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Reversible hydrogenation and dehydrogenation of N-ethylcarbazole over bimetallic Pd-Rh catalyst for hydrogen storage

Highlights•Develop a bimetallic Pd-Rh catalyst for both hydrogenation and dehydrogenation reaction.•The catalyst structure that Rh clusters isolated by the surrounding Pd atoms was proved by various ex- and in-situ characterizations.•The mechanism of NEC hydrogenation was proposed and verified by DFT calculations.AbstractHydrogen is a promising candidate to replace the exhausting fossil fuels. However, it is still a big challenge for hydrogen storage. Liquid organic hydrogen carrier (LOHC), which possesses high safety and purity, easy transport and reversibility, is highly attractive for hydrogen storage. Herein we report a new reusable bimetallic Pd-Rh nanoparticles (NPs) catalyst with synergy effect, boosting both the hydrogenation of N-ethylcarbazole (NEC) and dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC), which allows multiple cycles of reversible high-weight% hydrogen storage and uptake in short reaction time. Various ex- and in-situ characterizations evidenced that the superior activity was attributed to the bimetallic Pd-Rh NPs cluster structure on the surface of γ-Al2O3 support. The mechanism of NEC hydrogenation over the Pd-Rh catalyst was proposed and verified by density functional theory (DFT) calculations. Such a strategy can be extended to other LOHCs and sheds light onto the development of LOHCs as energy vectors.Graphical abstractDownload : Download high-res image (132KB)Download : Download full-size image


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