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期刊论文 9

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Pd局域环境 1

乙炔半加氢 1

反应动力学 1

电子效应 1

载体效应 1

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Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 142-153 doi: 10.1007/s11705-015-1516-4

摘要： Recent advances with Pd containing catalysts for the selective hydrogenation of acetylene are described. The overview classifies enhancement of catalytic properties for monometallic and bimetallic Pd catalysts. Activity/selectivity of Pd catalysts can be modified by controlling particle shape/morphology or immobilisation on a support which interacts strongly with Pd particles. In both cases enhanced ethylene selectivity is generally associated with modifying ethylene adsorption strength and/or changes to hydride formation. Inorganic and organic selectivity modifiers (i.e., species adsorbed onto Pd particle surface) have also been shown to enhance ethylene selectivity. Inorganic modifiers such as TiO change Pd ensemble size and modify ethylene adsorption strength whereas organic modifiers such as diphenylsulfide are thought to create a surface template effect which favours acetylene adsorption with respect to ethylene. A number of metals and synthetic approaches have been explored to prepare Pd bimetallic catalysts. Examples where enhanced selectivity is observed are generally associated with decreased Pd ensemble size and/or hindering of the ease with which an unselective hydride phase is formed for Pd. A final class of bimetallic catalysts are discussed where Pd is not thought to be the primary reaction site but merely acts as a site where hydrogen dissociation and spillover occurs onto a second metal (Cu or Au) where the reaction takes place more selectively.

关键词： acetylene     ethylene     selective hydrogenation     palladium     bimetallic    

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Selective hydrogenation of acetylene over Pd/CeO

Kai Li, Tengteng Lyu, Junyi He, Ben W. L. Jang

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 929-936 doi: 10.1007/s11705-019-1912-2

摘要： Five hundred ppm Pd/CeO catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction. Pd/CeO catalyst could be activated by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction. Excellent ethylene selectivity of ~100% was obtained in the whole reaction temperature range of 50°C–200°C for samples calcined at temperatures of 600°C and 800°C. This could be ascribed to the formation of Pd Ce O or Pd-O-Ce surface species based on the X-ray diffraction and X-ray photoelectron spectroscopy results, indicating the strong interaction between palladium and ceria.

关键词： selective hydrogenation     acetylene     Pd/CeO2     strong interaction    

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Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1031-1059 doi: 10.1007/s11705-021-2113-3

摘要： Ethylene is an important feedstock for various industrial processes, particularly in the polymer industry. Unfortunately, during naphtha cracking to produce ethylene, there are instances of acetylene presence in the product stream, which poisons the Ziegler–Natta polymerization catalysts. Thus, appropriate process modification, optimization, and in particular, catalyst design are essential to ensure the production of highly pure ethylene that is suitable as a feedstock in polymerization reactions. Accordingly, carefully selected process parameters and the application of various catalyst systems have been optimized for this purpose. This review provides a holistic view of the recent reports on the selective hydrogenation of acetylene. Previously published reviews were limited to Pd catalysts. However, effective new metal and non-metal catalysts have been explored for selective acetylene hydrogenation. Updates on this recent progress and more comprehensive computational studies that are now available for the reaction are described herein. In addition to the favored Pd catalysts, other catalyst systems including mono, bimetallic, trimetallic, and ionic catalysts are presented. The specific role(s) that each process parameter plays to achieve high acetylene conversion and ethylene selectivity is discussed. Attempts have been made to elucidate the possible catalyst deactivation mechanisms involved in the reaction. Extensive reports suggest that acetylene adsorption occurs through an active single-site mechanism rather than via dual active sites. An increase in the reaction temperature affords high acetylene conversion and ethylene selectivity to obtain reactant streams free of ethylene. Conflicting findings to this trend have reported the presence of ethylene in the feed stream. This review will serve as a useful resource of condensed information for researchers in the field of acetylene-selective hydrogenation.

关键词： selectivity     hydrogenation     acetylene     ethylene     palladium    

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Efficient acetylene/carbon dioxide separation with excellent dynamic capacity and low regeneration energy

《化学科学与工程前沿（英文）》   页码 1616-1622 doi: 10.1007/s11705-022-2183-x

摘要： Adsorptive separation of acetylene/carbon dioxide mixtures by porous materials is an important and challenging task due to their similar sizes and physical properties. Here, remarkable acetylene/carbon dioxide separation featuring a high dynamic breakthrough capacity for acetylene (4.3 mmol·g–1) as well as an ultralow acetylene regeneration energy (29.5 kJ·mol–1) was achieved with the novel TiF62–-pillared material ZU-100 (TIFSIX-bpy-Ni). Construction of a pore structure with abundant TiF62– anion sites and pores with appropriate sizes enabled formation of acetylene clusters through hydrogen bonds and intermolecular interactions, which afforded a high acetylene capacity (8.3 mmol·g–1) and high acetylene/carbon dioxide uptake ratio (1.9) at 298 K and 1 bar. Moreover, the NbO52– anion-pillared material ZU-61 investigated for separation of acetylene/carbon dioxide. In addition, breakthrough experiments were also conducted to further confirm the excellent dynamic acetylene/carbon dioxide separation performance of ZU-100.

