|
|
|
题名
|
作者
|
年代
|
出处
|
被引量
|
| 1 | 钙改性的Pd/CeO_2-ZrO_2-Al_2O_3催化剂催化甲醇裂解反应显示文摘采用共沉淀法制备了未改性的和Ca掺杂的CeO2-ZrO2-Al2O3样品,进一步用浸渍法制备了Pd/CeO2-ZrO2-Al2O3(Pd/CZA)和Pd/CeO2-ZrO2-Al2O3-CaO(Pd/CZACa)催化剂.运用X射线衍射、N2吸附-脱附、储氧量测定、CO化学吸附、NH3程序升温脱附、CO2程序升温脱附、H2程序升温还原和X射线光电子能谱对催化剂进行了表征,并考察了其催化甲醇裂解反应活性.结果表明,Ca的添加使载体酸性位中毒,弱碱中心数目增加,从而影响了催化剂上吸附物种的吸附-脱附平衡过程;同时,使得金属和载体间相互作用增强,增加了Pd周围的电子密度,使Pd保持在部分氧化状态Pdδ+(0<δ<2),进而提高了甲醇催化裂解反应的活性,使甲醇完全裂解温度降低了34°C. | 李雪 王晓文 赵明 刘建英 龚茂初 陈耀强 | 2011 | 催化学报2011，32，11： | 8 |
| 2 | 多级孔ZSM-5分子筛的合成及其在甲醇脱水制二甲醚反应中的应用(英文)显示文摘以四丙基氨为微孔模版剂, 阳离子高分子聚合物为介孔模版剂, 合成了具有多级介孔的ZSM-5分子筛, 并用于甲醇气相脱水合成二甲醚. 结果表明, 加入阳离子高分子聚合物后, 合成的HZSM-5分子筛样品既保持了其MFI典型结构, 又呈现了多级介孔特征; 随着阳离子高分子聚合物模板剂加入量的增加, 其多级介孔特征更为明显. 具有多级介孔的HZSM-5分子筛表现出比常规微孔HZSM-5分子筛高的反应稳定性和二甲醚选择性, 这主要是由于其织构和酸性的双重作用. | 杨琦 张海涛 孔猛 包秀秀 费金华 郑小明 | 2013 | 催化学报2013，34，8： | 7 |
| 3 | Effect of ultrasonic irradiation and /or halogenation on the catalytic performance of γ-Al_2O_3 for methanol dehydration to dimethyl ether显示文摘Dimethyl ether(DME) is amongst one of the most promising alternative,renewable and clean fuels being considered as a future energy carrier.In this study,the comparative catalytic performance of the halogenated γ-Al 2 O 3 prepared from two halogen precursors(ammonium chloride and ammonium fluoride) is presented.The impact of ultrasonic irradiation was evaluated in order to optimize both the halogen precursor for the production of DME from methanol in a fixed bed reactor.The catalysts were characterized by SEM,XRD,BET and NH 3-TPD.Under reaction conditions where the temperature ranged from 200 to 400 ℃ with a WHSV = 15.9 h-1was found that the halogenated catalysts showed higher activity at all reaction temperatures.However,the halogenated alumina catalysts prepared under the effect of ultrasonic irradiation showed higher performance of γ-Al 2 O 3 for DME formation.The chlorinated γ-Al 2 O 3 catalysts showed a higher activity and selectivity for DME production than fluorinated versions. | Sameh M.K.Aboul-Fotouh | 2013 | 燃料化学学报2013，41，9： | 4 |
| 4 | 甲醇制低碳烯烃分子筛催化剂研究进展显示文摘MTO(甲醇制烯烃)和MTP(甲醇制丙烯)是两个重要的轻烯烃生产新工艺。总结用于MTP、MTO的催化剂的研究进展,着重介绍了ZSM-5和SAPO-34两种分子筛催化剂的改进。 | 尚会建 张少红 周艳丽 张高 赵丹 赵彦 郑学明 | 2012 | 天然气化工—C1化学与化工2012，37，5： | 4 |
| 5 | Ag对Pd/CeO_2-ZrO_2-La_2O_3-Al_2O_3催化氧化甲醇性能的影响显示文摘采用等体积共浸渍法制备了一系列Pd-Ag/CeO2-ZrO2-La2O3-Al2O3催化剂。运用N2吸附-脱附,X射线衍射(XRD),H2程序升温还原(H2-TPR),紫外-可见漫反射光谱(UV-Vis DRS),X射线光电子能谱(XPS)对催化剂进行表征,并考察其对甲醇的催化氧化性能。活性测试结果表明,Ag的添加可显著改善Pd催化剂对甲醇的催化氧化活性,T50、T90以及ΔT分别为125℃,150℃和25℃,具有较好的应用前景。H2-TPR表明,引入Ag可明显改善催化剂的还原性能,使表面易还原氧物种量增多,还原速率加快;UV-Vis DRS及XPS表明,Pd、Ag金属之间以及金属与载体之间存在电子效应,这种效应促使金属与载体界面产生大量具有活性的氧物种,不仅提高了催化剂的低温活性,还提高了催化剂的氧化速率。 | 张雪乔 王世丹 信欣 刘盛余 陈耀强 赵明 | 2012 | 无机化学学报2012，28，8： | 4 |
