Sulphur poisoning of Ni catalysts in the SNG production from biomass: A TPO/XPS/XAS study

Struis, Rudolf Paul Wilhelm Jozef; Schildhauer, Tilman J.; Czekaj, Izabela; Janousch, M.; Biollaz, Serge M.A.; Ludwig, Christian

doi:10.1016/j.apcata.2009.04.030

Cited by 111 publications

(76 citation statements)

References 36 publications

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“…However, so far, there are no spectroscopic experiments made operando under realistic SOFC anode operation conditions with oxide ion flux from cathode to anode or under electrochemical polarization of the anode. And, when it comes to study of the nickelesulphur chemistry in detail, we realize that Ni K-edge XAS is less informative than S K-edge XAS [40], particularly because the sulphur K-edge spectra provide a very detailed picture about the molecular structure of the various sulphur species being formed on the anode during typical SOFC operation. Therefore, the present study demonstrates a novel powerful approach with sulphursensitive XAS under operando SOFC conditions for studying processes during sulphur poisoning of an IT-SOFC dedicated electrochemical element.…”

Section: Motivation and Goalmentioning

confidence: 99%

“…4 ), respectively (cf. [40] and references cited). Instead, performing PCA with WINXAS [47] was inconclusive, because none of the calculated statistical indicators passed through a minimum value for increasing number of PCs assumed.…”

Section: Relevant Number Of Sulphur Constituents With the Operando Spmentioning

confidence: 99%

“…The combined principal component analysisetarget transformationelinear combination fitting (PCAeTTeLCF) approach has been applied and described by different authors (cf. [40,45]). The goal of PCA is to find a transformation matrix allowing reproducing a set of data by a minimal number of relevant, independent PCs using Eigenvalue analysis.…”

Section: Sulphur Speciation With the Operando-recorded Xanes Spectramentioning

confidence: 99%

“…discussion and references in Ref. [40]). But, for mixtures, the "after peak" and white-line positions induced by different sulphur forms may coincide (overlap) with each other.…”

Section: Relevant Number Of Sulphur Constituents With the Operando Spmentioning

confidence: 99%

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Redox dynamics of sulphur with Ni/GDC anode during SOFC operation at mid- and low-range temperatures: An operando S K-edge XANES study

Nurk

Huthwelker

Braun

et al. 2013

Journal of Power Sources

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h i g h l i g h t s g r a p h i c a l a b s t r a c tAn operando SOFC anode S-poisoning XAS experiment at 550 C to 250 C was performed. S K-edge XANES spectral information at Ni/GDC outer surface was collected.Intermediates with different sulphur oxidation states (6þ, 4þ, 0, 2À) were observed. Proportion of oxidation states changed as a function of temperature. Differences between TD calculations and XAS information were observed and discussed. a r t i c l e i n f o a b s t r a c t Sulphur poisoning of nickelebased solid oxide fuel cell (SOFC) anode catalysts is a well-documented shortcoming, but not yet fully understood. Here, a novel experiment is demonstrated to obtain spectroscopic information at operando conditions, in particular the molecular structure of sulphur species in the sulphur K-shell X-ray absorption near edge structure (XANES) region for a SOFC anode under realistic operando conditions, thus, with the flux of O 2À from cathode to anode. Cooling from T ¼ 550 C stepwise down to 250 C, 5 ppm H 2 S/H 2 reacting with Ni-gadolinium doped ceria (GDC) anode resulted in several sulphur species in different oxidation states (6þ, 4þ, 0, À2) and in amounts being at a minimum at high temperature. According to sulphur speciation analysis, the species could either relate to eSO 4 2À or SO 3 (g), eSO 3 2À or SO 2 (g), S 2 (g) or surface-adsorbed S atoms, and, Ni or Ce sulphides, respectively. The coexistence of different sulphur oxidation states as a function of temperature was analysed in the context of thermodynamic equilibrium calculations. Deviations between experimental results and calculations are most likely due to limitations in the speed of some intermediate oxidation steps as well as due to differences between stoichiometric CeO 2 used in calculations and partially reduced Ce 0.9 Gd 0.1 O 2Àd .

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Section: Motivation and Goalmentioning

confidence: 99%

Section: Relevant Number Of Sulphur Constituents With the Operando Spmentioning

confidence: 99%

Section: Sulphur Speciation With the Operando-recorded Xanes Spectramentioning

confidence: 99%

“…discussion and references in Ref. [40]). But, for mixtures, the "after peak" and white-line positions induced by different sulphur forms may coincide (overlap) with each other.…”

Section: Relevant Number Of Sulphur Constituents With the Operando Spmentioning

confidence: 99%

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Redox dynamics of sulphur with Ni/GDC anode during SOFC operation at mid- and low-range temperatures: An operando S K-edge XANES study

Nurk

Huthwelker

Braun

et al. 2013

Journal of Power Sources

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“…The main processes are deposition of carbon [15], formation of nickel tetracarbonyl (Ni(CO) 4 ) at low temperatures (< 230°C) [16], sintering of nickel particles at high temperatures (> 600°C) [17], and poisoning by chemisorption of sulfur compounds [18].…”

Section: Reactions and Catalystsmentioning

confidence: 99%

Low‐Temperature CO Methanation in Oil‐Tempered Plate Reactors by Optimization of Catalyst Activation Conditions

et al. 2017

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Ni-catalyzed methanation has been discovered more than 100 years ago. Since then, many applications based on syngas -from coal or biomass -for the production of synthetic natural gas (SNG) have been established. Nevertheless, methanation still bears great potential for optimization. Especially for decentralized, biomass-based applications, decreased methanation temperatures and pressures are expected to lower the costs of the overall process. Consequently, it is necessary to obtain a catalyst that is highly active under such reduced reaction conditions. This objective was successfully reached by a systematic variation of reduction temperature, pressure, and hydrogen concentration under the aspects of the design of experiment within the catalyst activation process.

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Methanation for Synthetic Natural Gas Production – Chemical Reaction Engineering Aspects

Schildhauer¹

2016

Synthetic Natural Gas From Coal, Dry Biomass, and Power‐to‐Gas Applications

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Sulphur poisoning of Ni catalysts in the SNG production from biomass: A TPO/XPS/XAS study

Cited by 111 publications

References 36 publications

Redox dynamics of sulphur with Ni/GDC anode during SOFC operation at mid- and low-range temperatures: An operando S K-edge XANES study

Redox dynamics of sulphur with Ni/GDC anode during SOFC operation at mid- and low-range temperatures: An operando S K-edge XANES study

Low‐Temperature CO Methanation in Oil‐Tempered Plate Reactors by Optimization of Catalyst Activation Conditions

Methanation for Synthetic Natural Gas Production – Chemical Reaction Engineering Aspects

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