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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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Corrigendum to ‘‘Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenationof Acetylene” [Engineering 7 (2021) 103–110] 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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Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenationof 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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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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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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The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 397-407 doi: 10.1007/s11705-021-2076-4

摘要： The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass. Herein, a series of Ni-doped PtSn catalysts were prepared, characterized and studied in the hydrogenation of acetic acid. The Ni dopant has a strong interaction with Pt, which promotes the hydrogen adsorption, providing an activated hydrogen-rich environment for the hydrogenation. Meanwhile, the presence of Ni also improves the Pt dispersion, giving more accessible active sites for hydrogen activation. The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol. As a result, the catalyst with 0.1% Ni exhibits the best reaction activity, and its space time yield is twice as that of the PtSn/SiO2 catalyst. It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.

关键词： acetic acid     ethanol     hydrogenation     Pt     Ni     cooperation effect    

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NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要： Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO2 catalyst exhibited exceptional catalytic performance in converting NO to NH3, achieving an NO conversion rate exceeding 80% and an NH3 selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH3 desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词： NO hydrogenation     synthetic ammonia     10Fe-xCu/TiO2     high selectivity    

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HDS of dibenzothiophenes and hydrogenation of tetralin over a SiO

Qiang Wei, Jinwen Chen, Chaojie Song, Guangchun Li

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 336-348 doi: 10.1007/s11705-015-1535-1

摘要： A one-step synthesized Ni-Mo-S catalyst supported on SiO was prepared and used for hydrodesulphurization (HDS) of dibenzothiophene (DBT), and 4,6-dimethyl-dibenzothiophene (4,6-DMDBT), and for hydrogenation of tetralin. The catalyst showed relatively high HDS activity with complete conversion of DBT and 4,6-DMDBT at temperature of 280 °C and a constant pressure of 435 psi. The HDS conversions of DBT and 4,6-DMDBT increased with increasing temperature and pressure, and decreasing liquid hourly space velocity (LHSV). The HDS of DBT proceeded mostly through the direct desulphurization (DDS) pathway whereas that of 4,6-DMDBT occurred mainly through the hydrogenation-desulphurization (HYD) pathway. Although the catalyst showed up to 24% hydrogenation/dehydrogenation conversion of tetralin, it had low conversion and selectivity for ring opening and contraction due to the competitive adsorption of DBT and 4,6-DMDBT and insufficient acidic sites on the catalyst surface.

关键词： hydrodesulphurization (HDS)     hydrogenation     dibenzothiophene (DBT)     4     6-dimethyldibenzothiophene (4     6-DMDBT)     tetralin    

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modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 461-474 doi: 10.1007/s11705-021-2072-8

摘要： The catalytic hydrogenation of nitroaromatics is an environmentally friendly technology for aniline production, and it is crucial to develop noble-metal-free catalysts that can achieve chemoselective hydrogenation of nitroaromatics under mild reaction conditions. In this work, zinc-modified Ni-Ti catalysts (NixZnyTi1) were fabricated and applied for the hydrogenation of nitroaromatics hydrogenation. It was found that the introduction of zinc effectively increases the surface Ni density, enhances the electronic effect, and improves the interaction between Ni and TiO2, resulting in smaller Ni particle size, more oxygen vacancies, higher dispersion and greater concentration of Ni on the catalyst surface. Furthermore, the electron-rich Niδ– obtained by electron transfer from Zn and Ti to Ni effectively adsorbs and dissociates hydrogen. The results reveal that NixZnyTi1 (Ni0.5Zn0.5Ti1) shows excellent catalytic performance under mild conditions (70 °C and 6 bar). These findings provide a rational strategy for the development of highly active non-noble-metal hydrogenation catalysts.

关键词： bimetal strategy     oxygen vacancy     non-noble metal catalyst     hydrogenation     aromatic nitro compounds    

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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 950-962 doi: 10.1007/s11705-022-2162-2

摘要： A series of Cu–Ce–Zr catalysts with different Ce contents are applied to the hydrogenation of CO2 to CO/CH3OH products. The Cu–Ce–Zr catalyst with 2 wt% Ce loading shows higher CO selectivity (SCO = 0.0%–87.8%) from 200–300 °C, while the Cu–Ce–Zr catalyst with 8 wt% Ce loading presents higher CO2 conversion ( XCO2 = 5.4%–15.6%) and CH3OH selectivity ( SCH3OH = 97.8%–40.6%). The number of hydroxyl groups and solid solution nature play a significant role in changing the reaction pathway. The solid solution enhances the CO2 adsorption ability. At the CO2 adsorption step, a larger number of hydroxyl groups over the Cu–Ce–Zr catalyst with 8 wt% Ce loading leads to the production of H-containing adsorption species. At the CO2 hydrogenation step, a larger number of hydroxyl groups assists in encouraging the further hydrogenation of intermediate species to CH3OH and improving the hydrogenation rate. Hence, the Cu–Ce–Zr catalyst with 8 wt% Ce loading favors CH3OH selectivity and CO2 activation, while CO is preferred on the Cu–Ce–Zr catalyst with 2 wt% Ce loading, a smaller number of hydroxyl groups and a solid solution nature. Additionally, high-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy shows that CO is produced from formate decomposition and that both monodentate formate and bidentate formate are active intermediate species of CO2 hydrogenation to CH3OH.

