CO 2 hydrogenation to methanol over CuO–ZnO–ZrO 2 –SiO 2 catalysts: Effects of SiO 2 contents

Phongamwong, Thanaree; Chantaprasertporn, Usanee; Witoon, Thongthai; Numpilai, Thanapa; Poo‐arporn, Yingyot; Limphirat, Wanwisa; Donphai, Waleeporn; Dittanet, Peerapan; Chareonpanich, Metta; Limtrakul, Jumras

doi:10.1016/j.cej.2017.02.010

Cited by 175 publications

(101 citation statements)

References 67 publications

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“…Moreover, the reduction peaks of CuIn/SiO 2 are observed to shift toward lower temperatures, compared with CuIn@SiO 2 . This indicates that a stronger interaction between metal oxides and silica exists in the core–shell structured catalyst than in the impregnated catalyst . Hence, considering the reduction temperature used in this study (350°C), CuO can be completely reduced in all catalysts, and only some In 2 O 3 metal oxides are reduced in In@SiO 2 , CuIn@SiO 2 , and CuIn/SiO 2 catalysts.…”

Section: Resultsmentioning

confidence: 86%

A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

Shi

Tan

2018

AIChE Journal

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CO 2 hydrogenation is one of the most promising processes in response to energy crisis and greenhouse gas emission. There is, however, still a lack of a highly efficient and sustainable catalyst for this reaction. In this study, a novel low-cost coreshell structured CuIn@SiO 2 catalyst is prepared by a solvothermal method and used for catalyzing CO 2 hydrogenation to methanol. A significant interaction exists between Cu and In, promoting Cu dispersion and reducibility, Cu 2 In alloy and oxygen vacancy formation. Moreover, plenty of interfacial sites are formed between Cu 2 In and In 2 O 3 , which further enhances CO 2 adsorption and activation. CuIn@SiO 2 , therefore, shows not only a satisfactory catalytic stability due to core-shell formation but also an excellent catalytic performance. 9.8% CO 2 conversion, 78.1% CH 3 OH selectivity, and 13.7 mmol CH 3 OH Áh −1 Ág cat −1 CH 3 OH space-time yield are obtained at the space velocity of 20,000 mLÁg cat −1 Áh −1 . CuIn@SiO 2 possesses a great potential as catalyst for CO 2 hydrogenation in a moderate condition in industry.

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Section: Resultsmentioning

confidence: 86%

A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

Shi

Tan

2018

AIChE Journal

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“…Zr was added to the support as active reaction sites for surface carbonate formation. The carbonate groups can then react with the atomic hydrogen generated by H2 splitting over Cu to finally form carbon based fuels 20,[23][24][25] . Two types of Cu-Zr-SBA-15 were synthesized.…”

Section: Introductionmentioning

confidence: 99%

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Atakan

Erdtman

Mäkie

et al. 2018

Journal of Catalysis

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The self-archived postprint version of this journal article is available at Linköping University Institutional Repository (DiVA): http://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-147297 N.B.: When citing this work, cite the original publication.Atakan, A., Erdtman, E., Mäkie, P., Ojamäe, L., Odén, M., (2018) ABSTRACT: Time evolution of catalytic CO2 hydrogenation to methanol and dimethyl ether (DME) has been investigated in a hightemperature high-pressure reaction chamber where products accumulate over time. The employed catalysts are based on a nano-assembly composed of Cu nanoparticles infiltrated into a Zr doped SiOx mesoporous framework (SBA-15): Cu-Zr-SBA-15. The CO2 conversion was recorded as a function of time by gas chromatography-mass spectrometry (GC-MS) and the molecular activity on the catalyst's surface was examined by diffuse reflectance in-situ Fourier transform infrared spectroscopy (DRIFTS). The experimental results showed that after 14 days a CO2 conversion of 25% to methanol and DME was reached when a DME selective catalyst was used which was also illustrated by thermodynamic equilibrium calculations. With higher Zr content in the catalyst, greater selectivity for methanol and a total 9.5 % conversion to methanol and DME was observed, yielding also CO as an additional product. The time evolution profiles indicated that DME is formed directly from methoxy groups in this reaction system. Both DME and methanol selective systems show the thermodynamically highest possible conversion.

