A DRIFTS and TPD study on the methanation of CO2 on Ni/Al2O3 catalyst

Schreiter, Norman; Kirchner, Johann; Kureti, Sven

doi:10.1016/j.catcom.2020.105988

Cited by 47 publications

(21 citation statements)

References 32 publications

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“…Usually, the increase of the first peak is attributed solely to an increase of basic sites on the support or due to the metal/support interface. 26 However, as shown by the measured CO 2 uptake for different Ni crystal sizes (see Figure 3), it can be concluded that the metal/support interface does not play a significant role for the CO 2 adsorption capacity. The Ni/SiO 2 catalyst provides new insights since the support showed nearly no CO 2 uptake.…”

Section: ■ Results and Discussionmentioning

confidence: 85%

“…The desorption kinetics from basic sites with medium strength and the heat of adsorption have to be similar to the kinetics for Ni(111). This reveals that for the interpretation of desorption profiles in the literature, 24,26 the desorption from different Ni facets must be considered.…”

Section: ■ Results and Discussionmentioning

confidence: 96%

“…Multiple CO 2 and CO desorption peaks are usually detected during the TPD. 24,26 The different CO 2 peaks are explained by desorption from basic sites from the support with different binding strengths. It is possible to use supports with an acidic surface like SiO 2 , which interacts with CO 2 to a minor extent and reduces the complexity.…”

Section: ■ Introductionmentioning

confidence: 99%

“…All TPD studies on CO 2 adsorption on Ni/γ-Al 2 O 3 catalysts focus only on the differentiation between adsorption on Ni and basic sites with different binding strength on the support. Multiple CO 2 and CO desorption peaks are usually detected during the TPD. , The different CO 2 peaks are explained by desorption from basic sites from the support with different binding strengths. It is possible to use supports with an acidic surface like SiO 2 , which interacts with CO 2 to a minor extent and reduces the complexity .…”

Section: Introductionmentioning

confidence: 99%

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Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

2021

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The conversion of CO 2 into valuable products with hydrogenation reactions on Ni catalysts requires a fundamental understanding of the interaction of CO 2 with the Ni surface. Microkinetic modeling is used to investigate the interaction of CO 2 with a multifaceted Ni crystal and compared to temperature-programmed desorption (TPD) experiments from supported Ni catalysts. TPD experiments were performed for Ni/γ-Al 2 O 3 and Ni/SiO 2 catalysts. Uncertainties in the DFT-derived model parameters were accounted for by a global uncertainty analysis (GUA). On the basis of the model, the adsorption and desorption of CO 2 exhibit a structure−sensitivity for the investigated Ni facets. Whereas the initial multifaceted TPD model is not in quantitative agreement with the experimentally recorded desorption profile, the GUA reveals a feasible set of model parameters that are in close agreement with the data. The comparison of the desorption profiles of the different catalysts and the multifacet simulation shows that desorption of CO 2 from basic sites and desorption from the Ni facets overlap and thus have similar desorption kinetics.

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Section: ■ Results and Discussionmentioning

confidence: 85%

Section: ■ Results and Discussionmentioning

confidence: 96%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

2021

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“…On the other side, in the region of 1700-1300 cm −1 are shown the symmetric and asymmetric stretching modes characteristic of superficial carbonates, formates or carboxylates. The bands at 1591 and 1371 cm −1 have been attributed to monodentate carbonates [59,60], whereas the shoulder at 1640 cm −1 is associated to physisorbed water. The intensities of both bands decrease on increasing the temperature during the reaction as is expected.…”

Section: Wgs Reaction Under Model Conditionsmentioning

confidence: 99%

Elucidation of Water Promoter Effect of Proton Conductor in WGS Reaction over Pt-Based Catalyst: An Operando DRIFTS Study

et al. 2020

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A conventional Pt/CeO2/Al2O3 catalyst physically mixed with an ionic conductor (Mo- or Eu-doped ZrO2) was tested at high space velocity (20,000 h−1 and 80 L h−1 gcat−1) under model conditions (only with CO and H2O) and industrial conditions, with a realistic feed. The promoted system with the ionic conductor physically mixed showed better catalytic activity associated with better water dissociation and mobility, considered as a rate-determining step. The water activation was assessed by operando diffuse reflectance infrared fourier transformed spectroscopy (DRIFTS) studies under reaction conditions and the Mo-containing ionic conductor exhibited the presence of both dissociated (3724 cm−1) and physisorbed (5239 cm−1) water on the Eu-doped ZrO2 solid solution, which supports the appearance of proton conductivity by Grotthuss mechanism. Moreover, the band at 3633 cm−1 ascribed to hydrated Mo oxide, which increases with the temperature, explains the increase of catalytic activity when the physical mixture was used in a water gas shift (WGS) reaction.

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Using Phosphonic Acid Monolayers to Control CO₂ Adsorption and Hydrogenation on Pt/Al₂O₃

Blanchette,

Zhou,

Schwartz

et al. 2024

ChemCatChem

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Phosphonic acid (PA) self‐assembled monolayers (SAMs) were deposited onto Pt/Al2O3 catalysts to enable control over CO2 adsorption and CO2 hydrogenation activity. Significant differences in catalytic activity toward CO2 hydrogenation (reverse water‐gas shift, RWGS) were observed after coating Al2O3 with PAs, suggesting that the reaction was mediated by CO2adsorption on the support. Amine‐functionalized PAs were found to outperform their alkyl counterparts in terms of activity, however there was little effect of amine location in the SAM (i.e., spacing between the amine functional group and phosphonate attachment group). One amine‐PA and one alkyl‐PA, aminopropyl phosphonic acid (C3NH2PA) and methyl phosphonic acid (C1PA), respectively, were investigated in more detail. The C3NH2PA‐modified catalyst was found to bind CO2 as a combination of carbamate and bicarbonate. Additionally, at 30 °C, both PAs were found to reduce CO2 adsorption uptake by approximately 50% compared to unmodified 5%Pt/Al2O3. CO2 adsorption enthalpy was measured for the catalysts and found to be strongly correlated with hydrogenation activity, with the trend in binding enthalpy and CO2 hydrogen rate trending as uncoated > C3NH2PA > C1PA. PA SAMs were found to have weaker effects on CO binding and CO selectivity, consistent with selective modification of the Al2O3support by the PAs.

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A DRIFTS and TPD study on the methanation of CO2 on Ni/Al2O3 catalyst

Cited by 47 publications

References 32 publications

Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

Elucidation of Water Promoter Effect of Proton Conductor in WGS Reaction over Pt-Based Catalyst: An Operando DRIFTS Study

Using Phosphonic Acid Monolayers to Control CO₂ Adsorption and Hydrogenation on Pt/Al₂O₃

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A DRIFTS and TPD study on the methanation of CO2 on Ni/Al2O3 catalyst

Cited by 47 publications

References 32 publications

Microkinetic Modeling of the CO2 Desorption from Supported Multifaceted Ni Catalysts

Microkinetic Modeling of the CO2 Desorption from Supported Multifaceted Ni Catalysts

Elucidation of Water Promoter Effect of Proton Conductor in WGS Reaction over Pt-Based Catalyst: An Operando DRIFTS Study

Using Phosphonic Acid Monolayers to Control CO2 Adsorption and Hydrogenation on Pt/Al2O3

Contact Info

Product

Resources

About

Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

Microkinetic Modeling of the CO₂ Desorption from Supported Multifaceted Ni Catalysts

Using Phosphonic Acid Monolayers to Control CO₂ Adsorption and Hydrogenation on Pt/Al₂O₃