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| 1 | 双功能TiSn-Beta分子筛限域的串联Lewis酸催化烯烃生成1,2-二醇显示文摘1,2-二醇主要由环氧化合物水合产生、广泛用于防冻剂,聚酯树脂和医药等化学品中间体的生产.研究表明,具有Lewis酸性的含锡沸石分子筛在环氧化物的水合反应中表现出优异的催化性能.环氧化合物是众所周知的碳亲电体之一,主要由烯烃环氧化生成.含Ti(Ⅳ)沸石,如Ti-Beta和TS-1,是烯烃环氧化反应的高效催化剂.串联催化可以将多步反应整合为一次反应,无需分离中间体,有效缩短合成路线,提高生产效率.因此,双功能Ti和Sn分子筛有望应用于烯烃制二醇的串联催化反应中,即烯烃在Ti活性位点上发生环氧化反应,随后在Sn位点上发生水合反应,进而串联一步生成1,2-二醇.在沸石分子筛中产生孤立的多功能活性位点是将多步反应整合成串联催化反应的一种有吸引力的设计策略.本文通过简单且可规模制备的后合成路线构建了双功能TiSn-Beta分子筛,并用于烯烃串联催化制1,2-二醇反应.一方面,该反应中的过氧化氢溶液既能提供氧化剂(如H2O2)用于烯烃环氧化反应,又能提供环氧化合物水合反应的亲核试剂(如H2O);同时TiSn-Beta作为一种高效双功能催化剂,孤立的Ti和Sn活性中心可以有效地将烯烃环氧化反应和环氧化物水合反应串联在沸石微反应器中,实现烯烃一步转化为1,2-二醇.另一方面,沸石的限域效应较好地保证了烯烃环氧化和环氧化物水合的高串联速率和目标产物的高选择性,在最优的反应条件下,1,2-二醇选择性高达90%以上,收率接近70%.本文结果表明沸石分子筛是构筑多功能孤立活性位点的理想载体,为其他串联反应催化剂的设计提供了良好的借鉴. | 雷琦锋 王畅 戴卫理 武光军 关乃佳 Michael Hunger 李兰冬 | 2021 | Chinese Journal of Catalysis2021，42，7： | 4 |
| 2 | Ce-Beta分子筛的制备及其催化性能(英文)显示文摘采用简单、易重现的两步后合成法成功制备了Ce-Beta分子筛.制备过程中,H-Beta分子筛首先经过脱铝处理得到Si-Beta分子筛,然后再以异丙醇铈为前驱体,通过干法浸渍的途径向Si-Beta分子筛引入Ce(IV).利用XRD,FT-IR,UV-Vis和1H MAS NMR等对其结构进行了表征,结果表明,Ce(IV)物种以四配位的形式成功引入Beta分子筛的骨架,Ce原子进入分子筛骨架的机理通过DRIFT光谱得以证实.通过环氧化合物水合制备1,2-二醇反应对所制的Ce-Beta催化剂进行了催化性能评价. | 唐波 戴卫理 孙晓明 武光军 李兰冬 关乃佳 Michael Hunger | 2015 | 催化学报2015，36，6： | 3 |
| 3 | High population and dispersion of pentacoordinated Al~Ⅴ species on the surface of ?ame-made amorphous silica-alumina显示文摘Pentacoordinated Al(Al~Ⅴ)species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts.However,pentahedral coordination(Al~Ⅴ)is rarely observed in conventionally prepared silica-alumina.Here,we show that high population and dispersion of Al~Ⅴ species on the surface of amorphous silica-alumina(ASA)can be achieved by means of flame spray pyrolysis.High resolution TEM/EDX,high magnetic-field NMR and DFT calculations are employed to characterize the structure of as-prepared ASAs.Solid-state ^(27)Al multi-quantum MAS NMR experiments show that most of the Al~Ⅴspecies are formed independently from the alumina phase and are accessible for guest molecules on the surface.Upon water adsorption,these Al~Ⅴ species are transformed to Al~Ⅵ species,structurally similar to surface Al~Ⅳ species,as confirmed by DFT calculations.The outstanding catalytic activity of as-synthesized ASA is demonstrated using the in situ H/D exchange reaction with deuterated benzene as an example.The Al~Ⅴ-rich ASA provides a much lower activation energy(~30 kJ/mol)than that reported for zeolite H-ZSM-5(~60 kJ/mol).The superior catalytic performance is attributed to the high Al~Ⅴcontent promoting the surface active sites in ASA.The knowledge gained on the synthesis of Al~Ⅴ-rich ASAs and the nature of aluminum coordination in these materials could pave the way to more efficient silica-alumina based catalysts. | Zichun Wang Yijiao Jiang Xianfeng Yi Cuifeng Zhou Aditya Rawal James Hook Zongwen Liu Feng Deng Anmin Zheng Michael Hunger Alfons Baiker Jun Huang | 2019 | Science Bulletin2019，64，8： | 2 |
