Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol

Li, Fengjiao; Wang, Liguo; Han, Xiao; He, Peng; Cao, Yan; Li, Huiquan

doi:10.1039/c6ra06464g

Cited by 36 publications

(46 citation statements)

References 41 publications

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“…As reported in previous literatures for the analogous reaction, Cu/SiO 2 catalysts as a versatile hydrogenation catalyst showed an excellent application in the hydrogenation of dimethyl oxalate to EG or ethanol . In particular, heterogeneous copper‐based catalysts, e. g., CuCr 2 O 4 , Cu‐SiO 2 ‐PG, Cu/HMS, Cu/SBA‐15 and Cu/SiO 2 ‐AE were investigated for EC hydrogenation to co‐produce methanol and EG, and displayed relatively good catalytic performance. Among these catalysts tested, a maximum turnover frequency (TOF) of 776 mg EC g cat −1 h −1 was obtained over Cu/SBA‐15.…”

Section: Introductionmentioning

confidence: 69%

“…On account of the convenient catalyst recovery, much work was devoted to developing effective and easily recyclable heterogeneous catalysts for the chemoselective hydrogenation of EC. Because the unique property demonstrated in the selective hydrogenation of carbonyl bonds, copper‐based catalysts were studied extensively in the catalytic hydrogenation of ester for the synthesis of alcohols, thus ensuring the good selectivity of target products . As reported in previous literatures for the analogous reaction, Cu/SiO 2 catalysts as a versatile hydrogenation catalyst showed an excellent application in the hydrogenation of dimethyl oxalate to EG or ethanol .…”

Section: Introductionmentioning

confidence: 99%

“…As also proposed, the size of the copper particles is considered to be the crucial factor in hydrogenation reaction. Therefore, the protocol for the preparation of the copper‐based catalysts with finely tuned particles is of great significance ,. Recently, Yao et al reported a robust copper‐based catalysts with the introduction of low‐cost dextrin and employed it in the system of dimethyl oxalate hydrogenation successfully .…”

Section: Introductionmentioning

confidence: 99%

“…The catalytic activity and stability of the as‐prepared catalysts were enhanced greatly with the formation of dextrin‐coating. Meanwhile, the deactivation reason responsible for the stability was also highly concerned for giving insights into stabilizing mechanism ,,…”

Section: Introductionmentioning

confidence: 99%

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Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂

et al. 2018

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The hydrogenation of ethylene carbonate to co‐produce commodity methanol and ethylene glycol has attracted growing interests due to the potential chemical utilization of CO2 in large scale. In this work, we report a novel and facile protocol for the preparation of mesoporous Cu@SiO2 catalysts and successfully applied the as‐synthesized catalysts in the hydrogenation of ethylene carbonate. The catalysts were characterized in detail by means of N2 physisorption, N2O titration, XRD, FT‐IR, H2‐TPR, TEM and XPS (XAES). This strategy is an effective method for fabricating the unique flower‐like mesoporous Cu@SiO2 with sub‐2.0 nm ultrasmall Cu particles. The results revealed that the involvement of β‐cyclodextrin improved the Cu dispersion and facilitated exposing more copper active sites, which also indicated that the confined catalyst inhibiting the sintering of copper particles. Meanwhile, the stability of the attained catalyst was superior with the modification of carbon. Importantly, among the catalysts tested in the hydrogenation of ethylene carbonate, 25Cu@SiO2‐β‐P with appropriate copper loading as well as moderate Cu+ ratio exhibited superior catalytic performance. Accordingly, the synergistic effect between the Cu+ and metallic Cu0 species was crucial for obtaining better catalytic activity.

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Section: Introductionmentioning

confidence: 69%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂

et al. 2018

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“…[17][18][19] An alternative method to obtain supported catalysts with well-dened metal particles is the preparation of supported catalysts from metal colloids. 2,20,21 Many parameters determine their catalytic activity in hydrogenation process. The great advantage of the chemical method is that it could provide relatively monodispersed metal particles and minimize the effect of the support on the metallic active phase.…”

Section: Introductionmentioning

confidence: 99%

Benzene hydrogenation over alumina-supported nickel nanoparticles prepared by polyol method

