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radical Carbonylation under Low CO Pressure:Synthesis of esters from Activated Alkylamines at Transition Metal-free Conditions

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Chinese Journal of Chemistry 2021年第4期39卷 927-932页

作者： fengqian Zhao Han-Jun Ai Xiao-feng Wu leibniz-institut fur katalyse e.v.an der universitat rostock Albert-Einstein-Straße 29a18059 RostockGermany Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China

Main observation and conclusion High CO pressure(>40 bar)is usually needed in radical carbonylation reactions in the absence of metal *** this communication,we developed a transition-metal-free radical carbonylation of activated alkylamines with phenols and alcohols under low CO pressure(1-6 bar).various esters were obtained in moderate to excellent yields under simple reaction conditions with good functional group compatibility.

关键词： Carbonylation radical ester Alkylamine Katritzky salt

过渡金属催化的羰基化的杂环化合成和官能团化（英文）

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有机化学 2019年第3期39卷 573-590页

作者：尹志平王泽超吴小锋 leibniz-institut für katalyse e.v. an der Universit?t rostock

杂环化合物广泛的存在于天然产物、药物、有机材料以及其他官能团化的分子中.所以发展杂环合成的新的方法学有着极其重要的意义.在所有的有机合成策略中,过渡金属催化的反应,由于其相对温和的反应条件和高效的原子利用率,无疑是一种理... 详细信息

杂环化合物广泛的存在于天然产物、药物、有机材料以及其他官能团化的分子中.所以发展杂环合成的新的方法学有着极其重要的意义.在所有的有机合成策略中,过渡金属催化的反应,由于其相对温和的反应条件和高效的原子利用率,无疑是一种理想的选择.这其中,过渡金属催化的羰基化反应又是一个比较理想的反应.自从20世纪30年代首度报道以来,羰基化反应经历了长足的发展.时至今日,各种羰基化反应类型都得到发展.反应底物也囊括了卤代芳烃、烯烃、炔烃及其它未经活化的化合物.羰基来源也从一氧化碳气体拓展到了其他原位释放一氧化碳的化合物,例如甲酸、醇、醛、生物质等.对我们课题组在过去5年中在过渡金属催化的羰基化合成杂环及杂环的官能团化领域的工作进行了总结.使用铜、钯、铑、钌和铱作为催化剂,基于碳卤键和碳氢键的活化,各种杂环化合物都能被高效的合成.

关键词：过渡金属催化羰基化杂环合成羰基来源环化反应多米诺反应

Industrially applied and relevant transformations of 1,3-butadiene using homogeneous catalysts

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Industrial Chemistry & Materials

Industrial Chemistry & Materials 2023年第2期1卷 155-174页

作者： Ji Yang Peng Wang Helfried Neumann ralf Jackstell Matthias Beller leibniz-institut für katalyse an der Universität rostock Albert-Einstein-Straße 29a18059 RostockGermany

In recent decades,the use of 1,3-butadiene as a comparably cheap and abundant raw material for new applications has attracted more and more interest,specifically in the chemical *** present review covers several of the most important homogeneously catalyzed processes and technologies which are currently used or have the potential to produce fine and bulk chemicals from 1,*** an example,palladium-catalyzed telomerizations provide valuable chemicals through the selective dimerization of 1,3-dienes with the simultaneous addition of various nucleophiles,which can be used for the synthesis of 1-octene,1-octanol,and various *** the other hand,direct carbonylation allows the selective introduction of functional groups onto 1,3-dienes,such as carbonyl,carboxyl or ester *** key to success in achieving these industrially relevant conversions of 1,3-butadiene was mainly the development of innovative efficient *** hope this review will make readers familiar with the industrially applied and relevant transformations of 1,3-butadiene and inspire them to further explore new and advanced systems.

关键词： 1,3-Butadiene Industrial chemistry Carbonylation reaction Bulk chemicals Telomerization.

Copper-Catalyzed Carbonylative Synthesis of β-Boryl Amides via Boroamidation of Alkenes

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CCS Chemistry 2021年第4期3卷 2643-2654页

作者： fu-Peng Wu Jens Holz Yang Yuan Xiao-feng Wu leibniz-institut für katalyse e.v.an der Universität rostock Rostock 18059 Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023

β-Boryl amide is a class of high value intermediates in organic *** this work,a copper-catalyzed carbonylative boroamidation of olefins toward the synthesize ofβ-boryl amides has been *** new chemical bonds were constructed in this transformation.A wide range ofβ-boryl amides were produced in excellent regioselectivity and good to excellent *** gas can be successfully transformed under the same standard conditions as ***,with the use of a chiral ligand,the first example of enantioselective carbonylative boroamidation of alkenes was *** addition,Piposulfan and Pipobroman,antineoplastic medicines,were prepared by this methodology in a straightforward manner.

关键词： carbonylative boroamidation copper catalyst enantioselective olefins

Co-aromatization of methane and hexane over Pt encapsulated in ZSM-5 zeolite and the electronic effect of K promoters

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Science China Chemistry 2024年第3期67卷 1017-1027页

作者： Bei Liu fan Wang Xiaomeng Dou Pengfei Li Hongwei Xiang Yong Yang Peng He State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Department of Chemistry Tsinghua UniversityBeijing 100084China National energy r&D Center for Coal to Liquid fuels Synfuels China Technology Co.Ltd.Beijing 101407China University of Chinese Academy of Sciences Beijing 101408China leibniz-institut für katalyse e.v.an der universitat rostock Rostock 18059Germany

The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MfI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MfI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMr studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.

