Dataset Information

Continuous selective deoxygenation of palm oil for renewable diesel production over Ni catalysts supported on Al₂O₃ and La₂O₃-Al₂O₃.

ABSTRACT: The present study provides, for the first time in the literature, a comparative assessment of the catalytic performance of Ni catalysts supported on γ-Al₂O₃ and γ-Al₂O₃ modified with La₂O₃, in a continuous flow trickle bed reactor, for the selective deoxygenation of palm oil. The catalysts were prepared via the wet impregnation method and were characterized, after calcination and/or reduction, by N₂ adsorption/desorption, XRD, NH₃-TPD, CO₂-TPD, H₂-TPR, H₂-TPD, XPS and TEM, and after the time-on-stream tests, by TGA, TPO, Raman and TEM. Catalytic experiments were performed between 300-400 °C, at a constant pressure (30 bar) and different LHSV (1.2-3.6 h^-1). The results show that the incorporation of La₂O₃ in the Al₂O₃ support increased the Ni surface atomic concentration (XPS), affected the nature and abundance of surface basicity (CO₂-TPD), and despite leading to a drop in surface acidity (NH₃-TPD), the Ni/LaAl catalyst presented a larger population of medium-strength acid sites. These characteristics helped promote the SDO process and prevented extended cracking and the formation of coke. Thus, higher triglyceride conversions and n-C₁₅ to n-C₁₈ hydrocarbon yields were achieved with the Ni/LaAl at lower reaction temperatures. Moreover, the Ni/LaAl catalyst was considerably more stable during 20 h of time-on-stream. Examination of the spent catalysts revealed that both carbon deposition and degree of graphitization of the surface coke, as well as, the extent of sintering were lower on the Ni/LaAl catalyst, explaining its excellent performance during time-on-stream.

SUBMITTER: Papageridis KN

PROVIDER: S-EPMC8695223 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Continuous selective deoxygenation of palm oil for renewable diesel production over Ni catalysts supported on Al2O3 and La2O3-Al2O3.

Papageridis Kyriakos N KN Charisiou Nikolaos D ND Douvartzides Savvas S Sebastian Victor V Hinder Steven J SJ Baker Mark A MA AlKhoori Ayesha A AA AlKhoori Sara I SI Polychronopoulou Kyriaki K Goula Maria A MA

RSC advances 20210224 15

The present study provides, for the first time in the literature, a comparative assessment of the catalytic performance of Ni catalysts supported on γ-Al2O3 and γ-Al2O3 modified with La2O3, in a continuous flow trickle bed reactor, for the selective deoxygenation of palm oil. The catalysts were prepared via the wet impregnation method and were characterized, after calcination and/or reduction, by N2 adsorption/de ...[more]

PMID: 35423403

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Project description:The influence of A- and/or B-site doping of Ruddlesden-Popper perovskite materials on the crystal structure, stability, and dry reforming of methane (DRM) reactivity of specific A2BO4 phases (A = La, Ba; B = Cu, Ni) has been evaluated by a combination of catalytic experiments, in situ X-ray diffraction, X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), and aberration-corrected electron microscopy. At room temperature, B-site doping of La2NiO4 with Cu stabilizes the orthorhombic structure (Fmmm) of the perovskite, while A-site doping with Ba yields a tetragonal space group (I4/mmm). We observed the orthorhombic-to-tetragonal transformation above 170 °C for La2Ni0.9Cu0.1O4 and La2Ni0.8Cu0.2O4, slightly higher than for undoped La2NiO4. Loss of oxygen in interstitial sites of the tetragonal structure causes further structure transformations for all samples before decomposition in the temperature range of 400 °C-600 °C. Controlled in situ decomposition of the parent or A/B-site doped perovskite structures in a DRM mixture (CH4:CO2 = 1:1) in all cases yields an active phase consisting of exsolved nanocrystalline metallic Ni particles in contact with hexagonal La2O3 and a mixture of (oxy)carbonate phases (hexagonal and monoclinic La2O2CO3, BaCO3). Differences in the catalytic activity evolve because of (i) the in situ formation of Ni-Cu alloy phases (in a composition of >7:1 = Ni:Cu) for La2Ni0.9Cu0.1O4, La2Ni0.8Cu0.2O4, and La1.8Ba0.2Ni0.9Cu0.1O4, (ii) the resulting Ni particle size and amount of exsolved Ni, and (iii) the inherently different reactivity of the present (oxy)carbonate species. Based on the onset temperature of catalytic DRM activity, the latter decreases in the order of La2Ni0.9Cu0.1O4 ∼ La2Ni0.8Cu0.2O4 ≥ La1.8Ba0.2Ni0.9Cu0.1O4 > La2NiO4 > La1.8Ba0.2NiO4. Simple A-site doped La1.8Ba0.2NiO4 is essentially DRM inactive. The Ni particle size can be efficiently influenced by introducing Ba into the A site of the respective Ruddlesden-Popper structures, allowing us to control the Ni particle size between 10 nm and 30 nm both for simple B-site and A-site doped structures. Hence, it is possible to steer both the extent of the metal-oxide-(oxy)carbonate interface and its chemical composition and reactivity. Counteracting the limitation of the larger Ni particle size, the activity can, however, be improved by additional Cu-doping on the B-site, enhancing the carbon reactivity. Exemplified for the La2NiO4 based systems, we show how the delicate antagonistic balance of doping with Cu (rendering the La2NiO4 structure less stable and suppressing coking by efficiently removing surface carbon) and Ba (rendering the La2NiO4 structure more stable and forming unreactive surface or interfacial carbonates) can be used to tailor prospective DRM-active catalysts.

Dataset Information

Continuous selective deoxygenation of palm oil for renewable diesel production over Ni catalysts supported on Al₂O₃ and La₂O₃-Al₂O₃.

Publications

Continuous selective deoxygenation of palm oil for renewable diesel production over Ni catalysts supported on Al<sub>2</sub>O<sub>3</sub> and La<sub>2</sub>O<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub>.

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