کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
---|---|---|---|---|
1271697 | 1497566 | 2012 | 8 صفحه PDF | دانلود رایگان |
The complete recovery of the H2 stored on dodecahydro-N-ethylcarbazole was achieved at 443 K and 101 kPa using Pd catalysts prepared by incipient wetness impregnation and calcination in He rather than air. Over a 4 wt% Pd/SiO2 catalyst, the reaction proceeded to complete conversion within 22 min and complete H2 recovery (5.8 wt%) within 1.6 h. The dehydrogenation rate of dodecahydro-N-ethylcarbazole and selectivity to the completely dehydrogenated product, N-ethylcarbazole, were dependent upon the Pd particle size. The dehydrogenation rate of dodecahydro-N-ethylcarbazole was compared to that of dodecahydrocarbazole and dodecahydrofluorene. The lower turn-over frequency (TOF) for dodecahydrocarbazole was attributed to a strong adsorption of the dehydrogenated products to Pd through the N atom, whereas the ethyl group in dodecahydro-N-ethylcarbazole prevented a strong N interaction with the surface. Density functional theory (DFT) results showed that dodecahydrocarbazole and dodecahydrofluorene were more strongly adsorbed on Pd than dodecahydro-N-ethylcarbazole leading to a significant decrease in their TOFs for H2 recovery.
► Complete H2 recovery from dodecahydro-N-ethylcarbazole is reported on Pd/SiO2.
► Catalyst precursor calcination in He rather than air increased catalyst activity.
► Dodecahydro-N-ethylcarbazole dehydrogenation is structure sensitive.
► Strong adsorption of dodecahydrofluorene to the Pd resulted in a very low TOF.
Journal: International Journal of Hydrogen Energy - Volume 37, Issue 3, February 2012, Pages 2715–2722