关键词： Pt encapsulation MfI zeolite methane activation co-aromatization ^(13)C solid-state NMr

Understanding the mechanisms of hydrogenation and transfer hydrogenation by using pincer-type catalysts–insights from computation

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Understanding the mechanisms of hydrogenation and transfer h...

C–f bond activation under transition-metal-free conditions

中国化学会第十二届全国物理有机化学学术会议

作者： Zhihong Wei Kathrin Junge Haijun Jiao leibniz-institut für katalyse e.v.an der Universit?t rostock

＜正＞In this contribution we will present computational investigations into the structures and stability of the pincer-type complexes of different transition metals（fe,ru,Os,Mn,Ir,Os,Cr,Mo and W）as well as their catalytic activity in hydrogenation and transfer hydrogenation of nitriles,esters,ketones and *** between theory and experiments reveals

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来源： cnki会议评论

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Science China Chemistry 2021年第10期64卷 1630-1659页

作者： Han-Jun Ai Xingxing Ma Qiuling Song Xiao-feng Wu leibniz-institut fur katalyse e.v.an der universitat rostock Rostock 18059Germany Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Key Laboratory of Molecule Synthesis and function Discovery Fujian Province UniversityCollege of ChemistryFuzhou UniversityFuzhou 350108China institute of Next Generation Matter Transformation College of Material Sciences&EngineeringHuaqiao UniversityXiamen 361021China

The unique properties of fluorine-containing organic compounds make fluorine substitution attractive for the development of pharmaceuticals and various specialty materials,which have inspired the evolution of diverse C–f bond activation *** many advances have been made in functionalizations of activated C–f bonds utilizing transition metal complexes,there are fewer approaches available for nonactivated C–f bonds due to the difficulty in oxidative addition of transition metals to the inert C–f *** this regard,using Lewis acid to abstract the fluoride and light/radical initiator to generate the radical intermediate have emerged as powerful tools for activating those inert C–f ***,these transition-metal-free processes are greener,economical,and for the pharmaceutical industry,without heavy metal *** review provides an overview of recent C–f bond activations and functionalizations under transition-metal-free *** key mechanisms involved are demonstrated and discussed in ***,a brief discussion on the existing limitations of this field and our perspective are presented.

关键词： transition-metal-free fluorinated compounds C–f activation coupling

Synthesis of quinazolinones from o-aminobenzamides and benzyl amines under metal-free conditions

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Chinese Chemical Letters 2016年第1期27卷 21-24页

作者： Xin-Xin Qi Zhen-Zhen Song Jin-Long Gong Zheng-Yu fang Xiao-feng Wu Department of Chemistry Zhejiang Sci-Tech University Xiasha Campus Hangzhou 310018 China Department of Anal-colorectal Surgery the First Affiliated Hospital of Zhejiang Chinese Medical University Hangzhou 310006 China leibniz-institut für katalyse e.v. an der Universit t rostock 18059 Rostock Germany

A convenient and transition-metal free protocol for quinazolinones synthesis with o-aminobenzamides and benzyl amines as substrates has been developed. Using H;O;as the oxidant, various quinazolinones were obtained in... 详细信息

关键词： Quinazolinones Metal-free Benzyl amine H2O2

A New Type of Strong Metal-Support Interaction Caused by Antimony Species

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Open Journal of Metal 2020年第2期10卷 17-33页

作者： A. Benhmid K. el Ttaib K. edbey v. N. Kalevaru B. Lücke Chemistry Department Benghazi University Benghazi Libya leibniz institute für katalyse e.v. an der universitat rostock Rostock Germany

Interactions between metals and supports are of fundamental interest in heterogeneous catalysis, Noble metal particles supported on transition metal oxides (TMO) may undergo a so-called strong metal-support interaction via encapsulation. This perspective addresses catalytic properties of the metal catalysts in the SMSI state which can be explained on the basis of complementary studies. The electronic geometric and bifunctional effects originating from strong metal-support interactions (SMSI) that are responsible for the catalyst’s activity, selectivity, and stability are key factors that determine performance. A series of Pd-Sb supported on different metal oxide (em>i.e.em> SiO2, em>γem>-Al2O3, TiO2, and ZrO2) were prepared by the impregnation method. The catalysts were characterized by N2 adsorption (BeT-SA and pore size distribution), TeM (transmission electron microscope), TPr (temperature-programmed reduction), CO-chemisorption, the structural characterization of Pd (dispersity, surface area), interaction between Pd and Sb2O3 and also the influence of the nature of the support were investigated. SiO2 supported Pd catalyst exhibited the highest surface area (192.6 m2/g) and pore volume (0.542 cm3/g) compared to the other supported oxides catalysts. The electron micrographs of these catalysts showed a narrow size particle distribution of Pd, but with varying sizes which in the range from 1 to 10 nm, depending on the type of support used. The results show almost completely suppressed of CO chemisorption when the catalysts were subjected to high temperature reduction (HTr), this suppression was overcome by oxidation of a reduced Pd/MeOx catalysts followed by re-reduction in hydrogen at 453 K low temperature reduction (LTr), almost completely restored the normal chemisorptive properties of the catalysts, this suppression was attributed by SbO

关键词： BeT-SA and Pore Size Distribution TeM SMSI effect Metal Oxide Supports TPr CO-Chemisorption SbOx Species