关键词： adsorption     acetylene/carbon dioxide separation     dynamic capacity     anion-pillared hybrid material    

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to ‘‘Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene Corrigendum

Yueqiang Cao, Xiaohu Ge, Yurou Li, Rui Si, Zhijun Sui, Jinghong Zhou, Xuezhi Duan, Xinggui Zhou

《工程（英文）》 2021年 第7卷 第5期   页码 701-701 doi: 10.1016/j.eng.2021.04.001

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Pd催化乙炔半加氢反应载体效应的结构根源和动力学分析 Article

曹约强, 葛小虎, 李雨柔, 司锐, 隋志军, 周静红, 段学志, 周兴贵

《工程（英文）》 2021年 第7卷 第1期   页码 103-110 doi: 10.1016/j.eng.2020.06.023

摘要：

本文从催化剂微结构和动力学角度，认识和理解碳纳米管和α-Al2O3负载Pd催化乙炔半加氢反应的载体效应。动力学分析、XPS、H2-TPR、TPHD和原位XRD研究结果表明：与α-Al2O3相比，碳纳米管作为载体降低了催化剂Pd0 3d的电子结合能且抑制了氢化钯物种的形成，从而显著提高了目标产物乙烯的收率。进一步结合XAS、HRTEM、C2H4-TPD和DFT计算，发现碳纳米管负载的催化剂中Pd纳米颗粒次表面存在碳原子，这种独特的局域环境能显著弱化目标产物乙烯的吸附，有利于乙炔半加氢反应的发生。这些研究结果预示着调变Pd催化剂的局域环境和电子性质是一种构筑乙炔半加氢Pd催化剂的有效策略。

关键词： 乙炔半加氢     反应动力学     载体效应     电子效应     Pd局域环境    

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Progress on cleaner production of vinyl chloride monomers over non-mercury catalysts

Jinli ZHANG, Nan LIU, Wei LI, Bin DAI

《化学科学与工程前沿（英文）》 2011年 第5卷 第4期   页码 514-520 doi: 10.1007/s11705-011-1114-z

摘要： Polyvinyl chloride (PVC) has become the third most used plastic after polyethylene and polypropylene and the worldwide demand continues to increase. Polyvinyl chloride is produced by polymerization of the vinyl chloride monomer (VCM), which is manufactured industrially via the dehydrochlorination of dichloroethane or the hydrochlorination of acetylene. Currently PVC production through the acetylene hydrochlorination method accounts for about 70% of the total PVC production capacity in China. However, the industrial production of VCM utilizes a mercuric chloride catalyst to promote the reaction of acetylene and hydrogen chloride. During the hydrochlorination, the highly toxic mercuric chloride tends to sublime, resulting in the deactivation of the catalyst and also in severe environmental pollution problems. Hence, for China, it is necessary to explore environmental friendly non-mercury catalysts for acetylene hydrochlorination as well as high efficiency novel reactors, with the aim of sustainable PVC production via the acetylene-based method. This paper presents a review of non-mercury heterogeneous and homogeneous catalysts as well as reactor designs, and recommends future work for developing cleaner processes to produce VCM over non-mercury catalysts with high activity and long stability.

关键词： polyvinyl chloride     vinyl chloride monomer     acetylene hydrochlorination     non-mercury catalysts     green chemical process    

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of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

《化学科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 442-449 doi: 10.1007/s11705-015-1547-x

摘要： Galvanic replacement, co-impregnation and sequential impregnation have been employed to prepare Pd-Cu bimetallic catalysts with less than 1 wt-% Cu and ca. 0.03 wt-% Pd for selective hydrogenation of acetylene in excess ethylene. High angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and H chemisorption results confirmed that Pd-Cu single-atom alloy structures were constructed in all three bimetallic catalysts. Catalytic tests indicated that when the conversion of acetylene was above 99%, the selectivity of ethylene of these three single atom alloy catalysts was still more than 73%. Furthermore, the single atom alloy catalyst prepared by sequential incipient wetness impregnation was found to have the best stability among the three procedures used.

关键词： H2 pulse chemisorption     palladium-copper bimetallic catalyst     single atom alloy     acetylene hydrogenation     HAADF-STEM    

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Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 522-533 doi: 10.1007/s11705-019-1822-3

摘要： A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu: Pd atomic ratios were prepared by conventionally sequential impregnation (CSI) and modified sequential impregnation (MSI) of Cu and Pd for selective hydrogenation of acetylene. Characterization indicates that the supported copper (II) nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO ) crystals. In addition, for the catalysts prepared by MSI, Pd atoms can form PdCu alloy on the surface of metal particles, however, for the catalysts prepared by CSI, Pd tends to migrate and exist below the surface layer of Cu. Reaction results indicate that compared with CSI, the MSI method enables samples to possess preferable stability as well as comparable reaction activity. This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles. Moreover, even Pd loading is super low,<0.045 wt-% in this study, by through adjusting Cu loading to an appropriate value, attractive reactivity and selectivity still can be achieved.

关键词： copper     palladium     catalysts     acetylene     selective hydrogenation    

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标题 作者 时间 类型 操作

Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

期刊论文

Selective hydrogenation of acetylene over Pd/CeO

Kai Li, Tengteng Lyu, Junyi He, Ben W. L. Jang

期刊论文

Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

期刊论文

Efficient acetylene/carbon dioxide separation with excellent dynamic capacity and low regeneration energy

期刊论文

to ‘‘Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

Yueqiang Cao, Xiaohu Ge, Yurou Li, Rui Si, Zhijun Sui, Jinghong Zhou, Xuezhi Duan, Xinggui Zhou

期刊论文

Pd催化乙炔半加氢反应载体效应的结构根源和动力学分析

曹约强, 葛小虎, 李雨柔, 司锐, 隋志军, 周静红, 段学志, 周兴贵

期刊论文

Progress on cleaner production of vinyl chloride monomers over non-mercury catalysts

Jinli ZHANG, Nan LIU, Wei LI, Bin DAI

期刊论文

of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

期刊论文

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

期刊论文