Highly efficient dehydrogenation of dodecahydro-N-ethylcarbazole over Al2O3 supported PdCo bimetallic nanocatalysts prepared by galvanic replacement.
In: International Journal of Hydrogen Energy, Jg. 49 (2024-01-03), S. 1547-1557
Online
academicJournal
Zugriff:
NEC is one of the most promising liquid organic hydrogen storage materials. The highly efficient and low cost dehydrogenation catalysts are crucial for large-scale hydrogen storage. In this paper, Co/Al 2 O 3 precursors were prepared by chemical reduction, and then a series of Pd 1 Co n /Al 2 O 3 catalysts for 12H-NEC dehydrogenation was prepared by galvanic replacement of Pd2+ using Co as a template and reducing agent. The prepared catalysts were characterized by TEM, FT-IR, XPS, H 2 -TPR and H 2 -TPD. The results demonstrated that Pd 1 Co n NPs were uniformly dispersed over the surface of Al 2 O 3 in the form of Co@Pd core-shell structure, CoPd alloy and PdNPs, with an average particle size of 2.78 nm. The electron transfer occurred between Co and Pd. For the dehydrogenation of H12-NEC, the produced Pd 1 Co 5 /Al 2 O 3 catalyst exhibited excellent catalytic activity. The dehydrogenation efficiency was 100% at 180 °C for 3 h and 98.5% at 150 °C for 6 h, and TOF reached 1.414 gH 2 /gPd min−1, which was significantly higher than that of monometallic Pd/Al 2 O 3 catalysts and that reported in the literature. The kinetic studies of the catalytic 12H-NEC dehydrogenation showed that 4H-NEC→NEC is the rate-limiting step with the highest apparent activation energy of 68.72 kJ/mol. The hydrogen release efficiency remained essentially unchanged after four cycles. [Display omitted] • Al 2 O 3 supported PdCo bimetallic catalyst for highly efficient 12H-NEC dehydrogenation was prepared by galvanic replacement. • Ultrafine nanosize, intermetallic electron transfer, and PdCo NPs and Al 2 O 3 interaction enhanced catalytic performance. • The 12H-NEC dehydrogenation efficiency over Pd 1 Co 5 /Al 2 O 3 reached 100% at 180 °C for 3 h and 98.5% at 150 °C for 6 h. • The complexation of PdCo NPs with O of hydroxyl groups on the Al 2 O 3 surface improved the catalytic stability. [ABSTRACT FROM AUTHOR]
Titel: |
Highly efficient dehydrogenation of dodecahydro-N-ethylcarbazole over Al2O3 supported PdCo bimetallic nanocatalysts prepared by galvanic replacement.
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Autor/in / Beteiligte Person: | Sun, Chuanran ; Liu, Xiaoran ; Bai, Xuefeng |
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Zeitschrift: | International Journal of Hydrogen Energy, Jg. 49 (2024-01-03), S. 1547-1557 |
Veröffentlichung: | 2024 |
Medientyp: | academicJournal |
ISSN: | 0360-3199 (print) |
DOI: | 10.1016/j.ijhydene.2023.10.118 |
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