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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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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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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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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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A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a Pd

Enxian Yuan, Xiangwei Ren, Li Wang, Wentao Zhao

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 177-184 doi: 10.1007/s11705-016-1604-0

摘要： The hydrogenation of 2-ethylanthraquinone (eAQ), 2- -amylanthraquinone (taAQ) and their mixtures with molar ratios of 1:1 and 1:2 to the corresponding hydroquinones (eAQH and taAQH ) were studied over a Pd/Al O catalyst in a semi-batch slurry reactor at 60 °C and at 0.3 MPa. Compared to eAQ, TaAQ exhibited a significantly slower hydrogenation rate (about half) but had a higher maximum yield of H O and a smaller amount of degradation products. This can be ascribed to the longer and branched side chain in taAQ, which limits its accessibility to the Pd surface and its diffusion through the pores of the catalyst. Density functional theory calculations showed that it is more difficult for taAQ to adsorb onto a Pd (111) surface than for eAQ. The hydrogenation of the eAQ/taAQ mixtures had the slowest rates, lowest H O yields and the highest amounts of degradation products.

关键词： hydrogenation     hydrogen peroxide     anthraquinone     Pd catalyst     AO process    

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Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1311-1319 doi: 10.1007/s11705-022-2281-9

摘要： A reconstructed Cu–ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol. According to the characterization results of the fresh Cu–ZnO and reconstructed Cu–ZnO, three different forms of ZnO were suggested to be presented on the catalysts: ZnO having strong interaction with Cu species, ZnO that weakly interacted with Cu species and isolated ZnO. The first form of ZnO was believed to be beneficial to the formation of efficient active site Cu+, while the latter two forms of ZnO took the main responsibility for the deactivation of Cu–ZnO catalysts in the liquid-phase hydrogenation of diesters. The reconstruction of the Cu–ZnO catalyst by the organic acid treatment method resulted in a new Cu–ZnO catalyst with more Cu+ and less ZnO species that leads to deactivation. Furthermore, the deactivation mechanism of Cu–ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed: the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the deactivation. These results provided meaningful instructions for designing highly efficient Cu–Zn catalysts for similar ester hydrogenation systems.

关键词： liquid phase     hydrogenation     Cu–ZnO     deactivation mechanism     1     4-butanediol     diester    

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Boehmite-supported CuO as a catalyst for catalytic transfer hydrogenation of 5-hydroxymethylfurfural

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 415-424 doi: 10.1007/s11705-022-2225-4

摘要： 2,5-bis(hydroxymethyl)furan (BHMF) is an important monomer of polyester. Its oxygen-containing rigid ring structure and symmetrical diol functional group establish it as an alternative to petroleum-based monomer with unique advantages for the prodution of the degradable bio-based polyester materials. Herein, we prepared a boehmite-supported copper-oxide catalyst for the selective hydrogenation of 5-hydroxymethylfurfural into BHMF via catalytic transfer hydrogenation (CTH). Further, ethanol successfully replaced conventional high-pressure hydrogen as the hydrogen donor, with up to 96.9% BHMF selectivity achieved under suitable conditions. Through characterization and factor investigations, it was noted that CuO is crucial for high BHMF selectivity. Furthermore, kinetic studies revealed a higher by-product activation energy compared to that of BHMF, which explained the influence of reaction temperature on product distribution. To establish the catalyst structure-activity correlation, a possible mechanism was proposed. The copper-oxide catalyst deactivated following CTH because ethanol reduced the CuO, which consequently decreased the active sites. Finally, calcination of the catalyst in air recovered its activity. These results will have a positive impact on hydrogenation processes in the biomass industry.

关键词： biomass     5-hydroxymethylfurfural     2     5-bis(hydroxymethyl)furan     transfer hydrogenation     catalysis    

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Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation to

《能源前沿（英文）》 2022年 第16卷 第5期   页码 697-699 doi: 10.1007/s11708-022-0843-7

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Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1807-1817 doi: 10.1007/s11705-022-2243-2

摘要： The Ru/C catalyst prepared by impregnation method was used for hydrogenation of 3,5-dimethylpyridine in a trickle bed reactor. Under the same reduction conditions (300 °C in H2), the catalytic activity of the non-in-situ reduced Ru/C-n catalyst was higher than that of the in-situ reduced Ru/C-y catalyst. Therefore, an in-situ H2 reduction and moderate oxidation method was developed to increase the catalyst activity. Moreover, the influence of oxidation temperature on the developed method was investigated. The catalysts were characterized by Brunauer–Emmett–Teller method, hydrogen temperature programmed reduction H2-TPR, hydrogen temperature-programmed dispersion (H2-TPD), X-ray diffraction, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, O2 chemisorption and oxygen temperature-programmed dispersion (O2-TPD) analyses. The results showed that there existed an optimal Ru/RuOx ratio for the catalyst, and the highest 3,5-dimethylpyridine conversion was obtained for the Ru/C-i1 catalyst prepared by in-situ H2 reduction and moderate oxidation (oxidized at 100 °C). Excessive oxidation (200 °C) resulted in a significant decrease in the Ru/RuOx ratio of the in-situ H2 reduction and moderate oxidized Ru/C-i2 catalyst, the interaction between RuOx species and the support changed, and the hard-to-reduce RuOx species was formed, leading to a significant decrease in catalyst activity. The developed in-situ H2 reduction and moderate oxidation method eliminated the step of the non-in-situ reduction of catalyst outside the trickle bed reactor.

关键词： Ru/C catalyst     in-situ H2 reduction and moderate oxidation     in-situ reduction     non-in-situ reduction     hydrogenation of 3     5-dimethylpyridine    

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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H2), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes     room-temperature hydrogenation     Ni nanoparticles     nitrogen-doped carbon nanoneedles     metal–organic-framework    

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标题 作者 时间 类型 操作

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

Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

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

Selective hydrogenation of acetylene over Pd/CeO

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

期刊论文

A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a Pd

Enxian Yuan, Xiangwei Ren, Li Wang, Wentao Zhao

期刊论文

Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

期刊论文

Boehmite-supported CuO as a catalyst for catalytic transfer hydrogenation of 5-hydroxymethylfurfural

期刊论文

Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation to

期刊论文

Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in

期刊论文

Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

期刊论文