Excellent performance in hydrogenation of esters over Cu/ZrO<sub>2</sub> catalyst prepared by bio-derived salicylic acid

Ding, Jian; Liu, Yanting; Zhang, Juan; Liu, Kefeng; Xiao, Haicheng; Kong, Fangfang; Sun, Yanan; Chen, Jiangang

doi:10.1039/c6cy00715e

Cited by 23 publications

(18 citation statements)

References 43 publications

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“…The surface compositions of copper species and silica were calculated from XPS and XAES spectra, as shown in Table 4. The content of surface copper species of 14 Cu-AS-AC and Cu-AM-AC were 11.6% and 10.8%, respectively, lower than those tested by ICP-AES. However, the content of copper species on the surface of Cu-AS-AE was 27.8%, higher than the one tested by ICP-AES.…”

Section: Surface Compositionsmentioning

confidence: 65%

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Ding

Popa

Tang

et al. 2017

Applied Catalysis B: Environmental

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Dimethyl Oxalate (DMO) hydrogenation for ethylene glycol (EG) production is problematic due to environmental concerns and safety regulations. Therefore, development of improved methods for diethyl oxalate (DEO) hydrogenation based EG production is desirable. The objective of this research was to develop a cost-effective © 2017. This manuscript version is made available under the Elsevier user license http://www.elsevier.com/open-access/userlicense/1.0/ 2 and environmentally benign approach for the synthesis of highly active and stable Cu/SiO 2 catalysts for selective hydrogenation of diethyl oxalate (DEO) to ethylene glycol (EG). Here, ammonium carbonate is used to prepare Cu/SiO 2 catalysts through deposition precipitation instead of the conventional pollution-producing evaporation process associated with the use of ammonia. The Cu/SiO 2 catalysts prepared with the new method achieved 6.9-13.1% higher selectivity and showed better stability. The improved stability and selectivity resulted from increased chemical adsorption of DEO and H 2 due to the high Cu 2 O concertation and Cu + /(Cu 0 +Cu + ) ratio (reduced from ion-exchanged Cu-O-Si units), and reduced carbon deposition on the Cu/SiO 2 catalyst. The Cu 2 O reduced from Cu-O-Si units in the Cu/SiO 2 catalyst prepared bythe new method was more stable than the Cu + species reduced from copper phyllosilicate in the Cu/SiO 2 catalyst prepared by the conventional method. Therefore, the new Cu/SiO 2 catalyst preparation method appears most promising.

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Section: Surface Compositionsmentioning

confidence: 65%

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Ding

Popa

Tang

et al. 2017

Applied Catalysis B: Environmental

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“…The stability of a Cu based catalyst can also be improved by choosing suitable support materials. In addition to Al 2 O 3 and carbon nanotubes, other metal oxides such as ZrO 2 and MgO have been used to support Cu NPs for the DMO-to-EtOH reaction. , For example, a Cu/ZrO 2 catalyst was fabricated with carboxylic acids as complex agents (Figure ). The obtained catalyst exhibited high metal dispersion with small Cu NPs and strong metal–support interactions, as well as abundant surface acidic/basic sites.…”

Section: Recent Progress In Catalyst Design For Dmo Hydrogenationmentioning

confidence: 99%

“…In addition to Al 2 O 3 and carbon nanotubes, other metal oxides such as ZrO 2 and MgO have been used to support Cu NPs for the DMO-to-EtOH reaction. , For example, a Cu/ZrO 2 catalyst was fabricated with carboxylic acids as complex agents (Figure ). The obtained catalyst exhibited high metal dispersion with small Cu NPs and strong metal–support interactions, as well as abundant surface acidic/basic sites. With the Cu/ZrO 2 catalyst, an ethanol yield of 92% at 270 °C was obtained over 144 h. It is highlighted that the electronic effect derived from an organic complex agent could enhance the resistance of Cu NPs to agglomeration .…”

Section: Recent Progress In Catalyst Design For Dmo Hydrogenationmentioning

confidence: 99%

“… The obtained catalyst exhibited high metal dispersion with small Cu NPs and strong metal–support interactions, as well as abundant surface acidic/basic sites. With the Cu/ZrO 2 catalyst, an ethanol yield of 92% at 270 °C was obtained over 144 h. It is highlighted that the electronic effect derived from an organic complex agent could enhance the resistance of Cu NPs to agglomeration . Cu catalysts could also be stabilized by doping a second element such as boron or cerium.…”

Section: Recent Progress In Catalyst Design For Dmo Hydrogenationmentioning

confidence: 99%

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Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate

Wang

et al. 2020

ACS Catal.

