Bimetallic Niobium-Based Catalysts Supported on SBA-15 for Hydrodeoxygenation of Anisole

Ballesteros‐Plata, Daniel; Barroso-Martín, Isabel; Cervantes, J.A. Medina; Maciel, Carmen; Huirache–Acuña, R.; Rodríguez‐Castellón, Enrique; Infantes‐Molina, Antonia

doi:10.1021/acs.iecr.1c02799

Cited by 10 publications

(4 citation statements)

References 62 publications

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“…Solids containing Pt over SBA-15 have been studied in m-cresol HDO [22] as well. Also, the effect of rather basic dopants (niobium in this case) on properties of SBA-15 Ni catalysts carrier was also studied in anisole HDO [23]. The effect of various metals (Nb, Ru, Pd, Pt) supported on SBA-16 was tested in phenol HDO [24] as well.…”

Section: Hdo Reaction Testmentioning

confidence: 99%

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

Morales-Hernández,

Escobar,

Pacheco-Sosa

et al. 2024

Preprint

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La integration (at various nominal contents) in SBA-15 prepared under acidic medium was intended from corresponding direct nitrate addition during mesoporous silica formation. Materials were impregnated with Pt (1.5 w%) and studied through several textural (N2 physisorption), structural (XRD, TG-DTG) and surface (FTIR, STEM-HAADF, SEM-EDS, NH3 and CO2 TPD) instrumental techniques. Pt-impregnated solids were tested in phenol hydrodeoxygenation (HDO, T=250 °C, 3.2 MPa, batch reactor, n-decane as solvent). Catalytic activity (in pseudo first order kinetic constant, kHDO basis) was related to Pt dispersion which was, however, not determined by nominal rare earth content. Determining actual composition of modified SBA-15 materials is crucial in reaching sound conclusions regarding their physicochemical properties, especially when La modifier is directly added during mesoporous matrices formation where efficient interaction among constituents could be difficult to get. Otherwise, results from some characterization techniques (N2 physisorption and FTIR, for instance) could be misleading and even contradictory. Indeed, extant modifier precursors when under SBA-15 synthesis conditions could affect the properties of prepared materials even though they were absent in obtained| formulations. Performing a simple compositional analysis could eliminate uncertainties regarding the role of various modifiers on characteristics of final catalysts. However, several groups have failed in doing so.

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Section: Hdo Reaction Testmentioning

confidence: 99%

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

Morales-Hernández,

Escobar,

Pacheco-Sosa

et al. 2024

Preprint

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“…and supports stood out among many catalyst types due to their high catalytic activity. , Supports were used to disperse and stabilize active metals, which also provided deoxidation catalytic sites (e.g., Brønsted/Lewis acids and oxygen vacancies) and even interacted with active metals to generate new catalytic sites . Molecular sieves (HZSM-5, SBA-15, MCM-41, etc.) and γ-Al 2 O 3 were common acid supports, widely used in the preparation of HDO catalysts.…”

Section: Introductionmentioning

confidence: 99%

Hydrodeoxygenation Performance of Lignin-Derived Phenolics to Cycloalkanes: Insights into the Crystal Structures of the Nb₂O₅ Support

Zhang,

Wu,

Hua

et al. 2023

Energy Fuels

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Hydrodeoxygenation (HDO) of lignin-derived phenolics is promising to produce high-value-added chemicals and liquid fuels. As a strong oxophilic support, Nb 2 O 5 maintains high catalytic activity for the deoxygenation of oxygen-rich reactants, while few studies have clarified the influence of crystal structures on reactivity. In this study, the Nb 2 O 5 supports with three crystal structures (pseudohexagonal-TT, orthorhombic-T, and monoclinic-H) were successfully prepared and used for the HDO of lignin-derived phenolics after loading bimetal Ni and Co. The structural properties and acidity of the supports and catalysts gradually deteriorated with the increase in calcination temperatures. The oxygen vacancy content and the interaction strength between supports and active metals followed the rule of Nb 2 O 5 -TT > Nb 2 O 5 -T > Nb 2 O 5 -H. In addition, oxygen vacancy content also had a volcanic relationship with the catalyst reduction times. Then, the catalytic activity of the catalysts was studied in the HDO reaction of guaiacol. The 10Ni−10Co/Nb 2 O 5 -TT (450 °C) catalyst exhibited the best catalytic performance with a complete conversion of reactant and a high cycloalkane selectivity of 98.6% under optimal conditions (250 °C, 3 MPa H 2 , and 3 h). More importantly, recycle tests indicated that it also had excellent stability. Moreover, other typical lignin-derived monomers and dimers were selected to test the reactant adaptability of the catalyst, and the selectivities of cycloalkanes also verged on the theoretical value. Therefore, the bifunctional catalyst composed of oxophilic Nb 2 O 5 -TT (450 °C) support and high-efficiency active metals possessed strong competitiveness in the HDO of lignin-derived phenolics.

