Investigating the dynamic structural changes on Cu/CeO2 catalysts observed during CO2 hydrogenation

Sripada, Pramod; Kimpton, Justin A.; Barlow, Anders J.; Williams, Tim; Kandasamy, Shalini; Bhattacharya, Sankar

doi:10.1016/j.jcat.2019.11.017

Cited by 58 publications

(37 citation statements)

References 51 publications

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“…All these values comply with those reported in the literature . For the 10% Fe 450 -Ce x Zr 1– x O 2 samples, the BET surface area gradually decreased from 104 to 63 m 2 /g with increase in cerium loading, which is in agreement with previous studies. , However, both pore size and pore volume depicted exactly opposite trends. Both Fe 450 -ZrO 2 (Figure A) and 10% Fe 450 -Ce x Zr 1– x O 2 catalyst samples (Figure B) depicted type IV isotherm, indicating mesoporosity according to the IUPAC classification. − It is possible that the samples have a majority of mesopores with some macro- and micropores, an exact interpretation of which requires rigorous DFT calculation or t-plot analysis or the Horvath–Kawazoe pore size distribution analysis, which is beyond the scope of the present article.…”

Section: Resultssupporting

confidence: 92%

“…37 For the 10% Fe 450 -Ce x Zr 1−x O 2 samples, the BET surface area gradually decreased from 104 to 63 m 2 /g with increase in cerium loading, which is in agreement with previous studies. 42,43 However, both pore size and pore volume depicted exactly opposite trends. Both Fe 450 -ZrO 2 (Figure 3A) and 10% Fe 450 -Ce x Zr 1−x O 2 catalyst samples (Figure 3B) depicted type IV isotherm, indicating mesoporosity according to the IUPAC classification.…”

Section: Results and Discussion 41 H 2 Consumptionmentioning

confidence: 93%

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A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

Biswas

Kundu

Kulkarni

et al. 2021

Ind. Eng. Chem. Res.

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Fe-impregnated Ce x Zr1–x O2 supports were studied for CO2 methanation at 300, 400, and 500 °C under pressures 1 bar to 30 bars using a H2/CO2 (4:1 v/v) mixture, and their performance was compared to Fe-impregnated ZrO2. The variables affecting performance included temperature, pressure, and iron and cerium loadings. The iron loading that resulted in maximum CH4 selectivity and yield was 10 wt %. At 500 °C, Fe-Ce x Zr1–x O2 increased the CO2 uptake of the catalyst and its conversion to CO and CH4 by more than 50% compared to Fe-ZrO2. As a result, CH4 yield monotonically increased with temperature, but for Fe-ZrO2, it gradually decreased with temperature. Contrarily, at lower temperatures, Fe-ZrO2 gave higher CO2 conversion and CH4 yield. The highest CH4 yield was 25% with 10% Fe-Ce0.1Zr0.9O2 at 500 °C and 30 bars. This composition was also found to be highly stable over a continuous testing period of 100 h at 500 °C and 20 bars. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies indicated the possibility of a formate-assisted pathway of CH4 formation on Fe-Ce x Zr1–x O2.

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Section: Resultssupporting

confidence: 92%

Section: Results and Discussion 41 H 2 Consumptionmentioning

confidence: 93%

A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

Biswas

Kundu

Kulkarni

et al. 2021

Ind. Eng. Chem. Res.

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“…We consider a monolayer Cu 8 cluster supported on a clean CeO 2 (111) surface and perform the simulations at 773 K, corresponding to the usual experimental temperature for preparing the Cu/CeO 2 catalyst. 40,41 Without surprise, we indeed observe the spillover of lattice oxygen to the Cu cluster. As shown in Fig.…”

Section: Resultsmentioning

confidence: 72%

Lattice oxygen self-spillover on reducible oxide supported metal cluster: the water–gas shift reaction on Cu/CeO₂ catalyst

Xia

Qin

et al. 2021

Chem. Sci.

