Structure evolution of mesoporous silica supported copper catalyst for dimethyl oxalate hydrogenation

Zhao, Yujun; Zhang, Yaqing; Wang, Yue; Zhang, Jian; Xü, Yao; Wang, Shengping; Ma, Xinbin

doi:10.1016/j.apcata.2017.04.001

Cited by 80 publications

(43 citation statements)

References 33 publications

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“…The β‐CD template displayed strong characteristic peaks from 2 θ =5° to 45° (Figure A), which were not observed on the dried catalyst precursors. As clearly depicted in Figure B, all the samples exhibited a broad and diffuse peak at 22°, which was attributed to the feature peak of amorphous SiO 2 . In addition, only the dried Cu‐SiO 2 and 0.05CD‐Cu‐SiO 2 samples were composed of a strong phase of Cu 2 (OH) 3 NO 3 as evident from the clear reflection at 2 θ =12.8° and 25.8° (JCPDS 75‐1779), indicating the poor dispersion of copper species in Cu‐SiO 2 catalyst.…”

Section: Resultsmentioning

confidence: 84%

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Liu

et al. 2017

ChemCatChem

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The β‐cyclodextrin (β‐CD) was successfully applied to synthesize Cu‐SiO2 catalysts by the sol‐gel method. The first and most important question addressed was increasing the copper loading with higher dispersion in the silica support. Another task was to elucidate the structure–performance relationship. Furthermore, catalysts with various β‐CD doping levels were systematically characterized and employed in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The 0.1CD‐Cu‐SiO2 catalyst with 17.39 wt % copper showed 99.9 % DMO conversion and the highest EG selectivity of 95.0 % at 210 °C, as well a lifetime of over 240 h. The reaction results disclosed that the catalytic performance could be tuned facilely by changing the amount of β‐CD doping, which effectively influenced the Cu metallic surface area and dispersion.

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Section: Resultsmentioning

confidence: 84%

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Liu

et al. 2017

ChemCatChem

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“…In addition, there are many Cu/SiO 2 catalytic systems for which different kinds of SiO 2 sources are employed, and therefore, the selected reduction temperatures for activating Cu are not the same, such as silica sol (350 °C), TEOS (350 °C), aerosil (250 °C), and mesoporous silica (300 °C). This probably depends on the degree of interaction between the copper particles and the different kinds of silica.…”

Section: Resultsmentioning

confidence: 99%

“…Silica‐supported copper catalysts have excellent performance and have widely been used in hydrogenation reactions because of their excellent performance . SiO 2 , as a kind of carrier, has been used in the preparation of catalysts, such as silica sol, tetraethyl orthosilicate (TEOS), aerosil, and mesoporous silica . Various dopants have also been used to modify the catalysts .…”

Section: Introductionmentioning

confidence: 99%

Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Sun

Meng

et al. 2018

ChemistryOpen

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Exposing a Cu‐based catalyst to a suitable temperature is of great importance to optimize its hydrogenation performance, as copper is sensitive to temperature. Herein, we investigated the effect of the initial oxidation state of copper, tuned by the reduction temperature, on its catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) through designing a series of catalysts with different reduction temperatures (200–350 °C). Among these catalysts, the Cu/SiO2 catalyst prepared by ammonia evaporation with a hydrogen reduction process at 250 °C showed the best performance in the hydrogenation of DMO with a conversion of 100 % and a selectivity to EG higher than 95 %. The relationship between the initial oxidation state of copper and catalytic performance was well established by characterizing the physicochemical properties of the Cu/SiO2 catalysts by XRD, TEM, H2 temperature‐programmed reduction, N2O adsorption, and in situ reduction Auger electron spectroscopy. The initial oxidation state of copper determined the conversion of DMO and the distribution of the products, and it could be balanced by reducing the temperature to improve the activity of the catalyst. This work provides a reference for further exploration of the mechanism and guidance for the design of catalysts for the hydrogenation of esters.

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“…Structural diversity, compatibility with various transition metals, high surface area, and finely dispersed metallic cations makes phyllosilicates attractive in numerous reactions, such as Fischer-Tropsch [43], esterification [44], cellulose conversion to glucose [45], oxidation of water [46,47], oxidation of CO [48][49][50][51][52], CO or CO2 reforming [34,[53][54][55][56][57][58][59][60][61], hydrogen generation from methanol steam reforming [62][63][64][65][66], and syntheses of valuable alcohols from hydrogenation of CO [67][68][69], CO2 [53,[70][71][72], and hydrogenolysis of esters [73][74][75][76][77][78][79][80][81][82][83][84][85][86]...…”

Section: Introductionmentioning

confidence: 99%

Copper Phyllosilicates-Derived Catalysts in the Production of Alcohols from Hydrogenation of Carboxylates, Carboxylic Acids, Carbonates, Formyls, and CO2: A Review

Lin

2021

Catalysts

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Copper phyllosilicates-derived catalysts (CuPS-cats) have been intensively explored in the past two decades due to their promising activity in carbonyls hydrogenation. However, CuPS-cats have not been completely reviewed. This paper focuses on the aspects concerning CuPS-cats from synthesis methods, effects of preparation conditions, and dopant to catalytic applications of CuPS-cats. The applications of CuPS-cats include the hydrogenation of carboxylates, carboxylic acids, carbonates, formyls, and CO2 to their respective alcohols. Besides, important factors such as the Cu dispersion, Cu+ and Cu0 surface area, particles size, interaction between Cu and supports and dopants, morphologies, and spatial effect on catalytic performance of CuPS-cats are discussed. The deactivation and remedial actions to improve the stability of CuPS-cats are summarized. It ends up with the challenges and prospective by using this type of catalyst.

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Structure evolution of mesoporous silica supported copper catalyst for dimethyl oxalate hydrogenation

Cited by 80 publications

References 33 publications

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Copper Phyllosilicates-Derived Catalysts in the Production of Alcohols from Hydrogenation of Carboxylates, Carboxylic Acids, Carbonates, Formyls, and CO2: A Review

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Structure evolution of mesoporous silica supported copper catalyst for dimethyl oxalate hydrogenation

Cited by 80 publications

References 33 publications

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO2 Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO2 Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Importance of the Initial Oxidation State of Copper for the Catalytic Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

Copper Phyllosilicates-Derived Catalysts in the Production of Alcohols from Hydrogenation of Carboxylates, Carboxylic Acids, Carbonates, Formyls, and CO2: A Review

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One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

One‐Pot Synthesis of Cyclodextrin‐Doped Cu‐SiO₂ Catalysts for Efficient Hydrogenation of Dimethyl Oxalate to Ethylene Glycol