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dehydrogenation Based Asymmetric Epoxidation of Arylalkanes to Chiral Epoxides

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Chinese Journal of Chemistry 2022年第19期40卷 2263-2268页

作者： Yiting Su Feng Yu Guixia Liu Zheng Huang Chang-Kung Chuang Institute East China Normal UniversityShanghai200062 China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of Sciences345 Lingling RoadShanghai200032 China School of Chemistry and Material Sciences Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of Sciences1 Sub-lane XiangshanHangzhouZhejiang310024 China

We report herein a formal asymmetric epoxidation of arylalkanes enabled by a one-pot dual-catalysts system comprising a pincer Ir catalyst for alkane dehydrogenation-alkene isomerization(AD-ISO)and a chiral ketone catalyst for asymmetric alkene *** protocol provides a catalytic method for the synthesis of aryl epoxides in useful yields with high regio-and stereoselectivity directly from readily available alkyl *** derivatizations of the epoxidation product allow access to various enantioenriched compounds.

关键词： Alkanes Asymmetric epoxidation dehydrogenation Dual-catalysts Iridium

dehydrogenation of Propane to Propylene in the Presence of CO2 over Steaming-treated HZSM-5 Supported ZnO

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Chinese Journal of Chemistry 2012年第4期30卷 929-934页

作者：张帆缪长喜乐英红华伟明高滋 Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and lnnovative Materials Fudan UniversityShanghai 200433China Shanghai Research Institute of Petrochemical Technology Shanghai 201208China

dehydrogenation of propane to propylene over zinc oxide catalysts supported on steaming-treated HZSM-5 in the presence of CO2 has been investigated. The highest catalytic performance can be achieved on the 5%ZnO/HZSM-5（650） catalyst with the HZSM-5 support steaming at 650 ~C, which allows the maximum propyl- ene yields of 29.7% and 20.3% at the initial and steady states, respectively, in the catalytic dehydrogenation of pro- pane at 600 ~C. The superior catalytic performance of this catalyst can be attributed to high dispersion of ZnO and appropriate Bronsted acidity of the HZSM-5（650） support. The catalytic stability is enhanced by the addition of CO2 to the feed gas due to the suppression of coke formation.

关键词： dehydrogenation supported catalysts ZnO steaming-treated HZSM-5 stability

dehydrogenation AND AROMATIZATION OF CH4 IN THE ABSENCE OF O2 ON Mo/HZSM-5

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Chinese Journal of Catalysis 1996年第2期17卷 99-100页

作者： Liu Wei Xu Yide Liu Shetian Guo Xiexian (State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics,Chinese Academy of Sciences, Dalian 116023) State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023

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ＤＥＨＹＤＲＯＧＥＮＡＴＩＯＮＡＮＤＡＲＯＭＡＴＩＺＡＴＩＯＮＯＦＣＨ＿４ＩＮＴＨＥＡＢＳＥＮＣＥＯＦＯ＿２ＯＮＭｏ／ＨＺＳＭ－５￥ＬｉｕＷｅｉ；ＸｕＹｉｄｅ；ＬｉｕＳｈｅｔｉａｎ；ＧｕｏＸｉｅｘｉａｎ（ＳｔａｔｅＫｅｙＬａｂｏｒａｔｏｒｙｏｆＣａｔ...

关键词： methane dehydrogenation aromatization Mo/HZSM- 5

Enhanced catalytic activity of monodispersed AgPd alloy nanoparticles assembled on mesoporous graphitic carbon nitride for the hydrolytic dehydrogenation of ammonia borane under sunlight

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Nano Research 2017年第5期10卷 1627-1640页

作者： Hamza Kahri Melike Sevim Onder Metin Department of Chemistry Faculty of Science Ataturk University 25240 Erzurum Turkey Laboratoire de Synthese Organique Asymetrique et Catalyse Homogene (UR11ES56) Faculte des Sciences de Monastir Universite de Monastir Bd. de I'Environnement 5019 Monastir Tunisia East Anatolian High Technology Research and Application Center (DAYTAM) Ataturk University 25240 Erzurum Turkey

