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. 2018 Mar 29;8(22):12282-12291.
doi: 10.1039/c8ra01507d. eCollection 2018 Mar 26.

Amine-functionalized MIL-53(Al) with embedded ruthenium nanoparticles as a highly efficient catalyst for the hydrolytic dehydrogenation of ammonia borane

Shuren Zhang  1 , Liqun Zhou  1 , Menghuan Chen  1
Affiliations

Amine-functionalized MIL-53(Al) with embedded ruthenium nanoparticles as a highly efficient catalyst for the hydrolytic dehydrogenation of ammonia borane

Shuren Zhang et al. RSC Adv. .

Abstract

Well-dispersed ruthenium nanoparticles (Ru NPs) are immobilized within the pores of amine-functionalized MIL-53 via an in situ impregnation-reduction method. The resulting Ru/MIL-53(Al)-NH2 catalyst exhibits superior catalytic performance for the dehydrogenation of ammonia borane (AB) at ambient temperature relative to the Ru/MIL-53(Al) catalyst; it has a turnover frequency (TOF) of 287 mol H2 min-1 (mol Ru)-1 and an activation energy (E a) of 30.5 kJ mol-1. The amine groups present in the MIL-53(Al)-NH2 framework facilitate the formation and stabilization of ultra-small Ru NPs by preventing their aggregation. Additionally, the Ru/MIL-53(Al)-NH2 catalyst exhibits satisfactory durability and reusability: 72.4% and 86.3% of the initial catalytic activity was maintained after the fifth successive cycle of the hydrolytic dehydrogenation of AB in the two respective tests.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. (a) Wide-angle and (b) magnified Ru PXRD patterns of Ru/MIL-53(Al), MIL-53(Al), Ru/MIL-53(Al)-NH2, and MIL-53(Al)-NH2.
Fig. 2
Fig. 2. FT-IR spectra of (a) MIL-53(Al)-NH2, (b) Ru/MIL-53(Al)-NH2, and (c) Ru/MIL-53(Al)-NH2 after the fifth run in the durability test.
Fig. 3
Fig. 3. TEM images of (a and b) initially prepared Ru/MIL-53(Al)-NH2 and (c and d) Ru/MIL-53(Al)-NH2 after five catalytic cycles; particle size distribution of (e) initially prepared Ru/MIL-53(Al)-NH2 and (f) Ru/MIL-53(Al)-NH2 after five catalytic cycles; (g) EDX spectrum of Ru/MIL-53(Al)-NH2.
Fig. 4
Fig. 4. XPS spectra of the synthesized Ru/MIL-53(Al)-NH2 catalyst: (a) survey scan and (b) Ru 3p spectrum.
Fig. 5
Fig. 5. Hydrogen generation from the hydrolysis of AB catalyzed by Ru/MIL-53(Al)-NH2, Ru/MIL-53, Ru NPs, MIL-53(Al), and MIL-53(Al)-NH2.
Fig. 6
Fig. 6. (a and c) Effect of temperature on the hydrogen generation rate catalyzed by Ru/MIL-53(Al)-NH2 and Ru/MIL-53(Al) catalysts; (b and d) Arrhenius plots obtained from the corresponding temperature effects.
Fig. 7
Fig. 7. (a and c) Durability of Ru/MIL-53(Al)-NH2 and Ru/MIL-53(Al) catalysts from the 1st to the 5th cycle; (b and d) corresponding percentage of the initial catalytic activity remaining after successive cycles of AB hydrolysis.
Fig. 8
Fig. 8. (a and c) Reusability of the Ru/MIL-53(Al)-NH2 and Ru/MIL-53(Al) catalysts from the 1st to the 5th cycle; (b and d) corresponding percentage of the initial catalytic activity remaining after successive cycles of AB hydrolysis.
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