CO2 hydrogenation to methanol over partially embedded Cu within Zn-Al oxide and the effect of indium

Stangeland, Kristian; Chamssine, Fawzi; Fu, Wenzhao; Huang, Zikun; Duan, Xuezhi; Yu, Zhixin

doi:10.1016/j.jcou.2021.101609

Cited by 19 publications

(10 citation statements)

References 56 publications

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“…Frei et al [60] reported that Cu + species are also detected during the reduction of Cu-based catalysts, although most of them turned to Cu 0 species after the reduction. This conclusion is agreed with in the work of Natesakhawat et al [47] and Zhou et al [48] However, other researchers propose [53,[61][62][63] different results, e.g., the Cu + species can be found during and after the reaction of CO2 hydrogenation. In this case, researchers started to pay attention to the role of Cu + species over the Cu-based catalysts in the CO2 hydrogenation.…”

Section: Active Sitessupporting

confidence: 91%

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Liu

2022

Catalysts

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The CO2 hydrogenation to dimethyl ether (DME) is a potentially promising process for efficiently utilizing CO2 as a renewable and cheap carbon resource. Currently, the one-step heterogeneous catalytic conversion of CO2 to value-added chemicals exhibits higher efficiency than photocatalytic or electrocatalytic routes. However, typical catalysts for the one-step CO2 hydrogenation to DME still suffer from the deficient space–time yield and stability in industrial demonstrations/applications. In this perspective, the recent development of the one-step CO2 hydrogenation to DME is focused on different catalytic systems by examining the reported experimental results and the reaction mechanism including the catalytic nature of active sites, activation modes and of CO2 molecules under relevant conditions; surface intermediates are comparatively analyzed and discussed. In addition to the more traditional Cu-based, Pd-based, and oxide-derived bifunctional catalysts, a further emphasis is given to the characteristics of the recently emerged In2O3-based bifunctional catalysts for the one-step conversion of CO2 to DME. Moreover, GaN itself, as a bifunctional catalyst, shows over 90% DME selectivity and a reasonably high activity for one-step CO2 hydrogenation, and the direct hydrogenation of CO2 via the unique non-methanol intermediate mechanism is highlighted as an important illustration for exploring new catalytic systems. With these analyses and current understandings, the research directions in the aspects of catalysis and DME economy are suggested for the further development of one-step DME synthesis from CO2 hydrogenation.

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Section: Active Sitessupporting

confidence: 91%

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Liu

2022

Catalysts

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“…Mg 2p spectra (Figure B) indicate a dominant band at 49.4 eV, characterizing Mg 2+ in the MgO or MgFe 2 O 4 structure . Cu 2p 3/2 spectra (Figure C) show a peak at 933.7 eV and a satellite peak at around 940–945 eV, assigned to the presence of Cu 2+ . In Zn 2p spectra (Figure D), the peaks at 1021.0–1021.3 and 1044.0–1044.4 eV correspond to Zn 2p 3/2 and Zn 2p 1/2 , respectively, assigned to Zn 2+ species.…”

Section: Resultsmentioning

confidence: 96%

“…55 Cu 2p 3/2 spectra (Figure 6C) show a peak at 933.7 eV and a satellite peak at around 940−945 eV, assigned to the presence of Cu 2+ . 56 In Zn 2p spectra (Figure 6D), the peaks at 1021.0−1021.3 and 1044.0−1044.4 eV correspond to Zn 2p 3/2 and Zn 2p 1/2 , respectively, assigned to Zn 2+ species. Regarding the reduced samples, in Cu 2p 3/2 spectra (Figure 6E), an additional peak at ∼932.6 eV (to the peak at 933.7 eV) can be assigned to the presence of Cu 0 or Cu + from the reduction of Cu 2+ species.…”

Section: Effect Of the Preparation Methodmentioning

confidence: 99%

Metallurgical Residue-Derived Cu–ZnO-Based Catalyst for CO₂ Hydrogenation to Methanol: An Insight on the Effect of the Preparation Method

Fongarland

Vanoye

et al. 2022

Ind. Eng. Chem. Res.

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Valorization of residual materials in the development of catalytic materials has an appealing potential from the perspective of a sustainable development. For the first time, Fe/Mg-containing metallurgical waste (UGSO) was utilized as a support for the development of innovative catalysts for CO2 hydrogenation into methanol. A series of different CuZn/UGSO catalysts were developed by conventional and modified deposition–coprecipitation methods. The addition of Cu/Zn into the structure of Fe3O4/MgxFe y O4 was found to improve Cu2+ and Zn2+ dispersion, while the presence of MgO favors methanol selectivity. Compared to 10Cu7.5Zn/UGSO (10 wt % Cu, 7.5 wt % Zn), the higher methanol yield obtained over 10Cu7.5Zn/UGSO–EtOH (10 wt % Cu, 7.5 wt % Zn, ethanol addition after coprecipitation) is a result of both higher CO2 conversion [attributed to (i) finer particle sizes of CuO and ZnO, (ii) a higher Cu0/Cu+ percentage, and (iii) higher oxygen vacancies and number of strong basic sites on the catalyst surface] and higher methanol selectivity [assigned to (i) the stronger interaction of Cu and ZnO and (ii) a higher number of medium basic sites] in comparison with its counterpart. This residue-based catalyst offers a 150% higher methanol yield than a commercial Cu-based methanol synthesis catalyst at 260 °C and 20 bar. These promising results can open a window to the utilization of this residue as a catalytic support in other CO2 hydrogenation processes.

