期刊
NATURE COMMUNICATIONS
卷 9, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-04845-x
关键词
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资金
- China Ministry of Science and Technology [0202801]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117]
- German Research Foundation (DFG)
- European Union's Horizon 2020 research and innovation programme [676580]
- Fundamental Research Funds of Shandong University [2018TB006]
- National Synchrotron Radiation Laboratory in Beijing and Shanghai
Sub-nano metal clusters often exhibit unique and unexpected properties, which make them particularly attractive as catalysts. Herein, we report a precursor-preselected wet-chemistry strategy to synthesize highly dispersed Fe-2 clusters that are supported on mesoporous carbon nitride (mpg-C3N4). The obtained Fe-2/mpg-C3N4 sample exhibits superior catalytic performance for the epoxidation of trans-stilbene to trans-stilbene oxide, showing outstanding selectivity of 93% at high conversion of 91%. Molecular oxygen is the only oxidant and no aldehyde is used as co-reagent. Under the same condition, by contrast, iron porphyrin, single-atom Fe, and small Fe nanoparticles (ca. 3 nm) are nearly reactively inert. First-principles calculations reveal that the unique reactivity of the Fe-2 clusters originates from the formation of active oxygen species. The general applicability of the synthesis approach is further demonstrated by producing other diatomic clusters like Pd-2 and Ir-2, which lays the foundation for discovering diatomic cluster catalysts.
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