期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 9, 页码 3650-3657出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201913453
关键词
alkynes; hydrogenation; metal-organic frameworks; palladium nanoparticle; styrene
资金
- National Key Basic Research Program of China [2014CB931801, 2016YFA0200700]
- National Natural Science Foundation of China [21890381, 21721002, 21475029, 91427302, 21722102, 51672053, 21303029]
- Beijing Natural Science Foundation [2182087]
- Frontier Science Key Project of Chinese Academy of Sciences [QYZDJ-SSW-SLH038]
- CAS-CSIRO Cooperative Research Program [GJHZ1503]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA09040100]
- Youth Innovation Promotion Association CAS [2016036]
- project of K.C. Wong Education Foundation
The semihydrogenation of alkynes into alkenes rather than alkanes is of great importance in the chemical industry. Unfortunately, state-of-the-art heterogeneous catalysts hardly achieve high turnover frequencies (TOFs) simultaneously with almost full conversion, excellent selectivity, and good stability. Here, we used metal-organic frameworks (MOFs) containing Zr metal nodes (UiO) with tunable wettability and electron-withdrawing ability as activity accelerators for the semihydrogenation of alkynes catalyzed by sandwiched palladium nanoparticles (Pd NPs). Impressively, the porous hydrophobic UiO support not only leads to an enrichment of phenylacetylene around the Pd NPs but also renders the Pd surfaces more electron-deficient, which leads to a remarkable catalysis performance, including an exceptionally high TOF of 13835 h(-1), 100 % phenylacetylene conversion 93.1 % selectivity towards styrene, and no activity decay after successive catalytic cycles. The strategy of using molecularly tailored supports is universal for boosting the selective semihydrogenation of various terminal and internal alkynes.
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