Characterization of surface processes at the Ni-based catalyst during the methanation of biomass-derived synthesis gas: X-ray photoelectron spectroscopy (XPS)

Czekaj, Izabela; Loviat, Francois; Raimondi, Fabio; Wambach, J.; Biollaz, Serge M.A.; Wokaun, Alexander

doi:10.1016/j.apcata.2007.06.027

Cited by 272 publications

(173 citation statements)

References 45 publications

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“…1 6,7 . However, recent experimental and theoretical studies show that this reaction mechanism, particularly on surfaces of non-model catalysts, is not fully understood [27][28][29][30][31][32] . The RWGS reaction is believed to follow either of two mechanisms: the direct dissociation of CO 2 to CO via a CO 2 -ion (pathway 1 in Fig.…”

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confidence: 99%

Unravelling structure sensitivity in CO2 hydrogenation over nickel

et al. 2018

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T he reduction of CO 2 emissions into the Earth's atmosphere is gaining legislative importance in view of its impact on the climate [1][2][3][4][5] . Reduction of the harmful effect of these emissions through reclamation of CO 2 is made attractive because CO 2 can be a zero-or even negative-cost carbon feedstock 6,7 . The conversion of renewably produced hydrogen and CO 2 into methane, or synthetic natural gas, over Ni is a solution that combines the potential to reduce CO 2 emissions with a direct answer to the temporal mismatch in renewable electricity production capacity and demand [8][9][10][11][12][13][14][15][16][17] . Chemical energy storage in the form of hydrogen production by electrolysis is a relatively mature technology; however, the required costly infrastructure, and inefficiencies in distribution and storage deem it inconvenient for large-scale application in the near future. Point-source CO 2 hydrogenation to methane represents an alternative approach with higher energy density. Furthermore, methane is more easily liquefied and can be stored safely in large quantities through infrastructures that already exist 18,19 . Power-to-gas (in this case methane) is thus actively considered as being capable of balancing electric grid stability, which will allow us to increase the renewable energy supply 20 .The search for fossil fuel alternatives, and application of a process such as that described above can arguably be achieved only with the help of advances in catalysis and the closely related field of nanomaterials. Continuous efforts in both fields have allowed us to make increasingly smaller and catalytically more active (metal) particles. However, it is already known that making progressively smaller supported catalyst particles does not necessarily linearly correspond to higher catalytic activity [21][22][23] . This phenomenon, where not all atoms in a supported metal catalyst have the same activity, is called structure sensitivity and is often attributed to the distinctly different chemistries on different lattice planes for π -bond activation in CO 2 , or σ -bond activation in, for example H 2 dissociation and C-H propagation 21,24 . The availability of stepped (less coordinated) versus terrace (more coordinated) sites on the surface of supported catalyst nanoparticles obviously changes with particle size, and atomic geometries become particularly interesting below 2 nm where, for example, π -bond activation is believed to not be able to occur 21 . While particle-size effects have been extensively studied for CO hydrogenation over Co 23,25 , the understanding of such structure sensitivity effects for these critical smaller metal particle sizes is lacking as sub-2-nm particles prove difficult to synthesize for first-row transition metals (Co, Fe and Ni). However, a particle-size effect for CO 2 hydrogenation is much less well established 26 .Here, we used a unique set of SiO 2 -supported Ni nanoparticles with diameters ranging from 1 to 7 nm in size, and show not only the existence of a distinct pa...

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Unravelling structure sensitivity in CO2 hydrogenation over nickel

et al. 2018

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“…Moreover, bio-syngas typically contains high amounts of CO 2 which is difficult to convert. 236,237 However, hydrotalcitelike materials are known to adsorb CO 2 and, hence, could potentially be used as combined catalytic and separation systems. Additionally, lignin often contains high amounts of sulphur originating from the separation process from biomass which, during gasification, leads to high concentrations of H 2 S and SO 2 .…”

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confidence: 99%

Recent advances on the utilization of layered double hydroxides (LDHs) and related heterogeneous catalysts in a lignocellulosic-feedstock biorefinery scheme

et al. 2017

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Layered double hydroxides (LDHs) and derived materials have been widely used as heterogeneous catalysts for different types of reactions either in gas or in liquid phase. Among these processes, the valorization/upgrading of lignocellulosic biomass and derived molecules have attracted enormous attention because it constitutes a pivotal axis in the transition from an economic model based on fossil resources to one based on renewable biomass resources with preference for biomass waste streams. Proof of this is the increasing amount of literature reports regarding the rational design and implementation of LDHs and related materials in catalytic processes such as: depolymerization, hydrogenation, selective oxidations, and C-C coupling reactions, among others, where biomass-derived compounds are used. The major aim of this contribution is to situate the most recent advances on the implementation of these types of catalysts into a lignocellulosic-feedstock biorefinery scheme, highlighting the versatility of LDHs and derived materials as multifunctional, tunable, cheap and easy to produce heterogeneous catalysts.

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“…The binding energies of the electron Ni 2p3/2 reported by different authors for NiO are between 854.2 and 854.6 eV; the shifts towards greater binding energies may result in the strong interactions produced by the formation of the solid solution. [35][36][37] The spectrum of the oxide calcined at 1000 °C exhibited shifts of +0.4 eV for the electron Ni 2 p 3/2 and +0.3 eV for the level Ni 2p1/2 , related with the formation of the spinel-like phase in which Ni has greater interactions in the crystalline structure. The CeO 2 spectrum was composed of different signals denominated v, v", v"' and u, u", u"' that describe the intensities of the photoelectrons 3d 5/2 and 3d 3/2 .…”

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confidence: 99%

Ce - promoted catalyst from hydrotalcites for CO2 reforming of methane: calcination temperature effect

Daza¹,

Moreno²,

Molina³

2012

Quím. Nova

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Recebido em 25/7/11; aceito em 11/2/12; publicado na web em 15/6/12Ce-promoted Ni-catalysts from hydrotalcites were obtained. The effect of calcination temperature on the chemical and physical properties of the catalysts was studied. Several techniques were used to determine the chemical and physical characteristics of oxides. The apparent activation energies of reduction were determined. Catalytic experiments at 48 L g -1 h -1 without pre-reduction in CO 2 reforming of methane were performed. The spinel-like phase in these oxides was only formed at 1000 °C. The reduction of Ni 2+ in the oxides was clearly affected by the calcination temperature which was correlated with catalytic performance. The catalyst calcined at 700 °C showed the greatest activity.

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Characterization of surface processes at the Ni-based catalyst during the methanation of biomass-derived synthesis gas: X-ray photoelectron spectroscopy (XPS)

Cited by 272 publications

References 45 publications

Unravelling structure sensitivity in CO2 hydrogenation over nickel

Unravelling structure sensitivity in CO2 hydrogenation over nickel

Recent advances on the utilization of layered double hydroxides (LDHs) and related heterogeneous catalysts in a lignocellulosic-feedstock biorefinery scheme

Ce - promoted catalyst from hydrotalcites for CO2 reforming of methane: calcination temperature effect

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