We address the composition-controlled synthesis of monodispersed AgPd alloy nanoparticles （NPs）, their assembly for the first time on mesoporous graphitic carbon nitride （mpg-C3N4）, and the unprecedented catalysis of mpg-CgN4@AgPd in the hydrolytic dehydrogenation of ammonia borane （AB） at room temperature. Monodispersed AgPd alloy NPs were synthesized using a high-temperature organic-phase surfactant-assisted protocol comprising the co-reduction of silver（I） acetate and palladium（II） acetylacetonate in the presence of oleylamine, oleic acid, and 1-0ctadecene. This protocol allowed the synthesis of four different compositions of AgPd alloy NPs. The AgPd alloy NPs were then assembled on mpg-C3N4, reduced graphene oxide, and Ketjenblack using a liquid-phase self-assembly method. Among the three supports tested, the mpg-CBN4@AgPd catalysts provided the best activity because of the Mott-Schottky effect, which was driven by the favorable work function difference between mpg-CBN4 and the metal NPs. Moreover, the activity of the mpg-CBN4@AgPd catalyst was further enhanced by an acetic acid treatment （AAt）, and a record initial turnover frequency of 94.1 mOl（hydrogen）＇mOl（catalyst）-l-min-1 was obtained. Furthermore, the mpg-CBN4@Ag42Pdss-AAt catalyst also showed moderate durability for the hydrolysis of AB. This study also includes a wealth of kinetic data for the mpg-CBN4@AgPd-catalyzed hydrolysis of AB.

关键词： silver palladium alloy nanoparticles graphitic carbon nitride ammonia borane dehydrogenation

Direct synthesis and dehydrogenation properties of NaAlH_4 catalyzed with ball-milled Ti–B

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Rare Metals 2017年第6期36卷 517-522页

作者： Li Li Zi-Chao Zhang Yi-Jing Wang Li-Fang Jiao Hua-Tang Yuan Laboratory of Inorganic Functional Materials School of Materials Science and Engineering University of Jinan Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Key Laboratory of Advanced Energy Materials Chemistry (MOE) College of University Nankai University

Ball-milled Ti-B-doped sodium aluminum hydride was directly synthesized via mechanical ball-milling of a NaH/Al mixture. The mixture was completely hydrogenated to NaAlH4 after 70 h under hydrogen pressure of 1 MPa. And higher hydrogen pressure is beneficial for the conversion from NaH/Al mixture to NaAlH4. The dehydrogenation properties of the as-synthesized Ti-Bdoped sodium aluminum were systematically *** result shows that ball-milled Ti-B has a remarkable catalytic effect on the enhanced dehydrogenation properties of NaAlH4. As-synthesized Ti-B-doped NaAlH_4 sample releases hydrogen at the temperature of about 100 ℃. Approximately 4.15 wt% H2 is released from ballmilled Ti-B-doped NaAlH_4 at 233.7 ℃. Even at 110 ℃, it also releases about 2.83 wt% hydrogen. The apparent activation energy（E_a） for the first step is estimated to be 83.97 k J·mol^-1 using Arrhenius equation. Thus, utilization of ball-milled Ti-B as catalyst would substantially enhance the practical applications of NaAlH_4 for hydrogen storage.

关键词： Hydrogen storage material NaAlH4 Ti-B dehydrogenation

One-step synthesis of Ni@Pd/NH_(2)-Fe_(3)O_(4)nanoparticles as affordable catalyst for formic acid dehydrogenation

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Chinese Journal of Chemical Engineering 2021年第4期34卷 168-174页

作者： Mohammad Reza Nabid Yasamin Bide Mahsa Jafari Department of Polymer&Material Chemistry Faculty of Chemistry&Petroleum ScienceShahid Beheshti UniversityTehran ***Iran

Currently,one of the critical issues in the world is finding an appropriate green alternative to fossil fuels due to the concerns about global *** a hydrogen source,formic acid has been given particular attention owing to the attractive features such as highenergy density,no toxicity,high stability at ambient temperature and high hydrogen *** an affordable and highly efficient catalyst with easy recovery from the reaction mixture for selective dehydrogenation of formic acid is still *** this report,we used a simple onestep process to synthesize Ni@Pd core shell nanoparticles on 3aminopropyltriethoxysilane modified Fe3O4 *** existence of Ni and Pd results in a synergic effect on the catalytic ***—NH2 groups play an important role for obtaining welldispersed ultrafine particles with high surface area and active *** addition,Fe3O4 lead to convenient magnetic recovery of the catalyst from reaction *** results indicate that the asprepared catalyst give the superb turnover frequency of 5367.8 h 1 with no additive,which is higher than most of the previously reported catalysts.

