Single Rh1Co catalyst enabling reversible hydrogenation and dehydrogenation of N-ethylcarbazole for hydrogen storage

Abstract

N-ethylcarbazole (NEC) has been considered one of the most prospective liquid organic hydrogen carriers (LOHCs) for hydrogen storage. However, designing single catalyst capable of driving both hydrogenation of NEC and dehydrogenation of dodecahydro-NEC (12 H-NEC) is of a big challenge. Herein, we develop an atomic-dispersion of Rh with the Co nanoparticles (NPs) to form a Rh1Co structure maximizing the Rh utilization, which boosts the reversible (de)hydrogenation of NEC, and enables multiple cycles of reversible hydrogen uptake and release. Significantly, a low temperature of 90 °C is realized for the complete hydrogenation (100%), representing one of the lowest temperatures yet reported for the total hydrogenation of NEC. The remarkable catalytic performance of Rh1Co catalysts is the result of the optimal electronic structure between atomic-dispersion of Rh and Co NPs confirmed by structural characterizations and density functional theory (DFT) calculations, which allowed fast interfacial electron transfer to intermediates.