Al2O3 nanofibers prepared from aluminum Di(sec-butoxide)acetoacetic ester chelate exhibits high surface area and acidity

M. A. Rodriguez-Olguin; H. Atia; M. Bosco; A. Aguirre; R. Eckelt; E. D. Asuquo; M. Vandichel; J. G.E. Gardeniers; A. Susarrey-Arce

doi:10.1016/j.jcat.2021.11.019

Al₂O₃ nanofibers prepared from aluminum Di(sec-butoxide)acetoacetic ester chelate exhibits high surface area and acidity

M. A. Rodriguez-Olguin, H. Atia, M. Bosco, A. Aguirre, R. Eckelt, E. D. Asuquo, M. Vandichel^*, J. G.E. Gardeniers, A. Susarrey-Arce

^*Corresponding author for this work

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Abstract

Alumina (Al₂O₃) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al₂O₃ play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al₂O₃ nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m² determined with temperature-programmed desorption of ammonia (NH₃-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH₃) on crystalline γ-Al₂O₃. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH₃. The computational results are compared with NH₃-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.

Original language	English
Pages (from-to)	520-533
Number of pages	14
Journal	Journal of catalysis
Volume	405
Early online date	22 Nov 2021
DOIs	https://doi.org/10.1016/j.jcat.2021.11.019
Publication status	Published - Jan 2022

Keywords

Acidity
DFT
Electrospinning
Nanofibers
NH-TPD
Porous Alumina

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@article{7910e6c3b8d944baaf4b9e61f6ed5efd,

title = "Al2O3 nanofibers prepared from aluminum Di(sec-butoxide)acetoacetic ester chelate exhibits high surface area and acidity",

abstract = "Alumina (Al2O3) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al2O3 play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al2O3 nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m2 determined with temperature-programmed desorption of ammonia (NH3-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH3) on crystalline γ-Al2O3. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH3. The computational results are compared with NH3-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.",

keywords = "Acidity, DFT, Electrospinning, Nanofibers, NH-TPD, Porous Alumina",

author = "Rodriguez-Olguin, {M. A.} and H. Atia and M. Bosco and A. Aguirre and R. Eckelt and Asuquo, {E. D.} and M. Vandichel and Gardeniers, {J. G.E.} and A. Susarrey-Arce",

note = "Funding Information: The authors thank Stephan Bartling (Leibniz Institute for Catalysis), Regina Lange and Ingo Barke (University of Rostock, Institute of Physics), Frank Morssinkhof (Membrane Science & Technology Cluster, University of Twente), and Mark Smithers (MESA + Institute, University of Twente) for their support. M.V. wishes to acknowledge the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. The research leading to the results in this report has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742004). Funding Information: The authors thank Stephan Bartling (Leibniz Institute for Catalysis), Regina Lange and Ingo Barke (University of Rostock, Institute of Physics), Frank Morssinkhof (Membrane Science & Technology Cluster, University of Twente), and Mark Smithers (MESA + Institute, University of Twente) for their support. M.V. wishes to acknowledge the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. The research leading to the results in this report has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742004). Publisher Copyright: {\textcopyright} 2021 The Author(s)",

year = "2022",

month = jan,

doi = "10.1016/j.jcat.2021.11.019",

language = "English",

volume = "405",

pages = "520--533",

journal = "Journal of catalysis",

issn = "0021-9517",

publisher = "Elsevier",

}

TY - JOUR

T1 - Al2O3 nanofibers prepared from aluminum Di(sec-butoxide)acetoacetic ester chelate exhibits high surface area and acidity

AU - Rodriguez-Olguin, M. A.

AU - Atia, H.

AU - Bosco, M.

AU - Aguirre, A.

AU - Eckelt, R.

AU - Asuquo, E. D.

AU - Vandichel, M.

AU - Gardeniers, J. G.E.

AU - Susarrey-Arce, A.

N1 - Funding Information: The authors thank Stephan Bartling (Leibniz Institute for Catalysis), Regina Lange and Ingo Barke (University of Rostock, Institute of Physics), Frank Morssinkhof (Membrane Science & Technology Cluster, University of Twente), and Mark Smithers (MESA + Institute, University of Twente) for their support. M.V. wishes to acknowledge the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. The research leading to the results in this report has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742004). Funding Information: The authors thank Stephan Bartling (Leibniz Institute for Catalysis), Regina Lange and Ingo Barke (University of Rostock, Institute of Physics), Frank Morssinkhof (Membrane Science & Technology Cluster, University of Twente), and Mark Smithers (MESA + Institute, University of Twente) for their support. M.V. wishes to acknowledge the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. The research leading to the results in this report has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742004). Publisher Copyright: © 2021 The Author(s)

PY - 2022/1

Y1 - 2022/1

N2 - Alumina (Al2O3) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al2O3 play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al2O3 nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m2 determined with temperature-programmed desorption of ammonia (NH3-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH3) on crystalline γ-Al2O3. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH3. The computational results are compared with NH3-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.

AB - Alumina (Al2O3) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al2O3 play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al2O3 nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m2 determined with temperature-programmed desorption of ammonia (NH3-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH3) on crystalline γ-Al2O3. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH3. The computational results are compared with NH3-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.

KW - Acidity

KW - DFT

KW - Electrospinning

KW - Nanofibers

KW - NH-TPD

KW - Porous Alumina

UR - http://www.scopus.com/inward/record.url?scp=85120798110&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2021.11.019

DO - 10.1016/j.jcat.2021.11.019

M3 - Article

AN - SCOPUS:85120798110

SN - 0021-9517

VL - 405

SP - 520

EP - 533

JO - Journal of catalysis

JF - Journal of catalysis

ER -

Al₂O₃ nanofibers prepared from aluminum Di(sec-butoxide)acetoacetic ester chelate exhibits high surface area and acidity

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Keywords

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