Reforming Methane with CO2 over Hierarchical Porous Silica-Supported Nickel Catalysts Modified with Lanthanum Oxide

Hierarchical porous silica-supported nickel catalysts modified with different amounts of lanthanum (La) were synthesized via “one-pot” method using cetyltrimethylammonium bromide as template, urea as precipitant, and tetraethyl orthosilicate as silica source. Their catalytic performances were evalua...

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Published inInternational journal of energy research Vol. 2023; pp. 1 - 16
Main Authors Li, Bin, Yuan, Xiaoqing, Li, Lvyin, Li, Baitao, Wang, Xiujun
Format Journal Article
LanguageEnglish
Published Bognor Regis Hindawi 30.06.2023
Hindawi Limited
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Abstract Hierarchical porous silica-supported nickel catalysts modified with different amounts of lanthanum (La) were synthesized via “one-pot” method using cetyltrimethylammonium bromide as template, urea as precipitant, and tetraethyl orthosilicate as silica source. Their catalytic performances were evaluated in dry reforming with methane under different conditions (La loading, reaction temperature, and time on stream). The synthesized and spent catalysts were extensively characterized by ICP, physisorption, chemisorption, XRD, TPR, XPS, HAADF-TEM, TPH, Raman’s spectroscopy, and TG analysis. The impact of lanthanum amount on the catalytic performance, sintering, and carbon deposition was discussed. Compared to unmodified catalyst, La promoter induced the nickel nanoparticles with larger crystallite sizes and weakened the metal-support interaction as well as the formation of 1 : 1 nickel-phyllosilicate, leading to the metal sintering increasing in the order Ni1.5La/SiO2 < Ni3.0La/SiO2 < Ni4.5La/SiO2. The modified catalysts exhibited better carbon resistance, which was significantly enhanced with increasing La content. Despite this, the stability increased following the sequence of Ni3.0La/SiO2 < Ni4.5La/SiO2 < Ni1.5La/SiO2. Ni1.5La/SiO2 displayed the best stability at 750°C within 10 h stability test, with CH4 conversion dropping from 61.3 to 58.0%. The deactivation reason for Ni1.5La/SiO2 was mainly the carbon deposition, while that for Ni3.0La/SiO2 and Ni4.5La/SiO2 was the metal sintering. These results emphasized that the activity and stability in the NiLa/SiO2 catalysts for the dry reforming of methane depended on two important factors, the metal-support interaction and the particles size of nickel, providing the necessity and sufficiency to balance two attributes.
AbstractList Hierarchical porous silica-supported nickel catalysts modified with different amounts of lanthanum (La) were synthesized via “one-pot” method using cetyltrimethylammonium bromide as template, urea as precipitant, and tetraethyl orthosilicate as silica source. Their catalytic performances were evaluated in dry reforming with methane under different conditions (La loading, reaction temperature, and time on stream). The synthesized and spent catalysts were extensively characterized by ICP, physisorption, chemisorption, XRD, TPR, XPS, HAADF-TEM, TPH, Raman’s spectroscopy, and TG analysis. The impact of lanthanum amount on the catalytic performance, sintering, and carbon deposition was discussed. Compared to unmodified catalyst, La promoter induced the nickel nanoparticles with larger crystallite sizes and weakened the metal-support interaction as well as the formation of 1 : 1 nickel-phyllosilicate, leading to the metal sintering increasing in the order Ni1.5La/SiO2 < Ni3.0La/SiO2 < Ni4.5La/SiO2. The modified catalysts exhibited better carbon resistance, which was significantly enhanced with increasing La content. Despite this, the stability increased following the sequence of Ni3.0La/SiO2 < Ni4.5La/SiO2 < Ni1.5La/SiO2. Ni1.5La/SiO2 displayed the best stability at 750°C within 10 h stability test, with CH4 conversion dropping from 61.3 to 58.0%. The deactivation reason for Ni1.5La/SiO2 was mainly the carbon deposition, while that for Ni3.0La/SiO2 and Ni4.5La/SiO2 was the metal sintering. These results emphasized that the activity and stability in the NiLa/SiO2 catalysts for the dry reforming of methane depended on two important factors, the metal-support interaction and the particles size of nickel, providing the necessity and sufficiency to balance two attributes.
Author Li, Lvyin
Li, Baitao
Li, Bin
Wang, Xiujun
Yuan, Xiaoqing
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CitedBy_id crossref_primary_10_1016_j_enconman_2024_118568
crossref_primary_10_1021_acs_energyfuels_3c03421
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ContentType Journal Article
Copyright Copyright © 2023 Bin Li et al.
Copyright © 2023 Bin Li et al. This is an open access article distributed under the Creative Commons Attribution License (the “License”), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. https://creativecommons.org/licenses/by/4.0
Copyright_xml – notice: Copyright © 2023 Bin Li et al.
– notice: Copyright © 2023 Bin Li et al. This is an open access article distributed under the Creative Commons Attribution License (the “License”), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. https://creativecommons.org/licenses/by/4.0
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Snippet Hierarchical porous silica-supported nickel catalysts modified with different amounts of lanthanum (La) were synthesized via “one-pot” method using...
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SubjectTerms Adsorption
Analytical methods
Aqueous solutions
Carbon
Carbon dioxide
Catalysts
Cetyltrimethylammonium bromide
Chemical synthesis
Chemisorption
Crystallites
Crystals
Deactivation
Deposition
Gases
Heavy metals
Hydrogen
Impact analysis
Lanthanum
Lanthanum oxides
Metals
Methane
Nanoparticles
Nickel
Particle size
Reforming
Sensors
Silica
Silicon dioxide
Sintering
Sintering (powder metallurgy)
Spectroscopy
Stability
Stability tests
Synthesis gas
Tetraethoxysilane
Tetraethyl orthosilicate
Urea
X ray photoelectron spectroscopy
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Title Reforming Methane with CO2 over Hierarchical Porous Silica-Supported Nickel Catalysts Modified with Lanthanum Oxide
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