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Rhodium nanoparticles supported on covalent triazine-based frameworks as re-usable catalyst for benzene hydrogenation and hydrogen evolution reaction

Abstract

Metal nanoparticles (M-NPs) of ruthenium, rhodium, iridium and platinum were synthesized and supported on covalent triazine-based framework from 1,4 dicyanobenzene (CTF-1) by rapid microwave induced decomposition of their binary metal(0) carbonyls for Ru, Rh and Ir or Pt(acac)2 in the presence of CTF-1 in the ionic liquid (IL) 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BMIm][NTf2]) or in propylene carbonate (PC). (High-resolution) transmission electron microscopy, (HR-)TEM showed the formation of M-NPs on CTF-1 with, e.g., size distributions of 3.0(± 0.5) nm for Ru@CTF-1 synthesized in [BMIm][NTf2] and 2(± 1) nm for Rh@CTF 1 synthesized in PC. The crystalline phases of the M-NPs and the absence of significant impurities were verified by powder X-ray diffraction (PXRD) and selected area electron diffraction (SAED). The metal content of the M@CTF-1 composites was determined by flame atomic absorption spectroscopy (AAS) between 3 to 12 wt.-%. The Rh@CTF-1 composite nanomaterial proved to be a highly active (~31000 mol cyclohexane x (mol Rh)‒1 x h‒1) heterogeneous catalyst for the hydrogenation of benzene to cyclohexane under mild (10 bar H2, 70 °C) and solvent-free conditions with over 99 % conversion. The catalyst could be re-used for at least ten consecutive hydrogenation reactions. Additionally, Rh@CTF-1 is an active electrocatalyst for the hydrogen evolution reaction (HER) with an operating potential of −58 mV, while Pt@CTF-1 and commercial Pt/C shows a more negative operating potential of −111 and –77 mV. Also the onset potential of −31 mV for Rh@CTF-1 is much more positive than that of Pt@CTF-1 (–44 mV) and commercial Pt/C (−38 mV).

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Publication details

The article was received on 22 Dec 2018, accepted on 14 Apr 2019 and first published on 15 Apr 2019


Article type: Paper
DOI: 10.1039/C8TA12353E
Citation: J. Mater. Chem. A, 2019, Accepted Manuscript

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    Rhodium nanoparticles supported on covalent triazine-based frameworks as re-usable catalyst for benzene hydrogenation and hydrogen evolution reaction

    M. Siebels, C. Schlüsener, J. Thomas, Y. Xiao, X. Yang and C. Janiak, J. Mater. Chem. A, 2019, Accepted Manuscript , DOI: 10.1039/C8TA12353E

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