Carbon dioxide hydrogenation to methanol over Cu/ZrO<sub>2</sub>/CNTs: effect of carbon surface chemistry

Wang, Guannan; Chen, Limin; Sun, Yuhai; Wu, Junliang; Fu, Mingli; Ye, Daiqi

doi:10.1039/c5ra04774a

Cited by 50 publications

(22 citation statements)

References 59 publications

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“…The monometallic Cu/ZrO 2 catalyst shows two peaks, one at about 200 °C assigned to the reduction of CuO to Cu 2 O and a broad peak between 250 and 400 °C assigned to the consecutive reduction of Cu 2 O to Cu 0 . The presence of the two overlapping peaks can be attributed to the different CuO species that are differently interacting with the support. , The H 2 -TPR spectrum of the bimetallic CuPd/ZrO 2 shows one clear band from Cu (∼230 °C) and a shoulder (∼300 °C) assigned to reduction of Cu 2 O to Cu 0 . The peak from Cu reduction is shifted to higher temperatures compared to monometallic Cu/ZrO 2 , indicating a Cu–Pd interaction .…”

Section: Resultsmentioning

confidence: 99%

“…The presence of the two overlapping peaks can be attributed to the different CuO species that are differently interacting with the support. 42,43 The H 2 -TPR spectrum of the bimetallic CuPd/ZrO 2 shows one clear band from Cu (∼230 °C) and a shoulder (∼300 °C) assigned to reduction of Cu 2 O to Cu 0 . The peak from Cu reduction is shifted to higher temperatures compared to monometallic Cu/ZrO 2 , indicating a Cu−Pd interaction.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Bagnato

Signoretto

Pizzolitto

et al. 2020

ACS Sustainable Chem. Eng.

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A series of monometallic and bimetallic metal catalysts (Pd, Cu, Fe, PdCu, PdFe) supported on ZrO 2 (6−8 nm) were synthesized and tested for the hydrogenation of bio-oil model compounds (furfural, vanillin, glucose) under 50 bar H 2 at 100°C. The catalysts were fully characterized and their properties related to their catalytic activity. The bimetallic PdFe and PdCu displayed enhanced catalytic performance compared to the monometallic catalysts for aldehyde hydrogenation (furfural, vanillin, glucose). For the best catalyst, 98% vanillin alcohol (VA) and 65.5% furfuryl alcohol (FA) conversion was obtained for 80 min batch-time. PdFe showed high selectivity toward sorbitol (74%) from glucose, though at low conversion (20%). Overall, we have demonstrated that bimetallic Fe-and Cu-based catalysts promoted by Pd show significantly better performance for the partial hydrogenation of bio-oil model compounds than the corresponding monometallic ones. The better performance of the Pd-doped Fe/Cu catalysts is linked to the presence of smaller and better dispersed Pd nanoparticles (STEM) and their lower acidity (∼90 μmol/g cat) than corresponding monometallic ones (∼167 μmol/g cat).

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Section: Resultsmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Bagnato

Signoretto

Pizzolitto

et al. 2020

ACS Sustainable Chem. Eng.

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“…Metal oxides are the most common supports for the methanol synthesis catalysts, and their properties greatly affect the catalyst activity in several ways. The non-metallic supports, including metal organic frameworks (MOFs), porous silica materials, layered double hydroxides (LDHs), carbon materials, metal carbides, graphene, and porous polymers, have also been investigated (Rodriguez et al, 2015;Wang et al, 2015;Díez-Ramírez et al, 2016;Fan and Wu, 2016;Liu et al, 2016;Din et al, 2018;Sun et al, 2018;Witoon et al, 2018;Mureddu et al, 2019 (Toyir et al, 2009;Zhan et al, 2014;Hu et al, 2018).…”

Section: Supported and Promoted Cu Catalystsmentioning

confidence: 99%

Improving the Cu/ZnO-Based Catalysts for Carbon Dioxide Hydrogenation to Methanol, and the Use of Methanol As a Renewable Energy Storage Media

2020

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Heterogeneous catalytic hydrogenation of carbon dioxide (CO2) to methanol is a practical approach to mitigating its greenhouse effect in the environment while generating good economic profits. Though applicable on the industrial scale through the syngas route, the catalyst of Cu/ZnO/Al2O3 suffers from a series of technical problems when converting CO2 to methanol directly, which include low single-pass conversion, low methanol selectivity, requiring high pressure and fast deactivation by the reverse water gas shift reaction. Over the years, intensive research efforts have been devoted to proffering solutions to these problems by modifying the existing catalyst or developing new active catalysts. However, the open question is if this type of widely used industrial catalyst still promising for CO2 methanolizing reaction or not? This paper reviews the history of the methanol production in industry, the impact of CO2 emission on the environment, and analyzes the possibility of the Cu/ZnO-based catalysts for the direct hydrogenation of CO2 to methanol. We not only address the theoretical and technical aspects but also provide insightful views on catalyst development.