2016

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A new catalyst composed of Ni nanoparticles supported on alumina for the hydrogenation of benzene was synthesized by the ethylene glycol reduction method, and characterized by XRD, TEM, EDX, H 2chemisorption, and H 2 -TPD. The catalytic performances of the obtained materials have been tested in the gas-phase hydrogenation of benzene. Metal particles with a size range 2-29 nm were obtained. The metal dispersion was found to be strongly influenced by the metal loading. It was found to decrease significantly with increasing Ni loading in the catalysts. The H 2 -TPD study showed that the Ni//Al 2 O 3 catalysts stored hydrogen with amounts changing with the nickel particle size. Further, the results show that the support may also actively participate in the hydrogen storage through the formation of Hspillover species. All catalysts have been found to be active and selective in the hydrogenation of benzene. The catalytic activity of these catalysts was dependent on the metal loading, particle size of the metal and the stored hydrogen in the catalyst. NiEG-05 catalyst was found to exhibit higher specific rate during the hydrogenation reaction than the other catalysts. This is attributed to the active nickel sites on the catalyst surfaces, which increase with the decrease of the metal loading.a Calculated from H 2 adsorption. b The average particle size was calculated from the XRD analysis.This journal is

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Highly dispersed Cu supported on mesoporous Al‐KIT‐6 for oxidative carbonylation of methanol to dimethyl carbonate

Yan

Zhao

et al. 2020

Applied Organom Chemis

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Microporous NaY zeolite is a common support of Cu catalysts for oxidative carbonylation of methanol, but the dispersion of Cu species on NaY is usually subjected to its micropore size. Here, ordered mesoporous KIT‐6 was employed as the support for Cu catalyst and Al was incorporated into its framework to increase the surface acidity, which eventually improves the surface exchange capacity and Cu dispersion. The evolution of the state of Cu species on KIT‐6 was analyzed combined with control of Cu loading. The physicochemical properties of the supports and corresponding catalysts were characterized by N2 adsorption–desorption, X‐ray diffraction, ammonia temperature programmed desorption, Fourier transform infrared spectra, transmission electron microscopy, hydrogen temperature programmed reduction, and X‐ray photoelectron spectroscopy. It was found that mesoporous KIT‐6 showed better Cu dispersion than microporous NaY zeolite. Agglomerated CuO, dispersed CuO, and Cu2+ are the major Cu species observed on the catalyst surface. The increased surface acidic sites of KIT‐6 by Al incorporation promoted the formation of Cu2+ and dispersion of CuO. With the increase in Cu loading, the Cu2+ content in the catalyst was decreased gradually along with increase in the bulk CuO. It was speculated that some exchanged Cu2+ could be transformed into highly dispersed CuO and even bulk CuO after calcination at a high Cu loading. Combined with the catalyst evaluation results, it was deduced that highly dispersed Cu2+ and CuO particles play significant roles in catalytic activity. The catalyst Cu/Al‐K‐10 achieved the highest space time yield of dimethyl carbonate of 135.4 mg/(g·h), which is 2.7 times the Cu/K‐10 owing to its more dispersed Cu species. This laid the basis for preparing highly dispersed Cu species on mesoporous silica supports.

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Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol

Abstract: Cu/SBA-15 was successfully prepared by ammonia evaporation method and exhibited a high activity for the hydrogenation of ethylene carbonate to co-produce ethylene glycol and methanol.

Cited by 36 publications

References 41 publications

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂

Benzene hydrogenation over alumina-supported nickel nanoparticles prepared by polyol method

Highly dispersed Cu supported on mesoporous Al‐KIT‐6 for oxidative carbonylation of methanol to dimethyl carbonate

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Influence of support on the performance of copper catalysts for the effective hydrogenation of ethylene carbonate to synthesize ethylene glycol and methanol

Abstract: Cu/SBA-15 was successfully prepared by ammonia evaporation method and exhibited a high activity for the hydrogenation of ethylene carbonate to co-produce ethylene glycol and methanol.

Cited by 36 publications

References 41 publications

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO2

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO2

Benzene hydrogenation over alumina-supported nickel nanoparticles prepared by polyol method

Highly dispersed Cu supported on mesoporous Al‐KIT‐6 for oxidative carbonylation of methanol to dimethyl carbonate

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Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂

Facile Fabrication of Ultrasmall Copper Species Confined in Mesoporous Silica for Chemo‐Selective and Stable Hydrogenation Ethylene Carbonate Derived from CO₂