| 4 | Mechanistic investigations of the methanol-to-olefin (MTO) process on acidic zeolite catalysts by in situ solid-state NMR spectroscopy 显示文摘 | Wang Wei Jiao Yi Michael Hunger | 2006 | Catalysis Today2006，113，12： | 1 |
| 5 | Mechanistic Inves- tigations of the Methanol-to-Olefin(MTO) Process on Acidic Zeolite Catalysts by in-Situ Solid-State NMR Spectroscopy 显示文摘 | Wang Wei Jiang Yijiao Michael Hunger | 2006 | CatalToday2006，113，12： | 1 |
| 6 | Biomechanical Evaluation of Subtalar Fusion: Influence of Screw Configuration and Placement显示文摘 | Sven Hungerer Sebastian Eberle Susanne Lochner Michael Maier Rainer Penzkofer Peter Augat | 2013 | The Journal of Foot and Ankle Surgery2013，，： | 1 |
| 7 | Formation of cyclic compounds and carbenium ions by conversionof methanol on weakly dealuminated zeolite H-ZSM-5 investigated via a novel in situ CF MASNMR/UV-Vis technique显示文摘 | Michael Hunger Wang Wei | 2004 | Chem Commun2004，，： | 1 |
| 8 | In situ solid-state NMR investigations of the vapor-phase Beckmann rearrangement of 15 N-cyclohexanone oxime on MFI-type zeolites and mesoporous SBA-15 materials in the absence and presence of the additive 13 C-methanol显示文摘 | V.R. Reddy Marthala Sandra Rabl Jun Huang Sayed A.S. Rezai Bejoy Thomas Michael Hunger | 2008 | Journal of Catalysis2008，，1： | 1 |
| 9 | Methanol‐to‐Olefin Conversion Catalyzed by Low‐Silica AlPO‐34 with Traces of Br?nsted Acid Sites: Combined Catalytic and Spectroscopic Investigations显示文摘 | Weili Dai Xin Wang Guanjun Wu Landong Li Naijia Guan Michael Hunger | 2012 | ChemCatChem2012，，9： | 1 |
| 10 | Zeolite HNU-87: synthesis, characterization and catalytic properties in the shape-selective conversion of methylnaphthalenes显示文摘 | Roger Gl?ser Ruifeng Li Michael Hunger Stefan Ernst Jens Weitkamp | 1998 | Catalysis Letters (-)1998，，3： | 1 |
| 11 | Muhinuclear MAS NMR and IR spectroscopic study of silicon incorporation into SAPO-5, SAPO-31, and SAPO-34 molecular sieves 显示文摘 | Bodo Zibrowius Elke Loffler Michael Hunger | 1992 | Zeolites1992，12，2： | 1 |
| 12 | Reactivity of surface alkoxy species on acidic zeohte eata|ysts显示文摘 | Wang Wei Hunger Michael | 2008 | Accounts of Chemica| Research2008，41，8： | 1 |
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