The role of lattice anion vacancies in the activation of CO and as the catalytic site for methanol synthesis over zirconium dioxide and yttria-doped zirconium dioxide

Silver, Ronald G.; Hou, Cheinchang J.; Ekerdt, John G.

doi:10.1016/0021-9517(89)90327-8

Cited by 95 publications

(23 citation statements)

References 21 publications

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“…The incorporation of ZnO into ZrO 2 to form solid solution enhanced the signal at g value of 2.003 and thus the generation of oxygen vacancies over both ZnO-ZrO 2 and K + -ZnO-ZrO 2 samples. We believe that the increased density of oxygen vacancy sites favours the activation of CO as well as H 2 30,45,47 .…”

Section: Resultsmentioning

confidence: 92%

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Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

et al. 2020

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Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture of H 2 and CO) is an important but challenging research target. The current conversion of syngas to ethanol suffers from low selectivity or multiple processes with high energy consumption. Here, we report a high-selective conversion of syngas into ethanol by a triple tandem catalysis. An efficient trifunctional tandem system composed of potassium-modified ZnO-ZrO 2 , modified zeolite mordenite and Pt-Sn/SiC working compatibly in syngas stream in one reactor can afford ethanol with a selectivity of 90%. We demonstrate that the K + -ZnO-ZrO 2 catalyses syngas conversion to methanol and the mordenite with eight-membered ring channels functions for methanol carbonylation to acetic acid, which is then hydrogenated to ethanol over the Pt-Sn/SiC catalyst. The present work offers an effective methodology leading to high selective conversion by decoupling a single-catalyst-based complicated and uncontrollable reaction into well-controlled multi-steps in tandem in one reactor.

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Section: Resultsmentioning

confidence: 92%

“…Oxygen vacancy sites on ZrO 2 surfaces have been proposed to account for CO activation 45 . Our electron paramagnetic resonance (EPR) spectroscopy measurements showed a signal at g value of 2.003 ( Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

et al. 2020

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“…The authors found that addition of CeO 2 into monometallic nickel effectively improves the dispersion of Ni particles on the catalyst surface and enhances the stability of the catalyst. In the presence of both, yttrium oxide and cerium oxide, it was shown that the metal-support interactions enhanced catalytic performance, due to the oxygen storage/transport characteristic of the support [38], or to the generation of active centers at the interface between metal and support [29,[39][40][41]. Thus, to take advantage of the metal-support synergistic effect in the treatment of CO 2 reforming of CH 4 , nickel in interaction with ceria-yttria appears to be appropriate for developing a catalyst that is resistant to carbon deposition and that exhibits stable operation for extended periods of time as we found in Figure 6 for both Y and Ce doped catalysts.…”

Section: Catalytic Performance In Dry Methane Reformingmentioning

confidence: 99%

Ce- and Y-Modified Double-Layered Hydroxides as Catalysts for Dry Reforming of Methane: On the Effect of Yttrium Promotion

et al. 2019

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Ce- and Y-promoted double-layered hydroxides were synthesized and tested in dry reforming of methane (CH4/CO2 = 1/1). The characterization of the catalysts was performed using X-ray fluorescence (XRF), X-ray diffraction (XRD), N2 sorption, temperature-programmed reduction in H2 (TPR-H2), temperature-programmed desorption of CO2 (TPD-CO2), H2 chemisorption, thermogravimetric analysis coupled by mass spectrometry (TGA/MS), Raman, and high-resolution transmission electron microscopy (HRTEM). The promotion with cerium influences textural properties, improves the Ni dispersion, decreases the number of total basic sites, and increases the reduction temperature of nickel species. After promotion with yttrium, the increase in basicity is not directly correlated with the increasing Y loading on the contrary of Ni dispersion. Dry reforming of methane (DRM) was performed as a function of temperature and in isothermal conditions at 700 °C for 5 h. For catalytic tests, a slight increase of the activity is observed for both Y and Ce doped catalysts. This improvement can of course be explained by Ni dispersion, which was found higher for both Y and Ce promoted catalysts. During DRM, the H2/CO ratio was found below unity, which can be explained by side reactions occurrence. These side reactions are linked with the increase of CO2 conversion and led to carbon deposition. By HRTEM, only multi-walled and helical-shaped carbon nanotubes were identified on Y and Ce promoted catalysts. Finally, from Raman spectroscopy, it was found that on Y and Ce promoted catalysts, the formed C is less graphitic as compared to only Ce-based catalyst.

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“…Estas modificações no ZrO 2 alteram suas propriedades como: aumento na estabilização de fases cristalinas, aumento da basicidade e de sua condutividade iônica, propriedade esta que tem sido bastante estudada e muitos trabalhos demonstram sua vantagem principalmente em cerâmicas e eletrólitos sólidos (Bellido, 2008;Kilner, 1983apud Bellido, 2008. A modificação do dióxido de zircônio com aditivos origina vacâncias de oxigênio com carga efetiva positiva, que podem atuar como centros eletrofílicos, podendo ativar moléculas oxigenadas (Takeguchi et al, 2003apud Bellido, 2008, Dow e Huang, 1996 apud Bellido, 2008;Silver et al, 1989apud Bellido, 2008.…”

Section: Introductionunclassified

ESTUDO DE CATALISADORES DE ZrO2 MODIFICADOS COM METAIS ALCALINOS TERROSOS APLICADOS À REAÇÃO DE DECOMPOSIÇÃO DE ISOPROPANOL

Reis¹,

Bellido²,

Essayem³

et al. 2015

Anais Do XX Congresso Brasileiro De Engenharia Química

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The role of lattice anion vacancies in the activation of CO and as the catalytic site for methanol synthesis over zirconium dioxide and yttria-doped zirconium dioxide

Cited by 95 publications

References 21 publications

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Ce- and Y-Modified Double-Layered Hydroxides as Catalysts for Dry Reforming of Methane: On the Effect of Yttrium Promotion

ESTUDO DE CATALISADORES DE ZrO2 MODIFICADOS COM METAIS ALCALINOS TERROSOS APLICADOS À REAÇÃO DE DECOMPOSIÇÃO DE ISOPROPANOL

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