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

Siebels, Marvin; Schlüsener, Carsten; Thomas, Jörg; Xiao, Yu-Xuan; Yang, Xiao-Yu; Janiak, Christoph

doi:10.1039/c8ta12353e

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

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Thomas, Jörg
Structure and Nano-/ Micromechanics of Materials, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Citation

Siebels, M., Schlüsener, C., Thomas, J., Xiao, Y.-X., Yang, X.-Y., & Janiak, C. (2019). Rhodium nanoparticles supported on covalent triazine-based frameworks as re-usable catalyst for benzene hydrogenation and hydrogen evolution reaction. Journal of Materials Chemistry A, 7(19), 11934-11943. doi:10.1039/c8ta12353e.

Cite as: https://hdl.handle.net/21.11116/0000-0009-738F-5

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) to be between 3 and 12 wt. The Rh@CTF-1 composite nanomaterial proved to be a highly active (∼31 000 mol cyclohexane per (mol Rh) per h) 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). This journal is © The Royal Society of Chemistry.