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“…26,27 Finally, NiNb and Ni−ZrO 2 catalysts supported on SBA-15 silica also showed high activity in the HDO of anisole and guaiacol, respectively, with high selectivity toward CHA production. 28,29 The activity of the NiNb/SBA-15 was explained in terms of acidity, metal surface exposure, and reducibility as a function of the interaction between the phases present, 28 while the good activities and selectivities toward total deoxygenation obtained for the silica supported Ni−ZrO 2 catalysts were associated with the proximity between Ni and ZrO 2 particles when confined in the silica mesopores. 29 Summarizing the above results, it can be noted that, in general, bifunctional metal-acid catalysts show catalytic performance in HDO superior to that of their metallic counterparts supported on unmodified SBA-15 silica.…”

Section: Introductionmentioning

confidence: 99%

“…Gbadamasi et al found that Ni/Al-SBA-15 catalysts were promising for HDO of dibenzofuran (DBF) into hydrocarbons, observing a synergetic effect between Ni and the Al-SBA-15 support. Li et al tested the performance of Ni/Al-SBA-15 catalysts in eugenol HDO and observed that the activity and selectivity of the catalysts were affected by both the quantity of acid sites and the dispersion of nickel species. , Finally, NiNb and Ni–ZrO 2 catalysts supported on SBA-15 silica also showed high activity in the HDO of anisole and guaiacol, respectively, with high selectivity toward CHA production. , The activity of the NiNb/SBA-15 was explained in terms of acidity, metal surface exposure, and reducibility as a function of the interaction between the phases present, while the good activities and selectivities toward total deoxygenation obtained for the silica supported Ni–ZrO 2 catalysts were associated with the proximity between Ni and ZrO 2 particles when confined in the silica mesopores . Summarizing the above results, it can be noted that, in general, bifunctional metal-acid catalysts show catalytic performance in HDO superior to that of their metallic counterparts supported on unmodified SBA-15 silica.…”

Section: Introductionmentioning

confidence: 99%

Boosting the Hydrodeoxygenation Activity and Selectivity of Ni/(M)-SBA-15 Catalysts by Chemical Alteration of the Support

Calzada,

Pérez-Estrada,

Sánchez-Ramírez

et al. 2023

ACS Omega

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The influence of the acid sites in the hydrodeoxygenation of anisole performed over Ni catalysts supported on SBA-15 modified with metal oxides (Ni/M-SBA-15, M = Ti, Zr, Al, or Nb) was demonstrated. Catalysts were characterized by SEM–EDX, nitrogen physisorption, XRD, UV–visible DRS, TPR, TPD of ammonia, IR-Py, O2 chemisorption, and high-resolution transmission electron microscopy. The mesoporous structure and the hexagonal arrangement of the supports were maintained in the catalysts. Ni catalysts supported on modified M-SBA-15 exhibited a higher metal-support interaction, an increase in the acidity and, as a consequence, improved selectivity to cyclohexane. The deoxygenation reaction rate constants increased as Ni/SBA-15 < Ni/Ti-SBA-15 < Ni/Nb-SBA-15 < Ni/Zr-SBA-15 < Ni/Al-SBA-15, which is attributed to the increase in the amount and strength of acid sites, especially of the Brønsted ones, which promotes the cleavage of the C–O bond. It is also important to keep the metal/acid sites together to obtain high activity and selectivity to hydrodeoxygenated products.

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Bimetallic Niobium-Based Catalysts Supported on SBA-15 for Hydrodeoxygenation of Anisole

Cited by 10 publications

References 62 publications

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

Hydrodeoxygenation Performance of Lignin-Derived Phenolics to Cycloalkanes: Insights into the Crystal Structures of the Nb₂O₅ Support

Boosting the Hydrodeoxygenation Activity and Selectivity of Ni/(M)-SBA-15 Catalysts by Chemical Alteration of the Support

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Bimetallic Niobium-Based Catalysts Supported on SBA-15 for Hydrodeoxygenation of Anisole

Cited by 10 publications

References 62 publications

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

La-Modified SBA-15 Prepared by Direct Synthesis: Importance of Determining Actual Composition

Hydrodeoxygenation Performance of Lignin-Derived Phenolics to Cycloalkanes: Insights into the Crystal Structures of the Nb2O5 Support

Boosting the Hydrodeoxygenation Activity and Selectivity of Ni/(M)-SBA-15 Catalysts by Chemical Alteration of the Support

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Product

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Hydrodeoxygenation Performance of Lignin-Derived Phenolics to Cycloalkanes: Insights into the Crystal Structures of the Nb₂O₅ Support