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

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 neutrality.The 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 sites.Furthermore,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 reaction.An effective catalyst should selectively activate the C–H bond but suppress the C–C cleavage.However,to prepare such a catalyst remains challenging.Chromium-based catalysts are always applied in industrial application of DHP;however,their toxic properties are harmful to the environment.In this aspect,exploring environment-friendly and sustainable catalytic systems with Cr-free is an important issue.In 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 reaction.We also present perspectives for future progress in the CO_(2)-ODHP.

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

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Two-dimensional atomically thin Pt layers on MXenes: The role of electronic effects during catalytic Dehydrogenation of ethane and propane

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Nano Research 2024年第3期17卷 1251-1258页

作者： Zhe Li Tobias K.Misicko Fan Yang Xiaopeng Liu Zhenwei Wu Xiaoyang Gao Tao Ma Jeffrey T.Miller Daniela S.Mainardi Collin D.Wick Zhenhua Zeng Yang Xiao Yue Wu Department of Chemical and Biological Engineering Iowa State University618 Bissell RoadAmesIA 50011USA Institute for Micromanufacturing Louisiana Tech University505 Tech DriveRustonLA 71272USA Davidson School of Chemical Engineering Purdue University480 Stadium Mall DriveWest LafayetteIN 47907USA Michigan Center for Materials Characterization University of Michigan2800 Plymouth RdAnn Arbor MI 48109USA College of Engineering and Science Louisiana Tech UniversityRustonLA 71272USA

Atomically thin Pt nanolayers were synthesized on the surface of Mo2TiC2 MXenes and used for the catalytic Dehydrogenation of ethane and propane into ethylene and propylene,two important chemicals for the petrochemical industry.As compared with Pt nanoparticles,the atomically thin Pt nanolayer catalyst showed superior coke-resistance(no deactivation for 24 h),high activity(turnover frequencies(TOFs)of 0.4–1.2 s^(-1)),and selectivity(>95%)toward ethylene and propylene.The unique Pt nanolayer has a similar geometric surface to Pt nanoparticles,enabling the investigations of the electronic effect on the catalytic performance,where the geometric effect is negligible.It is found that the electronic effect plays a critical role in dehydrogenative product selectivity and catalyst stability.The metal–support interaction is found dependent on the substrate and metal components,providing wide opportunities to explore high-performance MXene-supported metallic catalysts.

关键词： MXene catalysis alkane Dehydrogenation nanolayers

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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 epoxidation.This protocol provides a catalytic method for the synthesis of aryl epoxides in useful yields with high regio-and stereoselectivity directly from readily available alkyl arenes.Stereospecific derivatizations of the epoxidation product allow access to various enantioenriched compounds.

关键词： Alkanes Asymmetric epoxidation Dehydrogenation Dual-catalysts Iridium

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Y_(2)O_(3)-functionalized graphene-immobilized Ni–Pt nanoparticles for enhanced hydrous hydrazine and hydrazine borane Dehydrogenation

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Rare Metals 2023年第10期42卷 3410-3419页

作者： Qi-Lu Yao Meng He Ya-Ru Kong Tian Gui Zhang-Hui Lu State-Province Joint Engineering Laboratory of Zeolite Membrane Materials Institute of Advanced Materials(IAM)Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationKey Laboratory of Energy Catalysis and Conversion of NanchangJiangxi Normal UniversityNanchang330022China

Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hydrogen economy.In this work,ultrafine and well-dispersed bimetallic NiPt nanoparticles(3.4 nm) were successfully immobilized on Y_(2)O_(3)-functionalized graphene(Y_(2)O_(3)/rGO) without any surfactant by a simple liquid impregnation approach.It is firstly found that integration of graphene and Y_(2)O_(3) not only can facilitate the formation of ultrafine NiPt nanoparticles(NPs),but also can effectively modulate the electronic structure of NiPt NPs,thereby boosting the catalytic performance.Compared with NiPt/Y_(2)O_(3) and NiPt/rGO,the NiPt/Y_(2)O_(3)/rGO nanocomposites(NCs) show remarkable enhanced catalytic efficiency for hydrogen production from N_(2)H_(4)-H_(2)O.In particular,the optimized Ni_(0.6)Pt_(0.4/)Y_(2)O_(3)/rGO NCs display the best catalytic efficiency and 100% H_(2) selectivity for N_(2)H_(4)-H_(2)O Dehydrogenation,providing a turnover frequency(TOF) of2182 h^(-1) at 323 K,which is among the highest values ever reported.Moreover,the Ni_(0.6)Pt_(0.4)/Y_(2)O_(3)/rGO NCs also exhibit an excellent catalytic performance(TOF=3191 h^(-1)) and 100% H_(2) selectively for N_(2)H_(4)BH_(3)Dehydrogenation at 323 K.The outstanding catalytic results obtained provide more possibilities for the potential applications of N_(2)H_(4)·H_(2)O and N_(2)H_(4)BH_(3) as promising chemical hydrogen storage materials.

