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High Recyclability Magnetic Iron Oxide‐Supported Ruthenium Nanocatalyst for H2 Release from Ammonia‐Borane Solvolysis

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Ru@Fe3O4 nanocomposites displayed high recyclability over ten runs for the production at room temperature (25 °C) of three equiv. dihydrogen H2 from ammonia-borane H3NBH3, either from hydrolysis or methanolysis fast reactions. The nanocatalyst maintains consistent turnover frequencies while is operated very simple magnetic recovering without any further treatment.


Abstract

We report the high capacity of recycling of a technologically simple, easily recoverable, Ru@Fe3O4 magnetic nanocatalyst, efficient in the release of H2 from ammonia-borane (AB) solvolysis, using H2O or methanol at room temperature (25 °C). The initially oxidized Ru small nanoparticles (2–4 nm) are well-dispersed on an iron oxide support (i. e. super paramagnetic iron oxide of spinel structure, SPIO, as aggregates of 20 nm to a few μm). As nanocatalyst, this composite achieved short-time (<10 min) AB full hydrolysis (3 equiv. H2, no NH3, [AB]=0.1 mol L−1) with a turnover frequency (TOF) of ca 20 min−1 (86 min−1 at 50 °C). The post-catalysis characterization of the composite showed the formation of well-defined crystalline hcp Ru(0) dispersed on the SPIO. The activity for full H2 release from AB is conserved over ten cycles, which is among the most effective recycling processes reported to date (a magnetic recycling is achieved in <2 min). Pleasingly, an even superior activity was found in the more challenging AB methanolysis, with a TOF up to ca 30 min−1 for full H2 release, achieved in a recycling process repeated over 8 cycles.

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