关键词： CO2 hydrogenation     Cu–Ce–Zr     hydroxyls     CO/CH3OH selectivity    

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Utilization of waste vanadium-bearing resources in the preparation of rare-earth vanadate catalysts for semi-hydrogenation

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1793-1806 doi: 10.1007/s11705-022-2191-x

摘要： Recycling industrial solid waste not only saves resources but also eliminates environmental concerns of toxic threats. Herein, we proposed a new strategy for the utilization of petrochemical-derived carbon black waste, a waste vanadium-bearing resource (V > 30000 ppm (10 −6)). Chemical leaching was employed to extract metallic vanadium from the waste and the leachate containing V was used as an alternative raw material for the fabrication of vanadate nanomaterials. Through the screening of various metal cations, it was found that the contaminated Na+ during the leaching process showed strong competitive coordination with the vanadium ions. However, by adding foreign Ce3+ and Y3+ cations, two rare-earth vanadates, viz., flower-like CeVO4 and spherical YVO4 nanomaterials, were successfully synthesized. Characterization techniques such as scanning electron microscopy, transmission electron microscopy, X-ray diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared, and N2 physisorption were applied to analyze the physicochemical properties of the waste-derived nanomaterials. Importantly, we found that rare-earth vanadate catalysts exhibited good activities toward the semi-hydrogenation of α,β-unsaturated aldehydes. The conversion of cinnamaldehyde and cinnamic alcohol selectivity were even higher than those of the common CeVO4 prepared using pure chemicals (67.2% vs. 27.7% and 88.4% vs. 53.5%). Our work provides a valuable new reference for preparing vanadate catalysts by the use of abundant vanadium-bearing waste resources.

关键词： petrochemical solid wastes     vanadium recovery     resource utilization     nanomaterials     semi-hydrogenation    

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Catalytic hydrogenation of insoluble organic matter of CS/Acetone from coal over mesoporous HZSM-5 supported

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1505-1513 doi: 10.1007/s11705-022-2164-0

摘要： Four supported catalysts, nickel and ruthenium on a HZSM-5 support, were prepared by equal volume impregnation and in-situ decomposition of carbonyl nickel. The properties of catalysts were investigated by catalytic hydro-conversion of 2,2′-dinaphthyl ether as the model compound and extraction residue of Naomaohu lignite as the sample under an initial H2 pressure of 5 MPa and temperature at 150 °C. According to the catalytic hydro-conversion results of the model compound, Ni−Ru/HZSM-5 exhibited the best catalytic performance. It not only activated H2 into H···H, but also further heterolytically split H···H into immobile H‒ attached on the acidic centers of Ni−Ru/HZSM-5 and relatively mobile H+. Catalytic hydro-conversion of the extraction residue from Naomaohu lignite was further examined over the optimized catalyst, Ni−Ru/HZSM-5. Detailed molecular compositions of products from the extraction residue with and without hydrogenation were characterized by Fourier transform infrared spectroscopy and gas chromatography/mass spectrometry. The analytical results showed that the oxygen-containing functional groups in products of hydrogenated extraction residue were obviously reduced after the catalytic treatment. The relative content of oxygenates in the product with catalytic treatment was 18.57% lower than that in the product without catalytic treatment.

关键词： HZSM-5     Ni-based catalyst     catalytic hydrogenation     coal     model compound    

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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

Corrigendum to ‘‘Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenationof Acetylene” [Engineering 7 (2021) 103–110]

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

期刊论文

Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenationof 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

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

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

期刊论文

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

期刊论文

NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

期刊论文

HDS of dibenzothiophenes and hydrogenation of tetralin over a SiO

Qiang Wei, Jinwen Chen, Chaojie Song, Guangchun Li

期刊论文

modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation

期刊论文

An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

期刊论文

Utilization of waste vanadium-bearing resources in the preparation of rare-earth vanadate catalysts for semi-hydrogenation

期刊论文

Catalytic hydrogenation of insoluble organic matter of CS/Acetone from coal over mesoporous HZSM-5 supported

期刊论文