An overview of the kinetics and catalysis of hydrogen storage on organic liquids

作者：Sotoodeh Farnaz; Smith Kevin J^*

来源：Canadian Journal of Chemical Engineering, 2013, 91(9): 1477-1490.

DOI：10.1002/cjce.21871

• hydrogen storage
• hydrogenation
• dehydrogenation
• organic heteroaromatics
• kinetics
• catalyst
• Pd
• Ru
• structure sensitivity
• DFT

The potential for chemical H-2 storage on liquid organic hydrogen carriers (LOHCs) has focused attention on the catalytic reactions needed to store and release H-2 from the LOHCs. Herein we review our recent studies on the use of N-ethylcarbazole and carbazole as LOHCs. Experimental data show that the hydrogenation reactions are relatively facile, although N-ethylcarbazole hydrogenates 10x's faster than carbazole on a 5wt% Ru/Al2O3 catalyst at 150 degrees C. Dehydrogenation of dodecahydro-N-ethylcarbazole is more difficult than hydrogenation and is structure sensitive on Pd catalysts. Maximum activity and 100% selectivity to the completely dehydrogenated product, N-ethylcarbazole, was achieved over a 4wt% Pd/SiO2 catalyst with d(Pd)approximate to 9nm. The dehydrogenation TOF of dodecahydrocarbazole and dodecahydrofluorene were much lower than dodecahydro-N-ethylcarbazole. DFT was used to identify the dehydrogenation mechanism and explain the experimental observations. Both theoretical and experimental results lead to the conclusion that dodecahydro-N-ethylcarbazole is a better H(2)storage candidate than dodecahydrocarbazole.

• 出版日期2013-9