| 6 | Dimethylether production on zeolite catalysts activated by Cl^-,F^- and / or ultrasonication显示文摘The chlorinated and fluorinated zeolite catalysts were prepared by the impregnation of zeolites( H-ZSM-5,H-MOR or H-Y) using two halogen precursors( ammonium chloride and ammonium fluoride) in this study. The influence of ultrasonic irradiation was evaluated for optimizing both halogen precursors for production of dimethylether( DME) via methanol dehydration in a fixed bed reactor. The catalysts were characterized by SEM,XRD,BET and NH3-TPD. The reaction conditions were temperatures from 100 to 300 ℃ and a WHSV = 15. 9 h-1. All halogenated catalysts showhigher catalytic activities at all reaction temperatures studied. However, the halogenated zeolite catalysts prepared under ultrasonic irradiation showhigher performance for DME formation. The chlorinated zeolite catalysts show higher activity and selectivity for DME production than the respective fluorinated versions. | Sameh M.K.Aboul-Fotouh Noha A.K.Aboul-Gheit Mona A.Naghmash | 2016 | 燃料化学学报2016，44，4： | 2 |
| 7 | 异丁烯直接胺化合成叔丁胺反应的热力学研究(英文)显示文摘叔丁胺是一种重要的有机化工中间体,广泛应用于制备橡胶促进剂,医药,农药,着色剂等诸多下游产物.目前,叔丁胺主要的生产方法,如叔丁脲水解法,异丁烯-氢氰酸法(Ritter法),卤代烃胺化法等存在产品收率较低,涉及强酸/强碱的使用,对设备腐蚀和环境污染严重等问题.异丁烯直接胺化生产叔丁胺,原子利用率100%,是典型的绿色化学反应.20世纪末,BASF公司以β沸石为催化剂,率先实现了异丁烯胺化技术的工业应用.但是,其反应条件苛刻,压力达28MPa,生产过程能耗大,对设备材质要求高.目前,关于异丁烯直接胺化的文献较少,且相关研究多在远离工业应用的常压条件下进行.同时,对于异丁烯直接胺化反应过程的热力学,特别是缓和反应条件下的热力学尚待进一步系统和深入地研究分析,以期指导低温低压条件下高性能胺化催化剂的研发和工艺条件优化.我们计算了473–573 K间,异丁烯胺化制备叔丁胺反应的ΔrH,ΔrG,Kp等热力学数据.在此基础上,分析了反应温度,压力和氨烯比(摩尔比)对异丁烯平衡转化率(叔丁胺选择性>99%,未予考虑)的影响.结果表明,异丁烯胺化是中等强度的放热反应,升高反应温度会急剧降低异丁烯的平衡转化率,如在5 MPa,氨烯比1的条件下,反应温度从473 K提高到573 K,异丁烯平衡转化率从40.6%降到6.9%.但从动力学角度而言,升温可提高胺化反应速率,因此在特定的反应条件下和催化剂上,必然存在最佳反应温度.提高反应压力和氨烯比有利于提高异丁烯的热力学平衡转化率.开发在低温和相对较低的压力下具有较高胺化活性的催化剂是提高该过程经济性和实用性的关键.在较缓和的反应条件下(523 K,5 MPa,氨烯比4及异丁烯空速0.5 h^(–1)),考察了ZSM-5(R=50和R=412,R为硅铝比,下同),ZSM-11(R=48),MOR(R=10),SAPO-11(摩尔组成,1.6Al_2O_3:1.0SiO_2:1.4P_2O_5)等不同拓扑结构分子筛以及氧化铝在异丁烯胺化反应中的性能.结果表明,空白试验中,无叔丁胺产物生成.在ZSM-11上的获得最高的异丁烯胺化转化率,为14.2%(达到平衡转化率的52.2%),在ZSM-5(R=50),ZSM-5(R=412)和MOR上,异丁烯转化率分别为13.9%,6.4%和2.9%,叔丁胺选择性均大于99.8%.而SAPO-11和氧化铝未呈现出胺化反应活性.关联氨气程序升温脱附,吡啶吸附红外表征结果及分子筛孔结构特点,表明分子筛胺化活性与其孔径及Br?nsted酸的酸量和酸强度密切相关.为了进一步验证实际反应体系中反应条件对异丁烯胺化反应过程的影响规律,我们在ZSM-11催化剂上,系统考察了反应温度,压力,氨烯比和异丁烯空速对催化剂胺化反应性能的影响及变化规律.结果表明,在其他条件不变的情况下,异丁烯转化率随着温度的升高呈现出先增大后减小的趋势.适当提高原料中氨烯比和反应压力,以及采用较低异丁烯空速有利于促进异丁烯的转化.上述规律与热力学计算结果呈现出较好的一致性.在ZSM-11催化剂上,异丁烯直接胺化反应的较佳反应条件为523 K,5 MPa,氨烯比4,异丁烯空速0.5 h^(–1).上述结果可为异丁烯直接胺化合成叔丁胺过程新型高效催化剂的研发和反应工艺条件优化提供参考和指导. | 高尚耀 朱向学 李秀杰 王玉忠 张烨 谢素娟 安杰 陈福存 刘盛林 徐龙伢 | 2017 | Chinese Journal of Catalysis2017，38，1： | 2 |
| 8 | PtRe/H-ZSM-5的氢卤化对环己烯转化的影响(英文)显示文摘Extended use of supported Pt catalysts causes thermal migration of Pt particles to form large agglomerates,thus decreasing the catalytic activity.The combination of Pt with Re protects Pt against migration.In addition,Cl injection into the reactor assists Pt particles redispersion to prolong catalyst life.In this work,a PtRe/H-ZSM-5 catalyst was treated with either HCl or HF to investigate their role in activating or deactivating the catalyst.The conversion exceeded 90% in the whole temperature range with