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New Journal of Chemistry
Page 6 of 8
DOI: 10.1039/C7NJ02557B
Paper
NJC
6
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disappeared in the support and the Air-Pd/γ-Al2O3 samples.
The possible reason for the Air-Pd/γ-Al2O3 hardly showed
active in 1,3-butadiene hydrogenation reaction may be that
there were no 1,3-butadiene adsorption site. Comparing the
adsorption results of these three catalysts, it was manifested
that the adsorption of the 1,3-butadiene was beneficial for the
hydrogenation reaction.
7
8
9
In a word, we can speculate that part of biomolecules
remains on the surface of the Pd/γ-Al2O3 catalysts after
calcination. The active size for 1,3-butadiene hydrogenation
was metallic Pd, when increasing in the fraction of Pd0 in the
catalyst composition result in the further hydrogenation.
Moreover, as reported before22, 26, the biomolecule had
negative influence on the performance of catalysts, which had
been removed to enhance the catalytic activity, since the
active site may be covered. So, we speculated the better
catalytic performance over Fresh-Pd/γ-Al2O3 was largely
attributed to the coexistence between Pd0 and PdO/Pd2+
species.
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In conclusion, we have reported the effect of oxidative and
1212.
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performance of Pd/γ-Al2O3 catalysts for 1,3-butadiene
hydrogenation. It is found that there were no obvious
differences between the fresh Pd catalyst and the calcined
catalysts under different (H2 and air) atmospheres in physical
structure, and the particle diameter of these three catalysts 22 M. Du, D. Sun, H. Yang, J. Huang, X. Jing, T. Odoom-Wubah, H.
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24 G. Zhan, M. Du, J. Huang and Q. Li, Catal. Commun., 2011, 12
(7.4±0.5, 7.5±0.6 and 8.3±0.4 nm) was basically the same, but
the chemical state of Pd varied greatly, there only metallic Pd
species after calcination under H2 atmosphere, while calcined
under air atmosphere, catalyst existing mainly in the oxide
form. Therefore, we speculated that the metallic Pd was the
active specie for 1,3-butadiene catalytic hydrogenation over
the biosynthesized Pd/γ-Al2O3 catalysts at low temperature,
and the coexistence of small amount of oxidation state
PdO/Pd2+ was beneficial for the butene selectivity.
,
830-833.
25 J. L. Huang, L. Q. Lin, Q. B. Li, D. H. Sun, Y. P. Wang, Y. H. Lu,
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Acknowledgements
This work was supported by the National Natural Science
Foundation of China (21536010), and the Natural Science
Foundation of Fujian Province (2017J01025).
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