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调控铝在ITH沸石骨架中的位置以用于催化甲醇制烯烃

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Chinese Journal of Catalysis 2024年第1期56卷 114-121页

作者：范凯吴勤明刘烁孔海宇王森 Eduard Kunkes Trees De Baerdemaeker Andrei-Nicolae parvulescu Nils Bottke Toshiyuki Yokoi Dirk E.De Vos 孟祥举张维萍肖丰收浙江省应用化学重点实验室浙江大学化学系中国浙江杭州310028 浙江大学化学与生物工程学院中国浙江杭州310028 大连理工大学精细化工国家重点实验室中国辽宁大连116012 中国科学院山西煤炭化学研究所煤转化国家重点实验室中国山西太原030001 巴斯夫股份有限公司德国东京工业大学资源化学研究所日本鲁汶大学表面化学与催化中心比利时

随着低碳烯烃需求量的增加,甲醇制烯烃(MTO)成为由非石油资源制取低碳烯烃的关键技术,其中沸石由于具有可调节的酸度、有序的微孔结构和较好的择型性能而被广泛用作MTO反应催化剂.ITQ-13沸石(ITH拓扑结构)由于其独特的九元环结构在MTO... 详细信息

随着低碳烯烃需求量的增加,甲醇制烯烃(MTO)成为由非石油资源制取低碳烯烃的关键技术,其中沸石由于具有可调节的酸度、有序的微孔结构和较好的择型性能而被广泛用作MTO反应催化剂.ITQ-13沸石(ITH拓扑结构)由于其独特的九元环结构在MTO反应中表现出较好的丙烯选择性和反应寿命,引起了广泛关注.研究表明,分子筛的酸中心分布与MTO反应性能密切相关,因此,研究ITQ-13沸石中铝分布与MTO反应性能的关系,对进一步提升其MTO催化性能具有重要意义.本文分别以与ITH具有共同基本结构单元(双四元环,D4Rs)的LTA沸石(LTA-ITH)和薄水铝石(C-ITH)为铝源,合成了两类铝硅酸盐ITH沸石.X射线衍射、扫描电子显微镜以及氮气吸脱附表征结果表明,这两类分子筛具有相似的片状形貌和微孔性质.氨气程序升温脱附结果表明,具有相近硅铝比的两类ITH沸石具有相近的酸量.进一步采用27Al魔角旋转核磁共振(MAS NMR)、密度泛函理论计算和1-己烯裂解反应对两类ITH分子筛的铝分布进行研究.结果表明,两类分子筛具有不同的铝分布,LTA-ITH中有更多的铝进入ITH的正弦孔道与直孔道,而C-ITH中有更多的铝分布在交叉孔道.当前,研究者普遍认为MTO反应过程遵循双循环烃池机理,ITH交叉孔道由于具有较大的空间,相比于正弦孔道和直孔道,更有利于芳烃循环中间体的产生,从而有利于形成芳烃循环产物(乙烯),而正弦孔道和直孔道却更有利于烯烃循环过程,导致产生更多的丙烯.对两类ITH进行了MTO催化性能测试,结果表明,LTA-ITH比C-ITH表现出更高的丙烯选择性,并且表现出更高的丙烯与乙烯的比率,表明其烯烃循环过程得到加强,这与^(27)Al MAS NMR以及1-己烯裂解反应得到的结论一致,进一步证明ITH分子筛的铝分布得到有效调控.综上,本文阐明了ITH沸石中铝分布与其反应性能的关系,为调整沸石骨架中的Al位点提供一种新策略,为未来制备高效的MTO沸石基催化剂提供参考.

关键词：骨架铝分布硅铝ITH分子筛甲醇制烯烃铝核磁

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利用择形分子筛异构化亚甲基二苯胺

Chinese Journal of Catalysis 2024年第7期62卷 124-130页

作者： Sam Van Minnebruggen Ka Yan Cheung Trees De Baerdemaeker Niels Van Velthoven Matthias Degelin Galahad O’Rourke Hiroto Toyoda Andree Iemhoff Imke Muller Andrei-Nicolae parvulescu Torsten Mattke Jens Ferbitz 吴勤明肖丰收 Toshiyuki Yokoi Nils Bottke Dirk De Vos 巴斯夫股份有限公司膜分离、吸附、催化和光谱学可持续解决方案中心(cMACS) 比利时巴斯夫股份有限公司研究组德国东京工业大学纳米空间催化研究所横滨日本浙江大学化学系浙江杭州310028

亚甲基二苯胺(MDA)被广泛用作生产聚氨酯和聚异氰脲酸酯的中间体.然而,当前MDA的生产工艺在控制(4,4’/(2,4’+2,2’))异构体比例方面还存在局限.其中,4,4’-MDA被认为是最有价值的异构体.尽管2,4'-MDA在市场上也有一定的需求,但如果能... 详细信息

