期刊
CATALYSIS TODAY
卷 359, 期 -, 页码 124-132出版社
ELSEVIER
DOI: 10.1016/j.cattod.2019.06.076
关键词
Zeolitic imidazolate frameworks (ZIFs); Amine-functionalization; Post-synthetic modification; Acid-base reaction; One-pot tandem reaction
资金
- National Research Council of Science & Technology (NST) - Korea government (MSIP) [CMP-16-04-KITECH]
- R&D Convergence Program of Ministry of Science, ICT and Future Planning, National Research Council of Science Technology [CRC-14-1-KRICT]
- Korea Institute of Science and Technology (KIST) [2E28020]
A bifunctional zeolitic imidazolate framework catalyst with amine and sulfonic acid groups was successfully prepared through a simple two-step post-synthetic modification, showing good catalytic performance and reusability in the reaction.
An acid-base bifunctional zeolitic imidazolate framework catalyst (ZIF8-A61-SO3H) with amine and sulfonic acid groups was successfully prepared through simple two step post-synthetic modification: preparation of aminefunctionalized ZIF-8 with amine contents of 61% (ZIF8-A61) by the ligand exchange of 2-mIM with 3-amino1,2,4-triazole (Atz), followed by the sulfonic acid functionalization by the ring-opening reaction of 1,3-propanesultone with -NH2 groups in ZIF8-A61. Amine-functionalized ZIF8-A materials with difference amine contents (15%, 34%, and 61%, respectively) were also prepared by controlling the synthesis time. All obtained ZIF catalysts evaluated as a heterogeneous catalyst for one-pot deacetalization-Knoevenagel condensation tandem reaction. Compared with ZIF-8 and amine-functionalized ZIF-8 catalysts, ZIF8-A61-SO3H catalyst showed good catalytic performance with 100% conversion of the reactant and 98% selectivity of the final Knoevenagel product. An enhanced catalytic activity can be attributed to the co-existence of site-isolated acid-base groups on the ZIF8-A61-SO3H catalyst in close proximity. The heterogeneous nature of the catalytic system was confirmed by a hot-filtering test and the catalyst also exhibited reusable in the five repeated cycles. A plausible catalytic mechanism of deacetalization-Knoevenagel condensation reaction over ZIF8-A61-SO3H was also proposed.
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