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Ethylene polymerization and hydrodechlorination of 1,2-dichloroethane mediated by nickel(II) covalently anchored to silica xerogels

  • Original Paper: Nano- and macroporous materials (aerogels, xerogels, cryogels, etc.)
  • Published:
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Abstract

Ni/SiO2 cogelled xerogel catalysts have been prepared in ethanol containing nickel acetylacetonate, tetraethoxysilane (TEOS), an aqueous ammonia solution of 0.54 mol L−1 and either a commercial sylilated ligand, 3-(2-aminoethyl)aminopropyltrimethoxysilane (EDAPMS), or a home-made new silylated pyrazolypyridine ligands, respectively 2-[4-[3-(trimethoxysilyl)propyl]-3,5-dimethyl-1H-pyrazol-1-yl]pyridine (MS-PzPy) and 2-[4-[3-(trimethoxysilyl)propyl]-3,5-dimethyl-1H-pyrazol-1-yl]-6-methylpyridine (MS-PzPyMe), able to form a chelate with a metal ion such as Ni2+. All samples form homogeneous and very highly dispersed Ni/SiO2 cogelled xerogel catalysts. The resulting catalysts are composed of nickel nanoparticles with a diameter of about 2.8 nm, located inside primary silica particles exhibiting a monodisperse microporous distribution. The silylated organic ligand has a strong influence on the textural properties of cogelled xerogel catalysts, both before and after calcination and reduction steps. Changing the nature of the silylated ligand permits tailoring textural properties such as pore volume, pore size and surface area. Homogenous nickel complexes synthesized from pyrazolylpyridine derivatives are inactive for ethylene polymerization. In opposite, heterogenous nickel-based catalysts onto silica xerogel synthesized from pyrazolylpyridine derivatives bearing a tethered trialkoxysilyl group allow increasing ethylene polymerization activity. Although nickel nanoparticles are located inside the silica crystallites, their complete accessibility, via the micropore network, has been shown. For 1,2-dichloroethane hydrodechlorination over Ni/SiO2 catalysts, the conversion of 1,2-dichloroethane is high at the temperature of 350 °C and mainly ethane is produced.

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Acknowledgements

SDL. is grateful to the Belgian “Fonds de la Recherche Scientifique—Fonds National de la Recherche Scientifique (F.R.S.-F.N.R.S)” for her research associate position. The authors acknowledge the Ministère de la Région Wallonne Direction Générale des Technologies, de la Recherche et de l’Energie (DG06) and the Fonds de Recherche Fondamentale Collective and the Ministère de la Communauté Française (Action de Recherche Concertée no. 00-05-265) for financial supports.

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Authors and Affiliations

  1. Department of Chemical Engineering—Nanomaterials, Catalysis and Electrochemistry, B6a, University of Liège, Liège, B-4000, Belgium

    Julien G. Mahy, Vincent Claude & Stéphanie D. Lambert

  2. Laboratory of Macromolecular Chemistry and Organic Catalysis (CERM), B6a, University of Liège, Liège, B-4000, Belgium

    Luigi Sacco

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  1. Julien G. Mahy
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  2. Vincent Claude
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  3. Luigi Sacco
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  4. Stéphanie D. Lambert
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Correspondence to Stéphanie D. Lambert.

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Mahy, J.G., Claude, V., Sacco, L. et al. Ethylene polymerization and hydrodechlorination of 1,2-dichloroethane mediated by nickel(II) covalently anchored to silica xerogels. J Sol-Gel Sci Technol 81, 59–68 (2017). https://doi.org/10.1007/s10971-016-4272-0

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