100

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What should people do with the huge amount of CO 2 captured? CO 2 to CO is a promising way for using carbon resources because CO is one component of syngas for the production of many important synthesis intermediates such as dimethyl oxalate (DMO). Hydrogenation of DMO provides an economical and eco-friendly approach for the synthesis of methyl glycolate, ethylene glycol (EG), and ethanol, which is often determined by the reaction conditions and catalysts with different active sites. Thus, DMO or EG is also an important carbon carrier or CO 2 utilization product. Also, DMO hydrogenation is a representative reaction for studying the structure−activity relationship in CO/C−O bond hydrogenation. Therefore, this work provides a comprehensive review of the progress in DMO hydrogenation from the perspective of constructing and stabilizing the active sites. The silver and copper based catalysts with different structures and morphologies used for DMO hydrogenation have been discussed with regard to their catalytic performance and reaction mechanism. The synergy of Cu 0 and Cu + in DMO hydrogenation has been questioned, and new active sites are proposed with more experimental evidence. New reaction routes, hybrid active sites, and the effect of catalyst structure on the active sites for DMO hydrogenation have been achieved and reviewed. Moreover, a strategy of introducing organic additives to improve EG yield and stabilize copper species has been described. This work may help advance the understanding of active sites in DMO hydrogenation and guide the future rational design and fabrication of highly stable and low-cost DMO hydrogenation catalysts.

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“…One centered at 917.5 eV that is ascribed to Cu 0 , and a second one at lower kinetic energy that ascribed to Cu + . [26,[48][49][50] It points out that even for low Cu content, some of the copper is reduced. However, for the samples having high Cu content only one peak centered at 917.5 eV is detected.…”

Section: Characterization Of the First Generation Of Catalystsmentioning

confidence: 99%

CuOx/CeO2 catalyst derived from metal organic framework for reverse water-gas shift reaction

Ronda‐Lloret

Rico-Francés

Sepúlveda-Escribano

et al. 2018

Applied Catalysis A: General

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Highlights  An alternative route using a MOF as catalyst precursor has been studied  The MOF called Cu-BTC has been used as precursor  The MOF was impregnated with cerium precursor  The impregnated MOF was pyrolyzed to obtain the catalyst  With the pyrolysis method we could control the final properties of the catalysts ABSTRACT: Herein, we have studied an alternative route for preparing CuOx/CeO2 catalysts using metal organic frameworks (MOFs) as precursors. Usually, CuOx/CeO2 materials are prepared by wet impregnation of ceria support. In this study, we have impregnated a Cu-MOF with a ceria precursor and then pyrolized the impregnated MOF using different conditions and procedures. The prepared catalysts have been characterized by using a wide range of techniques such as XRD, XPS, Raman, and TPR. We have found that the pyrolysis method determines the dispersion of the oxidized copper species on the ceria surface what, in turn, controls the catalytic activity and selectivity of the catalysts in the reverse water-gas shift (RWGS) reaction. We have compared the behavior of the MOF-derived

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Excellent performance in hydrogenation of esters over Cu/ZrO₂ catalyst prepared by bio-derived salicylic acid

Abstract: A variety of bio-derived organic carboxylic acids are used to prepare Cu/ZrO2. In particular, salicylic acid provides superb control over the distribution of small Cu particles on t-ZrO2, which affords enhanced catalytic activity.

Cited by 23 publications

References 43 publications

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate

CuOx/CeO2 catalyst derived from metal organic framework for reverse water-gas shift reaction

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Excellent performance in hydrogenation of esters over Cu/ZrO2 catalyst prepared by bio-derived salicylic acid

Abstract: A variety of bio-derived organic carboxylic acids are used to prepare Cu/ZrO2. In particular, salicylic acid provides superb control over the distribution of small Cu particles on t-ZrO2, which affords enhanced catalytic activity.

Cited by 23 publications

References 43 publications

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Highly selective and stable Cu/SiO2 catalysts prepared with a green method for hydrogenation of diethyl oxalate into ethylene glycol

Perspectives on the Active Sites and Catalyst Design for the Hydrogenation of Dimethyl Oxalate

CuOx/CeO2 catalyst derived from metal organic framework for reverse water-gas shift reaction

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Excellent performance in hydrogenation of esters over Cu/ZrO₂ catalyst prepared by bio-derived salicylic acid