the PtRe/H-ZSM-5(HCl) catalyst,and its activity for the direct isomerization of cyclohexene to methylcyclopentenes(MCPEs) was the lowest but the activity for the hydrogenation of the MCPEs to methylcyclopentane was the highest.The reactivities of MCPEs and cyclohexadienes on the catalysts were similar because both are dehydrogenation reactions.Benzene production was significantly higher on the hydrochlorinated catalyst than on the other catalysts,and its hydrocracking activity was the lowest,which is a good characteristic for processing catalysts where cracking is undesired. | Sameh M.K.ABOUL-FOTOUH Noha A.K.ABOUL-GHEIT | 2012 | 催化学报2012，33，4： | 1 |
| 9 | Methanol conversion to DME as a blue fuel:The beneficial use of ultrasonic irradiation for the preparation of CuO/H-MOR nanocatalyst显示文摘Methanol conversion to DME was investigated over CuO /H-MOR nanocatalyst prepared by precipitation and /or by precipitation flowed by ultrasonic irradiation methods. BET,XRD,SEM,NH3-TPD and H2-TPR techniques were used to characterize nanocatalysts. The effective ultrasonication factors encountered during carrying out the dehydration of methanol on Cuo /H-MOR zeolite catalysts to produce dimethylether are studied in the present work. These factors include: the type of ultrasonication media,the ultrasonication time,and the fixed weight of the solid catalyst per the volume of the ultrasonication liquid media( Wcatalyst/ Vliquidratio). XRD showed that structure of H-MOR is not damaged even after it is loaded with CuO nanoparticles or with ultrasonication. H2-TPR profiles indicated that reducibility of sonicated CuO / H-MOR nanocatalyst is higher than non-sonicated catalyst. It is found that employing ultrasound energy for 60 min has the highest influence on the surface properties of nanocatalyst and its catalytic performance( activity and stability) of CuO / H-MOR catalyst. Surface morphology( SEM) of the sonicated CuO /H-MOR catalysts have clarified that methanol by itself used as an ultrasonication medium gives the best results concerning the homogeneity of particle sizes compared to the non-sonicated catalyst,where large agglomerates and non-homogeneous clusters appeared. Water used as a sonication medium showed many large agglomerates in addition to some smaller particles resulted in lowcatalytic activity. The different alcohols and( Wcatalyst/ Vliquid) ratio were examined to give precise correlation with the catalytic activity of the sonicated CuO / H-MOR zeolite catalyst. These findings certified that ultrasonication has a deep effect on the surface morphology and hence on the catalytic behavior of the dehydration of methanol to DME. NH3-TPD shows that ultrasound irradiation has enhanced the acidity of CuO / H-MOR catalyst and hence it's catalytic performance for DME formation. | Sameh M.K. Aboul-Fotouh | 2014 | 燃料化学学报2014，42，11： | 1 |
您所在的机构暂未开通此部分的功能，请联系管理员