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Highly Efficient, Easily Recoverable, and Recyclable Re–SiO2–Fe3O4 Catalyst for the Fragmentation of Lignin

  • Madalina Tudorache
    Madalina Tudorache
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
  • Cristina Opris
    Cristina Opris
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
  • Bogdan Cojocaru
    Bogdan Cojocaru
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
  • Nicoleta G. Apostol
    Nicoleta G. Apostol
    National Institute of Materials Physics, Atomistilor 105b, Magurele-Ilfov 077125, Romania
  • Alina Tirsoaga
    Alina Tirsoaga
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
  • Simona M. Coman
    Simona M. Coman
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
  • Vasile I. Parvulescu*
    Vasile I. Parvulescu
    University of Bucharest, Department of Organic Chemistry, Biochemistry, and Catalysis, B-dul Regina Elisabeta 4-12, Bucharest 030018, Romania
    *E-mail: [email protected] (V.I.P.).
  • Bahir Duraki
    Bahir Duraki
    ETH Zurich, Institute for Chemical and Bioengineering, Vladimir-Prelog-Weg 1-5/10, Zurich 8093, Switzerland
    More by Bahir Duraki
  • Frank Krumeich
    Frank Krumeich
    ETH Zurich, Institute for Chemical and Bioengineering, Vladimir-Prelog-Weg 1-5/10, Zurich 8093, Switzerland
  • , and 
  • Jeroen A. van Bokhoven*
    Jeroen A. van Bokhoven
    ETH Zurich, Institute for Chemical and Bioengineering, Vladimir-Prelog-Weg 1-5/10, Zurich 8093, Switzerland
    Paul Scherrer Institute, Villigen 5232, Switzerland
    *E-mail: [email protected] (J.A.v.B.).
Cite this: ACS Sustainable Chem. Eng. 2018, 6, 8, 9606–9618
Publication Date (Web):June 19, 2018
https://doi.org/10.1021/acssuschemeng.7b04294
Copyright © 2018 American Chemical Society

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    Abstract

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    A series of Fe3O4@SiO2@Re catalysts were prepared by deposition of rhenium by means of the precipitation–deposition and impregnation procedures. Characterization of the catalysts confirmed that the deposition of silica protected the magnetite nanoparticles, resulting in a stable SiO2@Fe3O4 composite, which was not affected by the treatments during the further deposition of rhenium. Rhenium was silent in XRD over the range of concentrations, at which it was deposited. Furthermore, XPS detected rhenium, only in the impregnation series; this may confirm that dispersion was high. As expected, rhenium was not reduced to the metallic state and generated weakly acidic Brønsted-type centers as detected by NH3-TPD. H2-TPD and chemisorption experiments demonstrate the capacity of these catalysts to chemisorb hydrogen. In line with these properties, rhenium catalyzed both C–C hydrogenolysis and C–O hydrolysis in successive steps. The performance of these catalysts was checked for a series of lignins of different origin and by means of different separation procedures. A very important finding is that these catalysts were highly stable and easy to recover.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acssuschemeng.7b04294.

    • Characterization of the catalysts based on XPS, EDS, and H2-TPD, identification of lignin fragments based on HPLC-MS/MS and GPC analysis, pressure dependence of the lignin fragmentation, and TGA of lignins from different sources and information from 1H NMR spectra of lignins (PDF)

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    2. Kakasaheb Y. Nandiwale, Andrew M. Danby, Anand Ramanathan, Raghunath V. Chaudhari, Ali Hussain Motagamwala, James A. Dumesic, Bala Subramaniam. Enhanced Acid-Catalyzed Lignin Depolymerization in a Continuous Reactor with Stable Activity. ACS Sustainable Chemistry & Engineering 2020, 8 (10) , 4096-4106. https://doi.org/10.1021/acssuschemeng.9b06556
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    17. Antigoni Margellou, Konstantinos Triantafyllidis. Catalytic Transfer Hydrogenolysis Reactions for Lignin Valorization to Fuels and Chemicals. Catalysts 2019, 9 (1) , 43. https://doi.org/10.3390/catal9010043

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