An in depth investigation of deactivation through carbon formation during the biogas dry reforming reaction for Ni supported on modified with CeO2 and La2O3 zirconia catalysts

Charisiou, Nikolaos D.; Siakavelas, Georgios I.; Tzounis, Lazaros; Sebastián, Víctor; Μοnzόn, A.; Baker, Mark; Hinder, Steven J.; Polychronopoulou, Kyriaki; Yentekakis, I.V.; Goula, Maria A.

doi:10.1016/j.ijhydene.2018.08.074

Cited by 184 publications

(99 citation statements)

References 95 publications

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“…A number of reports suggest that a higher initial conversion rate than noble metal-based systems can be achieved, with the exception of Rh [40]. However, the major challenge that needs to be overcome for the industrial application of Ni catalysts is deactivation due to carbon deposition and metal particle sintering [41,42].…”

Section: Introductionmentioning

confidence: 99%

“…If the metal particle is encapsulated within the filament, then a total loss in activity is to be expected. However, even if this is not the case-as the catalytic particle may be located at the tip of the filament growth and still be available to the reactants-filament formation is thought to have catastrophic consequences, as it can lead to the plugging of the reactor (due to the expansion of the catalyst bed), the breakage of the catalytic particles (due to the blockage of the porosity), an increased pressure drop, and even to the creation of hot spots that can cause the failure of the reactor [25,[41][42][43]. Filament formation also causes difficulties to the regeneration of the catalytic system, as the contact between the metal and the support is lost [42].…”

Section: Introductionmentioning

confidence: 99%

“…This necessitates targeted research and analysis of the surface of spent catalysts in an effort to obtain a better understanding of the effect that different carbon allotropes have on the deactivation mechanism. In previous BDR related works carried out by our group, the use of promoters on Ni/Al (La 2 O 3 [45]) and Ni/Zr (La 2 O 3 and CeO 2 [42]) systems, and their effect on carbon deposition and metal particle sintering, as a function of the reaction temperature and/or weight hour space velocity (WHSV) was investigated. For the work presented herein, the authors decided to provide a comparative examination of the carbonaceous deposits on un-promoted nickel catalysts based on some of the most widely used supporting materials, i.e., Al 2 O 3 , ZrO 2 and SiO 2 .…”

Section: Introductionmentioning

confidence: 99%

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The Relationship between Reaction Temperature and Carbon Deposition on Nickel Catalysts Based on Al2O3, ZrO2 or SiO2 Supports during the Biogas Dry Reforming Reaction

et al. 2019

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The tackling of carbon deposition during the dry reforming of biogas (BDR) necessitates research of the surface of spent catalysts in an effort to obtain a better understanding of the effect that different carbon allotropes have on the deactivation mechanism and correlation of their formation with catalytic properties. The work presented herein provides a comparative assessment of catalytic stability in relation to carbon deposition and metal particle sintering on un-promoted Ni/Al2O3, Ni/ZrO2 and Ni/SiO2 catalysts for different reaction temperatures. The spent catalysts were examined using thermogravimetric analysis (TGA), Raman spectroscopy, high angle annular dark field scanning transmission electron microscopy (STEM-HAADF) and X-ray photoelectron spectroscopy (XPS). The results show that the formation and nature of carbonaceous deposits on catalytic surfaces (and thus catalytic stability) depend on the interplay of a number of crucial parameters such as metal support interaction, acidity/basicity characteristics, O2– lability and active phase particle size. When a catalytic system possesses only some of these beneficial characteristics, then competition with adverse effects may overshadow any potential benefits.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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The Relationship between Reaction Temperature and Carbon Deposition on Nickel Catalysts Based on Al2O3, ZrO2 or SiO2 Supports during the Biogas Dry Reforming Reaction

et al. 2019

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“…A large number of studies have shown that Ni-based catalysts can result in high activity and stability in DRM [18][19][20][21][22][23][24][25][26][27].…”

Section: Introductionmentioning

confidence: 99%

Effect of low loading of yttrium on Ni-based layered double hydroxides in CO2 reforming of CH4

Świrk

Motak

Grzybek

et al. 2018

Reac Kinet Mech Cat

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Ni/Al/Mg layered double hydroxides (LDHs) modified with low loading of yttrium (0.2 and 0.4 wt%) were used in dry reforming of methane at 700 °C. Physicochemical characterization, such as: X-ray fluorescence, N2 sorption, X-ray diffraction, temperature programmed reduction in H2, temperature programmed desorption of CO2, H2 chemisorption, thermogravimetry analysis coupled by mass spectrometry and Raman spectroscopy, showed that the introduction of low loadings of yttrium lead to a smaller Niº crystallite size, a decrease in reducibility of the nickel, and a decreased number of basic sites in the modified Ni/LDHs catalysts. The doping with 0.4 wt% of Y improves catalytic activity resulting in higher CH4 and CO2 conversions at 700 °C, i.e. ca. 84 % and ca. 87 %, respectively with no clear deactivation observed after 5 h run. The increase in CO2 conversion and a decrease of H2/CO ratio indicates that side reactions occurs during DRM.

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“…The binding energy of the main Ni 2p peak may be found at 855.6 eV, while the rest of the peaks and satellites are visible at other binding energies. It is apparent from the shape of the main peak (Ni 2p 3/2 ) that it is the combination of Ni 0 and Ni 2+ /Ni 3+ oxides [32,33]. The Ni 2p spectra of Ni/La-Zr and Ni-Ce/Zr catalysts becomes complicated due to the overlapping of La 3d, Ce 3d, and La MNN Auger peaks.…”

Section: Physicochemical Features Of the Ceria Promoted Ni/x-zr (X=0mentioning

confidence: 99%

Catalytic Behaviour of Ce-Doped Ni Systems Supported on Stabilized Zirconia under Dry Reforming Conditions

et al. 2019

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Ni supported on bare and modified ZrO2 samples were synthesized using the incipient wet impregnation method. The t-ZrO2 phase was stabilized by incorporation of La2O3 into ZrO2. Moreover, the influence of CeO2-doping on the physico-chemical and catalytic properties under CO2 reforming conditions was probed. The characterization data of the investigated catalysts were obtained by using XRD, CO2/H2-TPD, BET, TPR, TPO, TGA, XPS and TEM characterization techniques. In the pristine Ni/Zr catalyst, the t-ZrO2 phase transformed into the monoclinic phase. However, upon support modification by La2O3, significant effects on the physicochemical properties were observed due to the monoclinic-to-tetragonal ZrO2 phase transformation also affecting the catalytic activity. As a result, superior activity on the La2O3 modified Ni/Zr catalyst was achieved, while no relevant change in the surface properties and activity of the catalysts was detected after doping by CeO2. The peculiar behavior of the Ni/La-ZrO2 sample was related to higher dispersion of the active phase, with a more pronounced stabilization of the t-ZrO2 phase.

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An in depth investigation of deactivation through carbon formation during the biogas dry reforming reaction for Ni supported on modified with CeO2 and La2O3 zirconia catalysts

Cited by 184 publications

References 95 publications

The Relationship between Reaction Temperature and Carbon Deposition on Nickel Catalysts Based on Al2O3, ZrO2 or SiO2 Supports during the Biogas Dry Reforming Reaction

The Relationship between Reaction Temperature and Carbon Deposition on Nickel Catalysts Based on Al2O3, ZrO2 or SiO2 Supports during the Biogas Dry Reforming Reaction

Effect of low loading of yttrium on Ni-based layered double hydroxides in CO2 reforming of CH4

Catalytic Behaviour of Ce-Doped Ni Systems Supported on Stabilized Zirconia under Dry Reforming Conditions

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