Ceria imparts superior low temperature activity to nickel catalysts for CO<sub>2</sub> methanation

Guo, Xinpeng; He, Hongyan; Traitangwong, Atsadang; Gong, Maoming; Meeyoo, Vissanu; Li, Ping; Li, Chunshan; Peng, Zhijian; Zhang, Suojiang

doi:10.1039/c9cy01186b

Cited by 46 publications

(16 citation statements)

References 57 publications

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“…It is consistent with the detection of the −OH group in the O 1s spectrum. 57 There was no detectable band of formate species (m-HCOO, 1372 and 1541 cm −1 ), methoxy species (1475 cm −1 ), or methane 58 as that observed in the spectra for the reaction over Ni/CeO 2 in the investigated temperature range (Figure S17), suggesting the dominant formation of CO over Ni/ZnO does not proceed through the formate-intermediate pathway. In this work, the Ni−Zn sites are considered to be the major active sites, given their much higher activity relative to ZnO and weak interfacial effect.…”

Section: Mechanistic Pathwaymentioning

confidence: 99%

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Lin

Wang

et al. 2022

ACS Catal.

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Controlling the selectivity of CO 2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO 2 hydrogenation. The alloying of Ni with Zn to charged (Ni σ− −Zn σ+ ) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H 2 , and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO 2 species in a η 2 (C, O) bridge configuration, directly dissociate the CO bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO 2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.

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Section: Mechanistic Pathwaymentioning

confidence: 99%

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Lin

Wang

et al. 2022

ACS Catal.

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“…The positive effect of Ce was attributed to the improved reducibility of Ni species (e.g., weakening of Ni-Al 2 O 3 interactions) and enhanced activation of CO 2 on Ce sites. Guo et al [84] developed an innovative catalyst by synthesizing Ni-Al 2 O 3 LDHs (layered double support) and using CeO 2 as promoter. Authors obtained the best performances when using ~50 wt% CeO 2 due to the small and highly dispersed Ni 0 particles formed and due to the existence of oxygen vacancies that directly increased the active sites and promoted CO 2 adsorption.…”

Section: Bimetallic Al 2 O 3 -Supported Catalystsmentioning

confidence: 99%

Promising Catalytic Systems for CO2 Hydrogenation into CH4: A Review of Recent Studies

et al. 2020

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The increasing utilization of renewable sources for electricity production turns CO2 methanation into a key process in the future energy context, as this reaction allows storing the temporary renewable electricity surplus in the natural gas network (Power-to-Gas). This kind of chemical reaction requires the use of a catalyst and thus it has gained the attention of many researchers thriving to achieve active, selective and stable materials in a remarkable number of studies. The existing papers published in literature in the past few years about CO2 methanation tackled the catalysts composition and their related performances and mechanisms, which served as a basis for researchers to further extend their in-depth investigations in the reported systems. In summary, the focus was mainly in the enhancement of the synthesized materials that involved the active metal phase (i.e., boosting its dispersion), the different types of solid supports, and the frequent addition of a second metal oxide (usually behaving as a promoter). The current manuscript aims in recapping a huge number of trials and is divided based on the support nature: SiO2, Al2O3, CeO2, ZrO2, MgO, hydrotalcites, carbons and zeolites, and proposes the main properties to be kept for obtaining highly efficient carbon dioxide methanation catalysts.

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“…Recently, much attention has been paid on determining the mechanism of CO 2 methanation over Ni- or Ru-supported catalysts. − Based on IR characterization techniques, two main reaction pathways have been proposed to describe the CO 2 hydrogenation to methane over different explored catalysts: (i) the associative adsorption of CO 2 and its hydrogenation-to-formate pathway, − and (ii) the dissociative adsorption of CO 2 in form CO*, which can be hydrogenated to formyl (CHO*) or dissociated to carbon (C*) and O* . However, there is no general agreement on the reaction mechanism on Ni/CeO 2 catalyst.…”

Section: Introductionmentioning

confidence: 99%

Kinetics, Model Discrimination, and Parameters Estimation of CO₂ Methanation on Highly Active Ni/CeO₂ Catalyst

Onrubia-Calvo

Quindimil

Davó‐Quiñonero

et al. 2022

Ind. Eng. Chem. Res.

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The reaction kinetics of CO2 methanation over a highly active 8.5% Ni/CeO2 catalyst was determined in a fixed-bed reactor, in the absence of heat- and mass-transfer limitations. Once the catalyst activity was stabilized, more than 120 kinetic experiments (with varying values of reaction temperature, total pressure, space velocity (GHSV), and partial pressure of products and reactants) were performed. From initial reaction rates, an apparent activation energy of 103.9 kJ mol–1 was determined, as well as the effect of reactants (positive) and water partial pressures (negative) on CO2 methanation rate. Three mechanistic models reported in the literature, in which CO2 is adsorbed dissociatively (carbon and formyl routes) or directly (formate route), were explored for modeling the entire reaction kinetics. For that, the corresponding rate equations were developed through the Langmuir–Hinshelwood–Hougen–Watson (LHHW) approach. In agreement with DRIFTS experiments, formate route, in which the hydrogenation of bicarbonate to formate is considered to be the rate-determining step, reflects the kinetic data accurately, operating from differential conversion to thermodynamic equilibrium. In fact, this mechanism results in a mean deviation (D) of 10.38%. Based on previous own mechanistic studies, the participation of two different active sites has been also considered. Formate route on two active sites maintains a high fitting quality of experimental data, providing kinetics parameters with a higher physical significance. Thus, the LHHW mechanism, in which Ni0 sites as well as oxygen vacant near to Ni-CeO2 interface participate in CO2 methanation, is able to predict the kinetics of Ni/CeO2 catalyst accurately for a wide range of operational conditions.

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Ceria imparts superior low temperature activity to nickel catalysts for CO₂ methanation

Abstract: Proposed reaction mechanism for CO2 methanation on NiAl-MO/CeO2-x catalysts.

Cited by 46 publications

References 57 publications

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Promising Catalytic Systems for CO2 Hydrogenation into CH4: A Review of Recent Studies

Kinetics, Model Discrimination, and Parameters Estimation of CO₂ Methanation on Highly Active Ni/CeO₂ Catalyst

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Ceria imparts superior low temperature activity to nickel catalysts for CO2 methanation

Abstract: Proposed reaction mechanism for CO2 methanation on NiAl-MO/CeO2-x catalysts.

Cited by 46 publications

References 57 publications

Ni–Zn Dual Sites Switch the CO2 Hydrogenation Selectivity via Tuning of the d-Band Center

Ni–Zn Dual Sites Switch the CO2 Hydrogenation Selectivity via Tuning of the d-Band Center

Promising Catalytic Systems for CO2 Hydrogenation into CH4: A Review of Recent Studies

Kinetics, Model Discrimination, and Parameters Estimation of CO2 Methanation on Highly Active Ni/CeO2 Catalyst

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Ceria imparts superior low temperature activity to nickel catalysts for CO₂ methanation

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Ni–Zn Dual Sites Switch the CO₂ Hydrogenation Selectivity via Tuning of the d-Band Center

Kinetics, Model Discrimination, and Parameters Estimation of CO₂ Methanation on Highly Active Ni/CeO₂ Catalyst