Reaction Intermediates and Side Products in the Methanation of CO and CO<sub>2</sub> over Supported Ru Catalysts in H<sub>2</sub>-Rich Reformate Gases

Eckle, Stephan; Anfang, Hans-Georg; Behm, R. Jürgen

doi:10.1021/jp108106t

Cited by 244 publications

(202 citation statements)

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“…Few works have been published on Ni supported on zeolites for CO 2 methanation [49,[105][106][107]. Recently, Graca et al [108] prepared, by ion exchange and impregnation, Ni-Ce catalysts supported on a partially exchanged HNaUSY zeolite.…”

Section: Alumina-supported Nickelmentioning

confidence: 99%

Supported Catalysts for CO2 Methanation: A Review

et al. 2017

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CO 2 methanation is a well-known reaction that is of interest as a capture and storage (CCS) process and as a renewable energy storage system based on a power-to-gas conversion process by substitute or synthetic natural gas (SNG) production. Integrating water electrolysis and CO 2 methanation is a highly effective way to store energy produced by renewables sources. The conversion of electricity into methane takes place via two steps: hydrogen is produced by electrolysis and converted to methane by CO 2 methanation. The effectiveness and efficiency of power-to-gas plants strongly depend on the CO 2 methanation process. For this reason, research on CO 2 methanation has intensified over the last 10 years. The rise of active, selective, and stable catalysts is the core of the CO 2 methanation process. Novel, heterogeneous catalysts have been tested and tuned such that the CO 2 methanation process increases their productivity. The present work aims to give a critical overview of CO 2 methanation catalyst production and research carried out in the last 50 years. The fundamentals of reaction mechanism, catalyst deactivation, and catalyst promoters, as well as a discussion of current and future developments in CO 2 methanation, are also included.

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Section: Alumina-supported Nickelmentioning

confidence: 99%

Supported Catalysts for CO2 Methanation: A Review

et al. 2017

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“…For more information about the adlayer and its reactionr elated changes,werefer the readertop revious studies. [17,34] On-top adsorbed/bridgedCO ad Followingt he sequence described in the kinetic measurements, the fresh catalystw as either exposed to dry reformate only (activation and reactionind ry reformate) or it was first activateda nd operated in SR-ref 6000 containing 5o r1 5% H 2 O, respectively,p rior to the reactioni nd ry SR-ref 6000 reformate. Representative spectra recorded after 700 min of reaction time during the reaction in dry reformate, after activationi nd ry or wet reformate, are presented in Figure 8.…”

Section: Time Evolution Of the Adlayermentioning

confidence: 99%

Improved Performance of Ru/γ‐Al₂O₃ Catalysts in the Selective Methanation of CO in CO₂‐Rich Reformate Gases upon Transient Exposure to Water‐Containing Reaction Gas

et al. 2015

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To better understand the role of water in the selective methanation of CO in CO2-rich reformate gases on Ru/Al2O3 catalysts, the influence of exposing these catalysts to H2O-rich reformate gases on their reaction characteristics in transient experiments was investigated by employing kinetic and in situ spectroscopic measurements as well as ex situ catalyst characterization. Transient exposure of the ruthenium catalyst to wet reaction gas (5 or 15% H2O) results in significantly enhanced activity and selectivity for CO methanation in subsequent reactions in dry reformate compared with activation and reaction in dry reformate directly. Operando X-ray absorption spectroscopy results reveal that this is in accordance with a significant decrease in ruthenium particle size, which is stable during subsequent reaction in dry reformate. The implications of these data and additional results from in situ IR spectroscopy on the role and influence of H2O on the reaction, also in technical applications, are discussed.

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“…The formation of formyl species was experimentally detected by Eckle et al [71] in time resolved in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements on Ru/Al2O3 catalyst in idealized reformate (CO/H2/N2) conditions (band at 1760 cm −1 ). As it happens for Co and Fe, barriers on Ru catalysts for the unassisted reaction are much higher than those calculated after hydrogenation; this is the case of CO dissociation on the planar (111) terraces and also on low-coordination atoms at step-edge sites.…”

Section: Co* + H* → Coh* + * (3a)mentioning

confidence: 91%

“…However, formation of formyl species is predicted on the Co(101 � 0)B surface but its decomposition seems to be unaffordable [54]. Interestingly, in the DRIFTS experiments of Eckle et al [71] but on a Ru/zeolite catalyst, it was not observed the band at 1760 cm −1 attributed to adsorbed HCO species. These results are strong evidences that quite small changes in the structure of a typical catalyst for the Fischer-Tropsch reaction can change dramatically its activity.…”

Section: Co* + H* → Coh* + * (3a)mentioning

confidence: 92%

Fischer-Tropsch Synthesis on Multicomponent Catalysts: What Can We Learn from Computer Simulations?

2015

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Abstract:In this concise review paper, we will address recent studies based on the generalized-gradient approximation (GGA) of the density functional theory (DFT) and on the periodic slab approach devoted to the understanding of the Fischer-Tropsch synthesis process on transition metal catalysts. As it will be seen, this computational combination arises as a very adequate strategy for the study of the reaction mechanisms on transition metal surfaces under well-controlled conditions and allows separating the influence of different parameters, e.g., catalyst surface morphology and coverage, influence of co-adsorbates, among others, in the global catalytic processes. In fact, the computational studies can now compete with research employing modern experimental techniques since very efficient parallel computer codes and powerful computers enable the investigation of more realistic molecular systems in terms of size and composition and to explore the complexity of the potential energy surfaces connecting reactants, to intermediates, to products of reaction. In the case of the Fischer-Tropsch process, the calculations were used to complement experimental work and to clarify the reaction mechanisms on different catalyst models, as well as the influence of additional components and co-adsorbate species in catalyst activity and selectivity.

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Reaction Intermediates and Side Products in the Methanation of CO and CO₂ over Supported Ru Catalysts in H₂-Rich Reformate Gases

Cited by 244 publications

References 44 publications

Supported Catalysts for CO2 Methanation: A Review

Supported Catalysts for CO2 Methanation: A Review

Improved Performance of Ru/γ‐Al₂O₃ Catalysts in the Selective Methanation of CO in CO₂‐Rich Reformate Gases upon Transient Exposure to Water‐Containing Reaction Gas

Fischer-Tropsch Synthesis on Multicomponent Catalysts: What Can We Learn from Computer Simulations?

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Reaction Intermediates and Side Products in the Methanation of CO and CO2 over Supported Ru Catalysts in H2-Rich Reformate Gases

Cited by 244 publications

References 44 publications

Supported Catalysts for CO2 Methanation: A Review

Supported Catalysts for CO2 Methanation: A Review

Improved Performance of Ru/γ‐Al2O3 Catalysts in the Selective Methanation of CO in CO2‐Rich Reformate Gases upon Transient Exposure to Water‐Containing Reaction Gas

Fischer-Tropsch Synthesis on Multicomponent Catalysts: What Can We Learn from Computer Simulations?

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Reaction Intermediates and Side Products in the Methanation of CO and CO₂ over Supported Ru Catalysts in H₂-Rich Reformate Gases

Improved Performance of Ru/γ‐Al₂O₃ Catalysts in the Selective Methanation of CO in CO₂‐Rich Reformate Gases upon Transient Exposure to Water‐Containing Reaction Gas