A new pathway for heterogenisation of molecular catalysts by non-covalent interactions with carbon nanoreactors
Schröder, Martin (2014) A new pathway for heterogenisation of molecular catalysts by non-covalent interactions with carbon nanoreactors. Chemistry of Materials, 26 (22). pp. 6461-6466. ISSN 0897-4756
Official URL: http://pubs.acs.org/doi/abs/10.1021/cm502986d
A novel approach to heterogenisation of catalytic molecules is demonstrated using the nanoscale graphitic step-edges inside hollow graphitised carbon nanofibres (GNFs). The presence of the fullerene C60 moiety within a fullerene-salen CuII complex is essential for anchoring the catalyst within the GNF nanoreactor as demonstrated by comparison with the analogous catalyst complex without the fullerene group. The presence of the catalyst at the step-edges of the GNFs is confirmed by high resolution transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDX) with UV/Vis spectroscopy demonstrating only negligible (c.a. 3 %) desorption of the fullerene-salen CuII complex from the GNFs into solution under typical reaction conditions. The catalyst immobilised in GNFs shows good catalytic activity and selectivity towards styrene epoxidation, comparable to the analogous catalyst in solution. Moreover, the fullerene-salen CuII complex in GNFs demonstrates excellent stability and recyclability as it can be readily separated from the reaction mixture and employed in multiple reaction cycles with minimal loss of activity, which is highly advantageous compared to catalysts not stabilised by the graphitic step-edges that desorb rapidly from GNFs.
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