亚甲基二苯胺(MDA)被广泛用作生产聚氨酯和聚异氰脲酸酯的中间体.然而,当前MDA的生产工艺在控制(4,4’/(2,4’+2,2’))异构体比例方面还存在局限.其中,4,4’-MDA被认为是最有价值的异构体.尽管2,4'-MDA在市场上也有一定的需求,但如果能将其有效地转化为4,4'-MDA,将能显著提升其附加值.本文在使用苯胺的条件下,利用β分子筛等催化剂,通过双分子机制,可以选择性地将2,4'-MDA异构化为4,4'-MDA.尽管实验显示,多种酸性沸石具有较高的异构化活性,但MCM-68(具有MSE拓扑结构)的催化性能尤为出色,它不仅展现出高异构化活性,而且具有很好的选择性.MCM-68主要催化2,4'-MDA异构化为4,4'-MDA,而2,2'-MDA和低聚物的形成则可以忽略不计.本文还深入探讨了该择形作用的原因,并详细研究了酸位置在MSE分子筛孔道限制中的关键作用.

关键词：铝分布多相催化异构化亚甲基二苯胺聚氨酯择形

Organosilane surfactant-assisted synthesis of mesoporous SSZ-39 zeolite with enhanced catalytic performance in the methanol-to-olefins reaction

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Frontiers of Chemical Science and Engineering 2020年第2期14卷 267-274页

作者： Hao Xu Chi Lei Qinming Wu Qiuyan Zhu Xiangju Meng Daniel Dai Stefan Maurer Andrei-Nicolae parvulescu Ulrich Muller Fengshou Xiao Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310028China BASF Catalysts(Shanghai)Co. Ltd.Shanghai 201206China BASF SE Ludwigshafen 67056Germany

SSZ-39 zeolite with AEI framework structure is a good catalyst candidate for the methanol-to-olefins(MTO)***,the diffusion limitation and coke formation often results in fast deactivation of the SSZ-39 zeolite *** solution for this challenge is to introduce mesoporosity in the SSZ-39 ***,we report the synthesis of mesoporous SSZ-39 zeolite using an organosilane surfactant,,-dimethyl--(3-(trimethoxysilyl)propyl)octan-1-aminium chloride,as a mesopore template and,-dimethyl--2,6-dimethylpiperidinium as a micropore *** obtained zeolites were characterized by X-ray diffraction,N sorption,scanning electron microscopy,temperature programmed desorption of ammonia,and magic angle spinning nuclear magnetic resonance of *** results show that the mesoporous SSZ-39 zeolite has high crystallinity,meso/microporosity,high surface area,cuboid morphology,and abundant acidic *** importantly,this mesoporous SSZ-39 zeolite exhibits enhanced catalyst lifetime in the MTO reaction due to the presence of mesoporosity for fast mass transfer,compared with a conventional SSZ-39 zeolite without mesoporosity.

关键词： SSZ-39 zeolite mesopores organosilane surfactant MTO reaction soft template mass transfer

Selective conversion of syngas to propane over ZnCrO_x-SSZ-39 OX-ZEO catalysts

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Journal of Energy Chemistry 2019年第9期28卷 141-147页

作者： Gen Li Feng Jiao Dengyun Miao Yong Wang Xiulian Pan Toshiyuki Yokoi Xiangju Meng Feng-Shou Xiao Andrei-Nicolae parvulescu Ulrich Müller Xinhe Bao State Key Laboratory of Catalysis National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023Liaoning China University of Chinese Academy of Sciences Beijing 100049 China Institute of Innovative Research Tokyo Institute of TechnologyYokohama 226-8503 Japan Department of Chemistry Zhejiang UniversityHangzhou 310028 Zhejiang China BASF SE Process Research and Chemical Engineering67056 Ludwigshafen Germany

Oxide-Zeolite(OX-ZEO) bifunctional catalyst design concept has been exemplified in several processes to direct conversion syngas to value-added chemicals and fuels such as mixed light olefins, ethylene, aromatics and *** we demonstrate that the product can be steered toward liquefied petroleum gas(LPG) with a selectivity up to 89% in hydrocarbons especially propane selectivity reaching 80% at CO conversion of 63% using ZnCrOx-H-SSZ-39 ***, the quantity of the acid sites of SSZ-39 does not influence obviously the hydrocarbon distribution but the strength is crucial for selective formation of *** finding provides an alternative route of LPG synthesis from a variety of carbon resources via syngas.

