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solution (0.2 M), the above catalytic reduction reactions followed 12 L. K. Zhu, D. L. Zhang, M. Xue, H. Li, S. L. Qiu, CrystEngComm.
,
the Langmuir–Hinshelwood apparent first order kinetics model,
whose kinetics was ln(C /C0)=-kt is apparent rate constant,
reaction time, Ct and C0 is concentrations of 4-NP at time
respectively). Fig. 4c showed ln(C /C0) versus reaction time for
2013, 15, 9356.
DOI: 10.1039/C6CC05366A
t
(
k
t
is 13 www.calidris-em.com/RED.php
and 0, 14 J. Zhao, M. G. Li, J. L. Sun, L. F. Liu, P. P. Su, Q. H. Yang, C. Li,
t
t
Chem. Eur. J, 2012, 18, 3163.
the reduction of 4-NP over the Ni-NPC-600. The rate constant
was calculated to be 5.9×10 s . In addition, the Ni NPs
k
15 B. Liu, H. Shioyama, H. L. Jiang, X. B. Zhang, Q. Xu, Carbon, 2010,
48, 456.
-
3
-1
deposited inside the nanoporous carbon were highly crystallized. 16 E. M. M. Ibrahim, S. Hampel, R. Kamsanipally, T. Juergen, K.
Therefore, it was highly desirable to obtain a high magnetization
value for easy separation by an external magnetic field and a
Erdmann, S. Fuessel, C. Taeschner, V. O. Khavrus, T. Gemming, A.
Leonhardt, B. Buechner, Carbon, 2013, 63, 358.
more stable catalyst for recycling (inset of Fig. 4c). Following, 17 Y. H. Deng, Y. Cai, Z. K. Sun, J. Liu, C. Liu, J. Wei, W. Li, C. Liu, Y.
the stability (reusability) acted as another significant issue for Ni- Wang, D. Y. Zhao, J. Am. Chem. Soc., 2010, 132, 8466.
NPC-600 was studied, as displayed in Fig. 4d. Also, the 18 K. Jiang, H. X. Zhang, Y. Y. Yang, R. Mothes, H. Lang, W. B. Cai,
conversion of the first cycle is calculated to reach nearly 98% Chem. Commun., 2011, 47, 11924.
from C /C0 (Fig. S12), and it is found that the conversion 19 S. H. Zhang, S. L. Gai, F. Y. He, L. Dai, P. Gao, L. Li, Y. J. Chen, P.
t
remained higher than 96% even up to 10 cycles. Table S1 gives a
P. Yang, Nanoscal, 2014, 6, 7025.
comparison of the catalytic activities and conversion in our work 20 Z. Y. Niu, S. H. Zhang, Y. B. Sun, S. L. Gai, F. He, Y. L. Dai, L. Li, P.
17-23
with previous reports.
Ni-NPC-600 was stable for at least 15 hours in the 4-NP reaction 21 S. H. Zhang, S. L. Gai, F. Y. He, S. J. Ding, L. Li, P. P. Yang,
solution, and not inclined to aggregate (Fig. S13). It′s clearly Nanoscale, 2014, , 11181.
found Ni-NPC-600 have higher stability, that is due to high 22 B. Y. Guan, X. Wang, Y. Xiao, Y. L. Liu, Q. S. Huo, Nanoscale, 2013,
Furthermore, TEM images showed that
P. Yang, Dalton Trans., 2014, 43, 16911.
6
content and uniform Ni particles dispersed inside nanoporous
carbon which protecting Ni particles from aggregating.
In conclusion, we have observed the transition from Ni-MOF
to Ni-NPC for the first time by the TEM combined with in situ
hot stage, which will be a powerful tool for the carbonization of
MOFs to obtain derivations of MOFs with different
applications.
5
, 2469.
23 X. M. Chen, Z. X. Cai, X. Chen, M. Oyama, J. Mater. Chem. A, 2014,
, 5668.
2
This work was supported by National Natural Science
Foundation of China (91022030, 21390394 and 21261130584),
the National Basic Research Program of China
(
2012CB821700), "111" project (B07016) and Ministry of
Education, Science and Technology Development Center
Project (20120061130012).
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