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“…For instance, ZrO 2 supported In 2 O 3 catalyst prepared by precipitation showed 100% selectivity to methanol at 300 °C and 5 MPa . Some studies also reported the effect of indium incorporation into Cu-based catalysts for CO 2 hydrogenation to methanol. , The authors found that Cu-In 2 O 3 catalysts prepared by coprecipitation showed high activity and selectivity for CO 2 hydrogenation to methanol ascribed to the formation of Cu 9 In 11 alloy in close contact with an In 2 O 3 phase. It was also noted that In 2 O 3 oxygen vacancies and the Cu 11 In 9 surface adsorb and dissociate H 2 , showing a synergistic effect …”

Section: Direct Hydrogenation Of Co2 To Methanolmentioning

confidence: 99%

“…It was also noted that In 2 O 3 oxygen vacancies and the Cu 11 In 9 surface adsorb and dissociate H 2 , showing a synergistic effect. 36 The industrial synthesis of methanol from the direct hydrogenation of CO 2 has been carried out at the pilot plant level. In the late 19th century, Germany's Lurgi AG and Japan's Mitsui Chemicals carried out the pilot plant experiment for CO 2 hydrogenation to methanol over Cu-based commercial catalysts at relatively harsh reaction conditions (250 °C and 5− 8 MPa).…”

mentioning

confidence: 99%

Engineered Chemical Utilization of CO₂ to Methanol via Direct and Indirect Hydrogenation Pathways: A Review

Fayisa

Yang

Zhen

et al. 2022

Ind. Eng. Chem. Res.

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Nowadays, more than 80% of the world’s energy supply is provided by nonrenewable fossil fuels (oil, coal, and natural gas), which are the main sources of CO2 emission. The conversion of CO2 into the most useful organic chemicals (methanol and ethylene glycol (EG)) not only effectively mitigates CO2 emissions but also produces value-added chemicals and replaces nonrenewable energy sources. This Review provides a comprehensive view of the significant research progress on indirect CO2 hydrogenation to methanol and EG through the ethylene carbonate intermediate. First, the advances and challenges of direct catalytic hydrogenation of CO2 to methanol are addressed. Subsequently, the advances in CO2 epoxidation to cyclic carbonates, particularly to ethylene carbonate, are summarized. This matured and commercialized ethylene carbonate (EC) production route is vital because of the efficient production of EG and methanol from catalytic hydrogenation of EC and hydrolysis of EC to EG, which replaces the conventional EG production process by hydration of ethylene oxide. Then, the progress on the catalytic hydrogenation of CO2-derived EC is discussed in detail, focusing on Cu-based heterogeneous catalysts. We provided a detailed discussion with emphasis on the nature, evolution, and precise role of active sites in Cu-based catalysts, including other influencing factors such as the preparation method, support, and addition of promoters. Moreover, the possible hydrogenation reaction mechanism, reaction conditions, design optimization, and on-site assessment of Cu-based catalysts for EC hydrogenation are included. Lastly, we provided a summary and outlook.

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CO2 hydrogenation to methanol over partially embedded Cu within Zn-Al oxide and the effect of indium

Cited by 19 publications

References 56 publications

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Metallurgical Residue-Derived Cu–ZnO-Based Catalyst for CO₂ Hydrogenation to Methanol: An Insight on the Effect of the Preparation Method

Engineered Chemical Utilization of CO₂ to Methanol via Direct and Indirect Hydrogenation Pathways: A Review

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CO2 hydrogenation to methanol over partially embedded Cu within Zn-Al oxide and the effect of indium

Cited by 19 publications

References 56 publications

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Metallurgical Residue-Derived Cu–ZnO-Based Catalyst for CO2 Hydrogenation to Methanol: An Insight on the Effect of the Preparation Method

Engineered Chemical Utilization of CO2 to Methanol via Direct and Indirect Hydrogenation Pathways: A Review

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Metallurgical Residue-Derived Cu–ZnO-Based Catalyst for CO₂ Hydrogenation to Methanol: An Insight on the Effect of the Preparation Method

Engineered Chemical Utilization of CO₂ to Methanol via Direct and Indirect Hydrogenation Pathways: A Review