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“…Stability is an important factor in determining whether a Cu‐based catalyst can be used for the direct synthesis of methanol from CO 2 hydrogenation in industrial production . To investigate the stability of the CuO–ZnO–ZrO 2 catalysts prepared by microwave‐assisted hydrothermal synthesis, a long‐term test of the best‐performing CZZ‐120 catalyst was performed in a continuous‐flow fixed‐bed reactor under the reaction conditions of 240 °C, CO 2 /H 2 =1:3 ( v / v ), 3.0 MPa, and space velocity (SV)=2400 mL g cat −1 h −1 .…”

Section: Resultsmentioning

confidence: 99%

“…Stability is an importantf actor in determining whether a Cu-based catalyst can be used for the direct synthesis of methanol from CO 2 hydrogenationi ni ndustrial production. [36,42] To investigate the stability of the CuO-ZnO-ZrO 2 catalysts prepared by microwave-assisted hydrothermal synthesis,along-term test of the best-performingC ZZ-120 catalyst was performed in ac ontinuous-flow fixed-bed reactor under the reaction conditions of 240 8C, CO 2 /H 2 = 1:3( v/v), 3.0 MPa, and space velocity( SV) = 2400 mL g cat À1 h À1 .T he conversion of CO 2 and the selectivity to methanold ecreased by 3.3 %a nd 1.3 %, respectively,a fter 100 hr eaction (Figure 9). This result indicates that the catalyst developed in this work is highly stable in the reaction.…”

Section: Catalytic Performancementioning

confidence: 99%

Microwave‐Assisted Hydrothermal Synthesis of CuO–ZnO–ZrO₂ as Catalyst for Direct Synthesis of Methanol by Carbon Dioxide Hydrogenation

et al. 2017

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A series of CuO–ZnO–ZrO2 catalysts was prepared by a facile microwave‐assisted hydrothermal synthesis method and used for the direct synthesis of methanol by CO2 hydrogenation in a fixed‐bed reactor at 240 °C, 3.0 MPa, CO2/H2=1:3 (v/v), and space velocity of 2400 mL gcat−1 h−1. The effects of the hydrothermal synthesis temperature (80–150 °C) on the physicochemical properties and catalytic activity of the CuO–ZnO–ZrO2 catalysts were investigated by using several techniques, including XRD, N2 adsorption, reactive N2O adsorption, SEM with energy‐dispersive X‐ray spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction by H2, and the temperature‐programmed desorption of adsorbed CO2 and H2. The catalyst prepared at 120 °C possessed a high surface area, a high dispersion of Cu species, a high adsorption capacity for CO2 and H2, and thus exhibited a high CO2 conversion and methanol selectivity. The surface area of metallic Cu (SCu) is the critical factor in determining the activity of the CuO–ZnO–ZrO2 catalyst.

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CO 2 hydrogenation to methanol over CuO–ZnO–ZrO 2 –SiO 2 catalysts: Effects of SiO 2 contents

Cited by 175 publications

References 67 publications

A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Microwave‐Assisted Hydrothermal Synthesis of CuO–ZnO–ZrO₂ as Catalyst for Direct Synthesis of Methanol by Carbon Dioxide Hydrogenation

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CO 2 hydrogenation to methanol over CuO–ZnO–ZrO 2 –SiO 2 catalysts: Effects of SiO 2 contents

Cited by 175 publications

References 67 publications

A novel Core–Shell structured CuIn@SiO2 catalyst for CO2 hydrogenation to methanol

A novel Core–Shell structured CuIn@SiO2 catalyst for CO2 hydrogenation to methanol

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Microwave‐Assisted Hydrothermal Synthesis of CuO–ZnO–ZrO2 as Catalyst for Direct Synthesis of Methanol by Carbon Dioxide Hydrogenation

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A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

A novel Core–Shell structured CuIn@SiO₂ catalyst for CO₂ hydrogenation to methanol

Microwave‐Assisted Hydrothermal Synthesis of CuO–ZnO–ZrO₂ as Catalyst for Direct Synthesis of Methanol by Carbon Dioxide Hydrogenation