关键词： Hydrous hydrazine(N_(2)H_(4)·H_(2)O) Hydrazine borane(N_(2)H_(4)BH_(3)) Dehydrogenation Graphene Catalysis

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Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane Dehydrogenation

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Chinese Journal of Chemical Engineering 2022年第3期35卷 124-134页

作者： Di Gao Yibo Zhi Liyuan Cao Liang Zhao Jinsen Gao Chunming Xu Mingzhi Ma Pengfei Hao State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China Hebei Jingzhi Technology Company Limited Cangzhou 061000China

Rational design of Zn-containing HZSM-5 zeolite(Zn/HZSM-5)with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired.We develop a new and uncomplicated method to synthesize Zn/HZSM-5(IMX/Z5)with superior aromatization performance in the paper.Compared to incipient wetness impregnation(IMP/Z5)and mechanical mixing(MIX/Z5),the asprepared IMX/Z5 presents a higher amount of surface ZnOH^(+)species(2.87%)while keeping identical bulk zinc content.As a result,more surface ZnOH^(+)favor both the aromatization of 1-hexene and cyclohexane Dehydrogenation.For the two olefin aromatization pathways(hydrogen transfer and Dehydrogenation),it is the first time found both the hydrogen transfer ability and the Dehydrogenation ability increase linearly with the amount of surface ZnOH^(+)species while keeping identical bulk zinc content.We believe that the linear relationships are essential to design next generation olefin aromatization catalysts.

关键词： Zinc state Catalyst Catalysis Hydrogen transfer Dehydrogenation Moleclar sieves

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Ca2MnO4-layered perovskite modified by NaNO3 for chemical-looping oxidative Dehydrogenation of ethane to ethylene

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CHINESE JOURNAL OF CHEMICAL ENGINEERING 2024年第4期68卷 53-64页

作者： Ding, Weixiao Zhao, Kun Jiang, Shican Huang, Zhen He, Fang Guilin Univ Technol Coll Chem & Bioengn Guilin 541006 Peoples R China Chinese Acad Sci Guangzhou Inst Energy Convers Guangzhou 510640 Peoples R China Nanjing Univ Sci & Technol Sch Chem & Chem Engn Nanjing 210094 Peoples R China

Chemical-looping oxidative Dehydrogenation (CL-ODH) is a process designed for the conversion of alkanes into olefins through cyclic redox reactions, eliminating the need for gaseous O2. In this work, we investigated the use of Ca2MnO4-layered perovskites modified with NaNO3 dopants, serving as redox catalysts (also known as oxygen carriers), for the CL-ODH of ethane within a temperature range of 700 degrees C -780 degrees C. Our findings revealed that the incorporation of NaNO3 as a modifier significantly enhanced the selectivity for ethylene generation from Ca2MnO4. At 750 degrees C and a gas hourly space velocity of 1300 h-1, we achieved an ethane conversion up to 68.17%, accompanied by a corresponding ethylene yield of 57.39%. X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO3 onto Ca2MnO4 not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst. Furthermore, formation of NaNO3 shell on the surface of Ca2MnO4 led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner. This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO3-doped Ca2MnO4 catalyst. These findings provide compelling evidence for the potential of Ca2MnO4-layered perovskites as promising redox catalysts in the context of CL-ODH reactions. (c) 2024 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.

关键词： Chemical-looping oxidative Dehydrogenation Ethane Ethylene NaNO3-dopedCa2MnO4 redox catalyst Layered perovskites MIXED OXIDES PROCESS SIMULATIONS OXYGEN CARRIERS STEAM CRACKING CATALYSTS COMBUSTION REACTOR SURFACE SCHEME TIO2

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Rapid Access to Free Phenols by Photocatalytic Acceptorless Dehydrogenation of Cyclohexanones at Room Temperature

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Chinese Journal of Chemistry 2023年第21期41卷 2773-2778页

作者： Lin Min Jiani Lin Wei Shu Shenzhen Grubbs Institute Department of Chemistryand Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhenGuangdong518055 China

Phenols are ubiquitous substructures in natural products and bioactive compounds.However,practical methods for the direct construction of phenols under mild conditions remain challenging.Herein,a photocatalytic acceptorless hydrogen-evolution aromatization of cyclohexanones or cyclohexenones at room temperature has been developed.The reaction features the visible-light and cobalt co-catalyzed sequential Dehydrogenation of in-situ formed enol silyl ethers,which are regarded as a challenging process.This operationally simple method enables the synthesis of a series of phenols with diverse substitution patterns from cyclohexanones or cyclohexenones.Moreover,diverse substituted 1,2-,1,3-,and 1,4-benzenediols were obtained from cyclohexanediones,providing a general and straightforward method for the synthesis of phenols from simple starting materials under mild conditions.

