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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

realizing methanol synthesis from CO and water via the synergistic effect of Cu^(0)/Cu^(+)over Cu/ZrO_(2) catalyst

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Journal of energy Chemistry 2024年第6期93卷 126-134,I0004页

作者： Yuan fang fan Wang Yang Chen Qian Lv Kun Jiang Hua Yang Huibo Zhao Peng Wang Yuyan Gan Lizhi Wu Yu Tang Xinhua Gao Li Tan institute of Molecular Catalysis and In Situ/Operando Studies Fujian Key Laboratory of Electrochemical Energy Storage MaterialsState Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108FujianChina leibniz-institut für katalyse e.v.an der universität rostock Albert-Einstein Strasse 9118059 RostockGermany Department of Chemistry Tsinghua UniversityBeijing 100084China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021Ningxi1China

The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a ***,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic *** Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the ***,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic *** present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.

关键词： H_(2)O CO Methanol Cu-based catalysts t-ZrO_(2)

Palladium-catalyzed oxidative double alkoxycarbonylation of ethylene toward succinic acid derivatives

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Green Carbon 2024年第2期2卷 205-208页

作者： Zhi-Peng Bao Cunyao Li Li Yan Yunjie Ding Xiao-feng Wu Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning 116023China leibniz-institut für katalyse e.v. Rostock 18059Germany

employing biodegradable plastics is one of the choices to solve white pollution *** succinate(PBS),as a biodegradable plastic with good stability and heat resistance,is produced by polymerization of succinic acid and butylene ***,inadequate supply of the direct upstream material succinic acid restricts the development of this *** this work,we provide a carbonylative strategy to construct succinic acid derivatives from carbon monoxide(CO),ethylene and *** reaction catalyzed by palladium catalyst under oxidative conditions.

关键词： ethylene Alcohols Palladium Carbonylation Succinic acid derivatives

Generation and transformation ofα-oxy carbene intermediates enabled by copper-catalyzed carbonylation

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Green Carbon 2024年第1期2卷 70-80页

作者： Yang Yuan Xiao-feng Wu Dalian National Laboratory for Clean energy Dalian Institute of Chemical PhysicsChinese Academy of Sciences116023 DalianLiaoningChina leibniz-institut für katalyse e.v. Albert-Einstein-Straße 29a18059 RostockGermany

Since the fischer-Tropsch reaction was discovered by Otto roelen in 1938,transition metal-catalyzed carbo-nylation reactions come in as one of the most important methods for preparing carbonyl-containing and carbon chain-increased *** a result,the field of carbonylation research has rece.v.d considerable attention over the past decades and continues to *** the continuous development of carbonylation and the in-depth study of the mechanism,more mechanistic details and variations have been revealed,which provide more possibilities for organic ***,copper catalysis has been introduced to the carbonylative functio-nalization of alkenes,thus enabling the rapid assembly of functionalized carbonyl compounds from simple starting *** this Account,we summarize the new findings in the Cu-catalyzed borocarbonylation of alkenes based on the generation and transformation ofα-oxy carbene *** believe that the results presented in this Account will further inspire the design of new carbonylation reactions.

关键词： Carbonylation Copper catalyst Carbene Carbon monoxide Domino reaction

recent advances in intermediate-temperature CO_(2) capture: Materials,technologies and applications

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Journal of energy Chemistry 2024年第3期90卷 435-452,I0010页

作者： Chengbo Zhao Leiming Wang Liang Huang Nicholas M.Musyoka Tianshan Xue Jabor rabeah Qiang Wang engineering research Center for Water Pollution Source Control&eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China State Key Laboratory of efficient Production of forest resources Beijing Forestry UniversityBeijing 100083China China Machinery Huanyu Certification and Inspection Co. Ltd.Beijing 102609China Nottingham Ningbo China Beacons of excellence research and Innovation institute University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina institute of Atmospheric e.v.ronment Chinese Research Academy of Environmental SciencesBeijing 100012China leibniz-institut für katalyse e.v. Albert-Einstein-Str.29aRostock D-18059Germany

Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate *** various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification *** processes are crucial for achieving carbon *** laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial e.v.ronments remains challenging,impeding the commercialization *** review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application ***,we provide an ove.v.ew of laboratory-level advanced technologies specifically tailored for industrial ***,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale *** insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial *** promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.

