-Co3O4负载Ir对香草醛加氢脱氧性能研究

以二维金属-有机框架M-Co₃O₄为载体制备了具有高活性的Ir/M-Co₃O₄催化剂.采用X射线粉末衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)、电感耦合等离子体发射光谱仪(ICP-OES)、 N₂物理吸/脱附等方法对催化剂进行了表征,并研究了催化剂、温度、时间、溶剂等因素对香草醛加氢脱氧反应的影响.结果表明, Ir/M-Co₃O₄催化剂具有较好的普适性和稳定性,在香草醛加氢脱氧制备4-甲基愈创木酚(MMP)反应中表现出较高的活性和选择性,香草醛的转化率达100%, MMP的选择性不低于99%.     

Preparation,characterization and application of NiGaCu/MSO catalyst in conversion of carbon dioxide to methanol under mild pressure

In this paper, a novel catalyst was prepared based on NiGaCu alloys supported on ordered mesoporous silicon oxide (NiGaCu/MSO catalyst), through impregnation method. The impregnation was followed by drying the precipitation overnight, calcining it at 600 ​°C for 6 ​h under the air, and activating it in NaBH₄/ethanol solution at ambient temperature for 6 ​h. The NiGaCu/MSO catalyst was applied in conversion of CO₂ to CH₃OH by H₂ under mild pressure. The investigations over the prepared catalyst showed that the conversion could be carried out under pressure of 15 ​bar with very high conversion of CO₂ and good selectivity of CH₃OH compared to previous catalysts. The NiGaCu/MSO was characterized by many techniques including SAXRD, WAXRD, FT-IR, H₂-TPR, SEM and TEM. GC coupled with TCD and FID was used for determining the gas composition of the process.     

In situ prepared CuI nanoparticles on modified poly(styrene-co-maleic anhydride): an efficient and recyclable catalyst for the azide–alkyne click reaction in water

A facile, high-yielding and straightforward methodology for the copper-catalyzed synthesis of 1,4-disubstituted 1,2,3-triazoles in water, using in situ prepared copper nanoparticles (NPs) on modified poly(styrene-co-maleic anhydride) [SMA] catalyst, is reported. The polymer support was easily prepared from the reaction of SMA with 4-aminopyridine and subsequently underwent reaction with CuI NPs. The catalyst was applied for the preparation of triazoles under air, followed by chromatographic separation of the products. The polymer-supported catalyst not only showed high catalytic activity but also showed high 1,4-regioselectivity for the [3 + 2] Huisgen cycloaddition in water as solvent. The products were obtained in good to excellent yields in all cases. The catalyst can be used without pre-activation and reloaded for at least five runs without significant decrease in its activity. The catalyst was characterized by SEM, energy dispersive spectroscopy analysis of X-rays, and inductively coupled plasma.     

Product oriented oxidative bromination of methane over Rh/SiO_2 catalysts

Rh/SiO2 was prepared for the oxidative bromination of methane. The catalyst was prepared by calcination at different temperatures and for different times to obtain catalysts with different specific surface areas for the purposes of producing either CH3Br or CH3Br and CO. It was found that the catalyst having a low specific surface area (calcined at relatively high temperature) favors the selective oxidation of methane to prepare CH3Br, while the catalyst having a high specific surface area favors the deeper partial oxidation of methane, which is good for CH3Br and CO preparation.The 650 h on stream life-time test revealed that the catalytic performance of the 0.4Rh/SiO2-900-10 catalyst was excellent.Both methane conversion and CH3Br selectivity kept increasing trends during the life-time test.No matter how serious was the Rh leaching during the reaction,the 0.4Rh/SiO2-900-10 catalyst did not deactivate at all.     

Product oriented oxidative bromination of methane over Rh/SiO2 catalysts

Rh/SiO2 was prepared for the oxidative bromination of methane. The catalyst was prepared by calcination at different temperatures and for different times to obtain catalysts with different specific surface areas for the purposes of producing either CH3Br or CH3Br and CO. It was found that the catalyst having a low specific surface area (calcined at relatively high temperature) favors the selective oxidation of methane to prepare CH3Br, while the catalyst having a high specific surface area favors the deeper partial oxidation of methane, which is good for CH3Br and CO preparation. The 650 h on stream life-time test revealed that the catalytic performance of the 0.4Rh/SiO2--900-10 catalyst was excellent. Both methane conversion and CH3Br selectivity kept increasing trends during the life-time test. No matter how serious was the Rh leaching during the reaction, the 0.4Rh/SiO2--900-10 catalyst did not deactivate at all.     

热稳定性能良好的磺化聚醚砜酮催化剂

采用磺酸化的方法制备了一种热稳定性能良好的新型固体酸树脂催化剂——磺化聚醚砜酮树脂(S-PPESK),并应用在异丁烯的低聚反应中.S-PPESK在较低的温度条件下对异丁烯的低聚反应表现出了很高的催化活性和二聚反应选择性.对S-PPESK的热稳定性能采用预处理的方法进行了测试,结果显示它的预处理温度高达180 ℃,与商业磺酸树脂的预处理温度相比高出约40 ℃. S-PPESK在异丁烯的低聚反应中表现出了良好的催化活性、优良的二聚反应选择性和很好的热稳定性能,其应用前景广泛.