关键词： Phenols Photocatalysis Dehydrogenation Cyclohexanones Cobalt catalysis Radicals

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Insights into carbon-based materials for catalytic Dehydrogenation of low-carbon alkanes and ethylbenzene

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Frontiers of Chemical Science and Engineering 2023年第11期17卷 1623-1648页

作者： Sijia Xing Sixiang Zhai Lei Chen Huabin Yang Zhong-Yong Yuan School of Materials Science and Engineering Smart Sensing Interdisciplinary Science CenterNankai UniversityTianjin 300350China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

Direct Dehydrogenation with high selectivity and oxidative Dehydrogenation with low thermal limit has been regarded as promising methods to solve the increasing demands of light olefins and styrene.Metalbased catalysts have shown remarkable performance for these reactions,such as Pt,CrOx,Co,ZrOx,Zn and V.Compared with metal-based catalysts,carbon materials with stable structure,rich pore texture and large surface area,are ideal platforms as the catalysts and the supports for Dehydrogenation reactions.In this review,carbon materials applied in direct Dehydrogenation and oxidative Dehydrogenation reactions including ordered mesoporous carbon,carbon nanodiamond,carbon nanotubes,graphene and activated carbon,are summarized.A general introduction to the Dehydrogenation mechanism and active sites of carbon catalysts is briefly presented to provide a deep understanding of the carbon-based materials used in Dehydrogenation reactions.The unique structure of each carbon material is presented,and the diversified synthesis methods of carbon catalysts are clarified.The approaches for promoting the catalytic activity of carbon catalysts are elaborated with respect to preparation method optimization,suitable structure design and heteroatom doping.The regeneration mechanism of carbon-based catalysts is discussed for providing guidance on catalytic performance enhancement.In addition,carbon materials as the support of metal-based catalysts contribute to exploiting the excellent catalytic performance of catalysts due to superior structural characteristics.In the end,the challenges in current research and strategies for future improvements are proposed.

关键词： carbon materials Dehydrogenation active sites mechanism catalytic performance support

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Core-shell Cu@SiO_(2)/SiO_(2) catalyst for 1,6-hexanediol Dehydrogenation toε-caprolactone:High activity and stability from core-shell nanostructure

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Nano Research 2023年第10期16卷 12270-12280页

作者： Fengyang Jiang Tian Lan Jiaqiang Sun Guofeng Zhao Yong Lu Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China

The gas-phase Dehydrogenation of 1,6-hexanediol(1,6-HDO)toε-caprolactone(ε-CL)over the high-performance Cu-based catalysts is highly desirable,but with grand challenges,because the Cu nanoparticles(NPs)are easy to be sintered with the low Hüttig temperature(250℃ of reaction temperature).Herein,we report a highly efficient silica-encapsulated nano-Cu catalyst(Cu@SiO_(2)/SiO_(2))prepared via a complexation–impregnation method for the Dehydrogenation of 1,6-HDO,exhibiting a 1,6-HDO conversion of 95.3%andε-CL selectivity of 80.0%at 270℃.The catalyst also has the outstanding thermal stability(without sintering up to 270℃ for 100 h on stream),which can be attributed to the effective encapsulation of the SiO_(2)shell.In addition,the reaction network of 1,6-HDO Dehydrogenation is proved.Finally,the pyridine-diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and in-situ X-ray photoelectron spectroscopy(XPS)reveal that the Cu^(0) species favor the conversion of 1,6-HDO toε-CL.The synergistic effect of Cu+and Cu^(0) benefits the conversion ofε-CL to 2-methylcyclopentanone(2-MCPN).This study is beneficial for designing the high-performance Cu-based catalysts for 1,6-HDO toε-CL,understanding the reaction network of 1,6-HDO Dehydrogenation over the Cu-based catalysts,and offering a strong foundation for the largescale production ofε-CL.

关键词： core–shell nanostructure Cu-based catalyst 1 6-hexanediol Dehydrogenation ε-caprolactone

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An efficient single atom catalysts Os/P_(3)C sheet for ammonia borane Dehydrogenation

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Chinese Chemical Letters 2022年第6期33卷 3281-3286页

作者： Chaozheng He Quan Zhang Jinrong Huo Ling Fu Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringInstitute of Environment and Energy CatalysisXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

Ammonia borane(NH_(3)BH_(3),AB)has been considered to be a promising chemical hydrogen storage material.Based on density functional theory,a series of transition metal atoms supported P_(3)C(P_(3)C_O)sheet is systematically investigated to screen out the most promising catalyst for Dehydrogenation of AB.The results indicate that the Os/P_(3)C and Os/P_(3)C_O could be an efficient single atom catalyst(SACs)and the stepwise reaction pathway with free energy barrier of 2.07 and 1.54 e V respectively.Remarkably,the rate constant further quantitatively confirmed the real situation of the first step of Dehydrogenation of AB on the Os/P_(3)C and Os/P_(3)C_O substrates.We found that k_(f1)at 400 K is equivalent to k_(f2)at 800 K,which greatly improves the temperature of the first step of AB Dehydrogenation on P_(3)C_O.We hope this work can provide a promising method for the design of catalysts for AB Dehydrogenation reactions on the surface of two-dimensional materials(2D).

关键词： Ammonia borane Two-dimensional materials Dehydrogenation Single atom catalyst Microkinetic model

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