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“…Peaks were observed at 2800, 2625, 2125, 1950, 1810, 1625, 1440, 1375, and 1200 cm –1 during adsorption on ZSM-5/Ga 15 at 25 °C (Figure a). The vibrational modes at 1625 and 1440 cm –1 were attributed to carbonates and bicarbonates, respectively. − Other vibrational modes could not be assigned with complete confidence based on our literature review, but they could be reasonably be attributed to various carbonate/bicarbonate species. When the sample was heated to 200 °C for desorption (Figure b), the bands at 2800, 1810, 1440, 1375, and 1200 cm –1 disappeared, indicating that the associated carbonates were not strongly tethered to the surface.…”

Section: Resultsmentioning

confidence: 93%

Direct Ink Writing of Metal Oxide/H-ZSM-5 Catalysts for n-Hexane Cracking: A New Method of Additive Manufacturing with High Metal Oxide Loading

Lawson

Farsad

Rezaei

et al. 2020

ACS Appl. Mater. Interfaces

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Previously, 3D printing of porous materials and metal oxides was limited to low loading metal loadings, as increasing the nitrate salt concentrations, which are used to generate the oxide component, gave rise to poor rheological properties beyond 10 wt %. In this study, we addressed this problem by directly printing insoluble oxides alongside H-ZSM-5 zeolite, which allowed for increased oxide loadings. Various metal oxides such as V2O5, ZrO2, Cr2O3, and Ga2O3 were doped onto H-ZSM-5 through the additive manufacturing method. Characterization and correlation between the X-ray diffraction, NH3-temperature-programmed desorption, O2-temperature programmed oxidation, temperature-programmed reduction, scanning electron microscopy–energy dispersive spectroscopy, and in situ CO2 DRIFTS experiments revealed that directly 3D printing metal oxides/H-ZSM-5 inks leads to significant modification in the surface properties and oxide bulk dispersion, thereby enhancing the composites’ reducibility and giving rise to widely differing product distributions in n-hexane cracking reaction. The obtained metal oxide/zeolite structured materials were used as bifunctional structured catalysts for the selective formation of light olefins from hexane at 550–600 °C and GHSV = 9000 mL/gcatalst·h in a packed-bed reactor. Among the various compositions of metal oxides/H-ZSM-5 examined (i.e., 15 wt % Ga2O3, 15 wt % ZrO2, 15 wt % V2O5, 15 wt % Cr2O3, or 5 wt % Cr/10 wt % ZrO2/10 wt % V2O5/10 wt % Ga2O3 balanced with H-ZSM-5), the 15 wt % Cr/ZSM-5 monolith displayed the best n-hexane cracking performance, as it achieved 80–85% conversion of hexane with a 40% selectivity toward propylene, 30% selectivity toward ethylene, and 10% selectivity toward butene at 550 °C. The sample also showed zero benzene/toluene/xylene selectivity and no deactivation after 6 h. This study represents a proof-of-concept for tailoring customizable heterogeneous structured catalysts by directly 3D printing high loading of metal oxides/porous zeolite and is a breakthrough in material science.

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Investigating the dynamic structural changes on Cu/CeO2 catalysts observed during CO2 hydrogenation

Cited by 58 publications

References 51 publications

A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

Lattice oxygen self-spillover on reducible oxide supported metal cluster: the water–gas shift reaction on Cu/CeO₂ catalyst

Direct Ink Writing of Metal Oxide/H-ZSM-5 Catalysts for n-Hexane Cracking: A New Method of Additive Manufacturing with High Metal Oxide Loading

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Investigating the dynamic structural changes on Cu/CeO2 catalysts observed during CO2 hydrogenation

Cited by 58 publications

References 51 publications

A Study on CO2 Hydrogenation Using a Ceria–Zirconia Mixed Oxide (CexZr1–xO2)-Supported Fe Catalyst

A Study on CO2 Hydrogenation Using a Ceria–Zirconia Mixed Oxide (CexZr1–xO2)-Supported Fe Catalyst

Lattice oxygen self-spillover on reducible oxide supported metal cluster: the water–gas shift reaction on Cu/CeO2 catalyst

Direct Ink Writing of Metal Oxide/H-ZSM-5 Catalysts for n-Hexane Cracking: A New Method of Additive Manufacturing with High Metal Oxide Loading

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Product

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A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

A Study on CO₂ Hydrogenation Using a Ceria–Zirconia Mixed Oxide (Ce_xZr_1–xO₂)-Supported Fe Catalyst

Lattice oxygen self-spillover on reducible oxide supported metal cluster: the water–gas shift reaction on Cu/CeO₂ catalyst