关键词： Intermediate-temperature CO_(2) capture MgO LDHs Industrialization

Deciphering orbital hybridization in heterogeneous catalysis

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electron 2024年第1期2卷 68-94页

作者： Xiaoyang Yue Lei Cheng eszter Baráth rajenahally v.Jagadeesh Quanjun Xiang State Key Laboratory of electronic Thin film and Integrated Devices School of Electronic Science and EngineeringUniversity of Electronic Science and Technology of ChinaChengduChina'2Synergies in CatalysisCatalysis for Sustainable SynthesesLeibniz‐Institut für Katalyse e.V.RostockGermany'3Jiangsu Key Laboratory of New Power BatteriesJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjingChina

The catalytic coordinate is essentially the evolving frontier orbital interaction while feeding with catalytic materials and adsorbates under proper reaction *** heterogeneous catalytic reaction mechanism involves the initial adsorption and activation of reactants,subsequent intermediate transformation,final target product desorption,and regeneration of catalytic *** these catalytic processes,interaction modulations in terms of orbital hybridization/coupling allow an intrinsic control on both thermodynamics and *** charge transfer and redistribution,orbital splitting and rearrangement with specific orientation,and spin change and crossover pose a formidable challenge on mechanism elucidation;it is hard to precisely correlate the apparent activity and selectivity,let alone rational modulations on ***,deciphering the orbital couplings inside a catalytic round is highly desirable and the dependent descriptor further provides in-depth insights into catalyst design at the molecule orbital *** review hopes to provide a comprehensive understanding on orbital hybridizations,modulations,and correlated descriptors in heterogeneous catalysis.

关键词： catalysis catalyst design and prediction descriptors interactions orbital hybridization

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

High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

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Journal of energy Chemistry 2024年第1期88卷 552-560,I0012页

作者： Wenhao Cui Yuanshuai Liu Pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong fan Zhenghao Jia Haifeng Qi Wenhao Luo Peng Tian Zhongmin Liu National engineering research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina university of Chinese Academy of Sciences Beijing 100049China Qingdao institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina College of Chemistry and Chemical engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina State Key Laboratory of He.v. Oil Processing and Key Laboratory of Catalysis of CNPC China University of PetroleumBeijing 102249China Department of Inorganic Spectroscopy Max Planck Institute for Chemical Energy ConversionMülheim an der Ruhr 45470Germany Beijing Synchrotron radiation facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Division of energy research resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina leibniz-institut für katalyse Albert-Einstein-Straβe 29aRostock 18059Germany

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable ***,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant ***,we have constructed ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAr)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal *** with the benchmark ru/H-USY and other analogues,the as-prepared ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

关键词： High-silica zeolite Y Metal encapsulation Bifunctional catalysis Hydrodeoxygenation Biofuels

Impact of Chain Length of Saturated fatty Acids during Their Heterogeneously Catalyzed Deoxygenation

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Journal of Sustainable Bioenergy Systems 2014年第3期4卷 183-193页

作者： Shrikant Mohite Udo Armbruster Manfred richter Andreas Martin ArMACO Chemical Process Systems Mumbai India leibniz-institut für katalyse e.v. an der universität rostock Rostock Germany

fatty acids with different chain length were deoxygenated in the absence of hydrogen (caprylic acid (CA), lauric acid (LA) and stearic acid (SA)). The catalytic tests were carried over Pd-containing catalysts out in a batch reactor under inert gas for 6 h at 250°C to 350°C and pressures from 18 to 75 bar in the absence of additionally fed hydrogen. Pd-containing catalysts were tested;the best performing catalyst was 10% Pd/C with 63% undecane yield at 327°C. These catalysts were used for a comparative decarboxylation of CA, LA and SA. At equal reaction conditions (300°C, 6 h), the chain length of the fatty acid had a strong impact on the conversion, which was steadily increasing, whereas the alkane selectivity ran through a maximum. This work demonstrated the usability of Pd-containing catalysts for the decarboxylation of various fatty acids in the absence of additionally fed hydrogen with respect to the manufacture of hydrocarbons that can be used as blending components for fuels.

关键词： Deoxygenation Decarboxylation fatty Acids Long-Chain Alkanes Catalysts