期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 131, 期 5, 页码 1883-1888出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja807357r
关键词
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资金
- National Science Foundation of China [20871027]
- Program for New Century Excellent Talents in University [NCET-07-0169]
- Program for Changiiang Scholars
- Innovative Research Team in University
A series of remarkable crystalline compounds [Cu-2(BTC)(4/3)(H2O)(2)](6)[HnXM12O40]center dot(C4H12N)(2) (X = Si, Ge, P, As; M = W, Mo) were obtained from the simple one-step hydrothermal reaction of copper nitrate, benzentricaboxylate (BTC), and different Keggin polyoxometalates (POMs). In these compounds, the catalytically active Keggin polyanions were alternately arrayed as noncoordinating guests in the cuboctahedral cages of a Cu-BTC-based metal-organic framework (MOF) host matrix. X-ray crystallographic analyses, TG, FT-IR, UV-vis, N-2 adsorption studies, and acid-base titration demonstrated their high stability and toleration for thermal and acid-base conditions. No POM leaching or framework decomposition was observed in our study. The representative acid catalytic performance of a compound containing PW12 species was assessed through the hydrolysis of esters in excess water, which showed high catalytic activity and can be used repeatedly without activity loss. Moreover, catalytic selectivity, which is dependent on the molecular size of substrates, and substrate accessibility for the pore surface were observed. It is the first time that the well-defined, crystalline, MOF-supported POM compound has behaved as a true heterogeneous acid catalyst. The unique attributes of MOF and well-dispersed level of POMs prohibited the conglomeration and deactivation of POMs, which allowed for the enhancement of their catalytic properties.
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