Fe3O4@UiO-66-NH2 core-shell nanohybrid as stable heterogeneous catalyst for Knoevenagel condensation

doi:10.1016/S1872-2067(16)62562-7

Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (12): 2106-2113.DOI: 10.1016/S1872-2067(16)62562-7

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Fe₃O₄@UiO-66-NH₂ core-shell nanohybrid as stable heterogeneous catalyst for Knoevenagel condensation

Yanmei Zhang^a, Tianlin Dai^b, Fan Zhang^a, Jing Zhang^b, Gang Chu^b, Chunshan Quan^a

a College of Life Science, Dalian Minzu University, Dalian 116600, Liaoning, China;
b School of Chemistry and Material Science, Liaoning Shihua University, Fushun 113001, Liaoning, China

Received:2016-08-25 Revised:2016-09-14 Online:2016-12-27 Published:2016-12-27
Contact: Yanmei Zhang
Supported by:
This work was supported by the National Natural Science Foundation of China (21203017), Open Fund of State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (N-11-3), Program for Liaoning Excellent Talents in University (LNET), and the Fundamental Research Funds for the Central Universities (DC201502020304).

Abstract

Abstract:

Magnetic separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase. Here, core-shell Fe₃O₄@UiO-66-NH₂ nanohybrids with well-defined structures were constructed by dispersing magnets in a dimethylformamide (DMF) solution containing two metal-organic framework (MOF) precursors, namely ZrCl₄ and 2-aminobenzenetricarboxylic acid. This method is simpler and more efficient than previously reported step-by-step method in which magnets were consecutively dispersed in DMF solutions each containing one MOF precursor, and the obtained Fe₃O₄@UiO-66-NH₂ with three assembly cycles has a higher degree of crystallinity and porosity. The core-shell Fe₃O₄@UiO-66-NH₂ is highly active and selective in Knoevenagel condensations because of the bifunctionality of UiO-66-NH₂ and better mass transfer in the nano-sized shells. It also has good recycling stability, and can be recovered magnetically and reused at least four times without significant loss of catalytic activity and framework integrity. The effects of substitution on the reactivity of benzaldehyde and of substrate size were also investigated.

Key words: Metal-organic framework, UiO-66-NH₂, Fe₃O₄, Heterogeneous catalyst, Knoevenagel condensation, Magnetic separation

Yanmei Zhang, Tianlin Dai, Fan Zhang, Jing Zhang, Gang Chu, Chunshan Quan. Fe₃O₄@UiO-66-NH₂ core-shell nanohybrid as stable heterogeneous catalyst for Knoevenagel condensation[J]. Chinese Journal of Catalysis, 2016, 37(12): 2106-2113.

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Fe₃O₄@UiO-66-NH₂ core-shell nanohybrid as stable heterogeneous catalyst for Knoevenagel condensation

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