关键词： Core-shell Fe_(3)O_(4) Catalysis dehydrogenation Formic acid

Boron nitride for enhanced oxidative dehydrogenation of ethylbenzene

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Journal of Energy Chemistry 2021年第6期30卷 477-484,I0012页

作者： Rui Han Jiangyong Diao Sonu Kumar Andrey Lyalin Tetsuya Taketsugu Gilberto Casillas Christopher Richardson Feng Liu Chang Won Yoon Hongyang Liu Xudong Sun Zhenguo Huang Key Laboratory for Anisotropy and Texture of Materials(Ministry of Education) Northeastern UniversityShenyang 110819LiaoningChina School of Civil and Environmental Engineering University of Technology SydneyUltimoNew South Wales 2007Australia Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina Institute for Chemical Reaction Design and Discovery(WPI-ICReDD) Hokkaido UniversitySapporo 001-0021Japan Center for Green Research on Energy and Environmental Materials National Institute for Materials Science(NIMS)Tsukuba 305-0044Japan Department of Chemistry Faculty of ScienceHokkaido UniversitySapporo 060-0810Japan Electron Microscopy Centre University of WollongongNew South Wales 2500Australia Molecular Horizons and School of Chemistry and Molecular Bioscience Faculty of ScienceMedicine and HealthUniversity of WollongongNew South Wales 2522Australia Center for Hydrogen and Fuel Cell Research Korea Institute of Science and TechnologySeoul 02792Republic of Korea

It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of *** catalyst is derived from carbon-doped hexagonal boron nitride nanosheets synthesized via a two-step reaction when participating the oxidative dehydrogenation *** first step yields a polymeric precursor with the atomic positions of B,C,N relatively constrained,which is conducive for the formation of carbon atomic clusters uniformly dispersed throughout the BN *** the oxidative dehydrogenation of ethylbenzene to styrene,the nanoscale carbon clusters are removed and highly defective boron nitride(D-BN)is obtained,exposing boron-rich zigzag edges of BN that act as the catalytic *** catalytic performance of D-BN is therefore remarkably better than un-doped *** results indicate that dispersed C-doping in h-BN is highly effective in terms of defect formation and resultant enhanced activity in oxidative dehydrogenation reactions.

关键词： Boron nitride dehydrogenation Ethylbenzene Carbon-doping Heterogeneous catalysis

A self-catalytic role of methanol in PNP-Ru pincer complex catalysed dehydrogenation

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Science China Chemistry 2016年第6期59卷 724-729页

作者： Yuan-Ye Jiang Zheng-Yang Xu Hai-Zhu Yu Yao Fu Department of Chemistry and Center for Atomic Engineering of Advanced Materials Anhui University Hefei 230601 China Collaborative Innovation Center of Chemistry for Energy Materials CAS Key Laboratory of Urban Pollutant Conversion Department of Chemistry University of Science and Technology of China Hefei 230026 China

Extracting hydrogen from methanol is a safe and cost-efficient strategy for fuel supply. This process was realized recently at a mild condition with excellent efficiency by ruthenium pincer catalysts. Despite the experimental success, the associated mechanism remains under debate. With the aid of density functional theory(DFT) calculations, an updated and self-consistent mechanism which involves Me OH-catalysed dehydrogenation of ruthenium hydride intermediate and pre-protonation of the pincer ligand was present herein. This mechanism is kinetically favoured over the previously-proposed water- or formic- acid-participated ones and more consistent with the optimal experimental condition where strong base and neat methanol solvent are used.

关键词： dehydrogenation ruthenium pincer ligand methanol density functional theory

Research progress of CO_(2)oxidative dehydrogenation of propane to propylene over Cr-free metal catalysts

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Rare Metals 2022年第7期41卷 2129-2152页

作者： Zhong-Yu Wang Zhen-Hong He Long-Yao Li Shao-Yan Yang Meng-Xin He Yong-Chang Sun Kuan Wang Jian-Gang Chen Zhao-Tie Liu Shaanxi Key Laboratory of Chemical Additives for Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi’an 710021China School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an 710119China

CO_(2)-assisted oxidative dehydrogenation of propane(CO_(2)-ODHP)is an attractive strategy to offset the demand gap of propylene due to its potentiality of reducing CO_(2)emissions,especially under the demands of peaking CO_(2)emissions and carbon *** introduction of CO_(2)as a soft oxidant into the reaction not only averts the over-oxidation of products,but also maintains the high oxidation state of the redox-active ***,the presence of CO_(2)increases the conversion of propane by coupling the dehydrogenation of propane(DHP)with the reverse water gas reaction(RWGS)and inhibits the coking formation to prolong the lifetime of catalysts via the reverse Boudouard *** effective catalyst should selectively activate the C–H bond but suppress the C–C ***,to prepare such a catalyst remains ***-based catalysts are always applied in industrial application of DHP;however,their toxic properties are harmful to the *** this aspect,exploring environment-friendly and sustainable catalytic systems with Cr-free is an important *** this review,we outline the development of the CO_(2)-ODHP especially in the last ten years,including the structural information,catalytic performances,and mechanisms of chromium-free metal-based catalyst systems,and the role of CO_(2)in the *** also present perspectives for future progress in the CO_(2)-ODHP.

关键词： Propane dehydrogenation Propylene CO_(2) Chromium-free metals Catalytic performance