关键词： Syngas conversion Liquefied petroleum gas (LPG) Propane Zeolites SSZ-39 OX-ZEO Bifunctional catalysts

Meta-analysis of CO_(2) conversion,energy efficiency,and other performance data of plasma-catalysis reactors with the open access PIONEER database

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Journal of Energy Chemistry 2023年第11期86卷 318-342,I0007页

作者： Antoine Salden Maik Budde Carolina A.Garcia-Soto Omar Biondo Jairo Barauna Marzia Faedda Beatrice Musig ChloéFromentin Minh Nguyen-Quang Harry Philpott Golshid Hasrack Domenico Aceto Yuxiang Cai Federico Azzolina Jury Annemie Bogaerts Patrick Da Costa Richard Engeln María Elena Gálvez Timo Gans Tomas Garcia Vasco Guerra Carlos Henriques Monika Motak Maria Victoria Navarro Vasile I.parvulescu Gerard Van Rooij Bogdan Samojeden Ana Sobota Paolo Tosi Xin Tu Olivier Guaitella Department of Physics University of Trento38100 PovoItaly Department of Applied Physics and Science Education Eindhoven University of Technology5600 MB EindhovenThe Netherlands Instituto de Plasmas e Fusão Nuclear Instituto Superior TécnicoUniversidade de Lisboa1049-001 LisboaPortugal LPP CNRSÉcole PolytechniqueSorbonne UniversitéUniversitéParis-SaclayIP-Paris 91128 PalaiseauFrance Department of Organic Chemistry Biochemistry and CatalysisUniversity of BucharestBucharestRomania Research Group PLASMANT Department of ChemistryUniversity of AntwerpUniversiteitsplein 1Wilrijk B-2610Belgium DIFFER 5612AJ EindhovenThe Netherlands Instituto de Carboquímica ICB-CSIC Zaragoza 50018Spain Faculty of Energy and Fuels AGH University of KrakowKrakowPoland Institut Jean le Rond d’Alembert CNRS UMR 7190-Sorbonne UniversitéSaint-Cyr l’Ecole 78210France Laboratoire Catalyse et Spectrochimie(LCS) CNRS-ENSICAEN-Universitéde Caen6 boulevard du Maréchal-Juin14000 CaenFrance CQE Centro de Química EstruturalInstituto Superior TécnicoUniversidade de LisboaAv.Rovisco Pais1049-001 LisboaPortugal School of Physical Sciences and National Centre for Plasma Science and Technology Faculty of Science and HealthDublin City UniversityDublinIreland ASML De Run 65015504 DR VeldhovenThe Netherlands Faculty of Science and Engineering Maastricht University6229 GS MaastrichtThe Netherlands CNR Istituto per la Scienza e Tecnologia dei Plasmi(ISTP)Italy Department of Electrical Engineering and Electronics University of LiverpoolLiverpool L693GJUK

This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online *** tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by *** creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or *** a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different ***,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard *** however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social *** enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole *** database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a *** data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the *** the database itself,a data extraction tool with direct visualisation features or advance

关键词： Open-access database on plasma-catalysis experiment CO_(2) conversion Plasma-catalysis Carbon capture and utilisation(CCU) Energy efficiency Specific energy input Dielectric barrier discharge Packed bed reactor Methanation Dry reforming of methane

Accelerated infliximab infusions for inflammatory bowel disease improve effectiveness

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World Journal of Gastrointestinal Pharmacology and Therapeutics 2012年第5期3卷 74-82页

作者： John McConnell Simona parvulescu-Codrea Brian Behm Beth Hill Elizabeth Dunkle Karen Finke Kathryn Snyder Anne Tuskey Debbie Cox Beth Woodward Digestive Health Center of Excellence University of Virginia Medical CenterBrookline College

AIM:To study the safety and effectiveness associated with accelerated infliximab infusion protocols in patients with inflammatory bowel disease(IBD).METHODS:Original protocols and infusion rates were developed for the administration of infliximab over 90-min and *** the IBD patients on stable maintenance infliximab therapy were offered accelerated *** be eligible for the study,patients needed a minimum of four prior *** initial infusion of 90-min was given to each patient;those tolerating the accelerated infusion were transitioned to a 60-min infusion protocol at their next and all subsequent *** patient having significant infusion reactions would be reverted to the standard 120-min protocol.A change in a patient's dose mandated a single 120-min infusion before accelerated infusions could be administered ***:The University of Virginia Medical Center's Institutional Review Board approved this *** IBD patients treated with infliximab 5mg/kg,7.5mg/kg and 10mg/kg were offered accelerated ***-six patients consented to participate in the ***(41.3%) were female,five(10.9%) were African American and nine(19.6%) had ulcerative *** mean age was 42.6 years *** under age 18 were *** patients used immunosuppressive drugs concurrently out of which six were taking azathioprine,three were taking 6-mercaptopurine and one was taking *** of the 46 study patients used corticosteroid therapy for his *** of the patients used prophylactic medications prior to receiving infusions;six patients received corticosteroids as *** patients had a history of distant transfusion reactions to *** reactions included shortness of breath,chest tightness,flushing,pruritus and *** patients all took prophylactic medications before receiving infusions.46 patients(27 males and 19 females) received a total of fifty 90-min infusions and ninety-three

关键词： Infliximab Accelerated infusion Crohn’s disease Ulcerative colitis Obesity