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“…The promoting effect of Nb 2 O 5 on the performance of Cu-ZrO 2 /CNF catalyst during the conversion of CO 2 to methanol was investigated by Din et al 233 The preparation of the catalyst involved mixing the solutions of zirconium nitrate with copper nitrate under vigorous stirring with added CNFs. The precipitate was aged at 90 °C for 20 h and filtered before 230−233 was investigated by Sun et al 234 and Wang et al, 235 using CNTs as supports. It is important to note that the Cu-ZrO 2/ CNF studies were conducted in a batch reactor while Cu-ZrO 2 /CNT catalysts were evaluated in a continuous fixed-bed reactor system at 220−260 °C and 3 MPa of H 2 , using a mixture of H 2 , CO 2 , and N 2 in concentrations of 69%, 23%, and 8%, respectively.…”

Section: Development Of Catalysts Supported Onmentioning

confidence: 99%

“…Note that little of CO was reported in the studies over Cu-ZrO 2 /CNF conducted in the batch reactor, 231,232 compared with CO being one of the major products over ZrO 2 /CNT observed in the continuous system. 234,235 In the former systems, the CO formation, as an intermediate, cannot be excluded. Thus, because it remains in the system, CO may be formed and then hydrogenated.…”

Section: Development Of Catalysts Supported Onmentioning

confidence: 99%

CO₂ Hydrogenation to Methanol and Methane over Carbon-Supported Catalysts

Furimsky¹

2020

Ind. Eng. Chem. Res.

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Methanol and methane are among the important products obtained during the hydrogenation (HYD) of CO2. The distribution of products and their yields can be influenced by operating conditions. In this case, the type of catalyst has a dominant effect. Gradual transformation of CO2 involves several surface intermediates. Special geometry of active site is required for maximizing the yield of methanol and for minimizing the reaction run-away to methane. Such a state can be attained over catalysts that contain CuO-ZnO components. Catalysts containing other transition metals and noble metals are less suitable, while the same catalysts exhibit good performance during the HYD of CO2 to methane. In industrial applications, catalysts supported on oxidic supports, i.e., Al2O3, SiO2, TiO2, etc., have been used. During HYD of CO2, 1 and 2 mol of water are generated for every mole of methanol and methane, respectively. The stability of catalysts used for HYD of CO2 can be enhanced by replacing oxidic supports with carbon supports. Amorphous carbons, such as activated carbon, and carbon nanomaterials, such as carbon nanotubes, carbon nanofibers, and graphene-derived solids, have been tested both as catalysts and supports. For methanol synthesis, CuO-ZnO catalysts supported on these carbons have been evaluated. Similar carbon supports have been used for the preparation and testing of methanation catalysts consisting of a wide range of transition and noble metals as active metals. Both monometallic and bimetallic catalysts were evaluated.

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Carbon dioxide hydrogenation to methanol over Cu/ZrO₂/CNTs: effect of carbon surface chemistry

Abstract: The excellent catalytic performance of Cu/ZrO2/CNTs is related to its H2 and CO2 adsorption capability, originating from nitrogen species on CNT.

Cited by 50 publications

References 59 publications

Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Improving the Cu/ZnO-Based Catalysts for Carbon Dioxide Hydrogenation to Methanol, and the Use of Methanol As a Renewable Energy Storage Media

CO₂ Hydrogenation to Methanol and Methane over Carbon-Supported Catalysts

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Carbon dioxide hydrogenation to methanol over Cu/ZrO2/CNTs: effect of carbon surface chemistry

Abstract: The excellent catalytic performance of Cu/ZrO2/CNTs is related to its H2 and CO2 adsorption capability, originating from nitrogen species on CNT.

Cited by 50 publications

References 59 publications

Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Hydrogenation of Biobased Aldehydes to Monoalcohols Using Bimetallic Catalysts

Improving the Cu/ZnO-Based Catalysts for Carbon Dioxide Hydrogenation to Methanol, and the Use of Methanol As a Renewable Energy Storage Media

CO2 Hydrogenation to Methanol and Methane over Carbon-Supported Catalysts

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Carbon dioxide hydrogenation to methanol over Cu/ZrO₂/CNTs: effect of carbon surface chemistry

CO₂ Hydrogenation to Methanol and Methane over Carbon-Supported Catalysts