Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation

Shubo Tian, Qiang Fu, Wenxing Chen, Quanchen Feng, Zheng Chen, Jian Zhang, Weng-Chon Cheong, Rong Yu, Lin Gu, Juncai Dong, Jun Luo, Chen Chen, Qing Peng, Claudia Draxl, Dingsheng Wang () and Yadong Li
Additional contact information
Shubo Tian: Tsinghua University
Qiang Fu: Humboldt-Universität zu Berlin
Wenxing Chen: Tsinghua University
Quanchen Feng: Tsinghua University
Zheng Chen: Tsinghua University
Jian Zhang: Tsinghua University
Weng-Chon Cheong: Tsinghua University
Rong Yu: Tsinghua University
Lin Gu: Chinese Academy of Sciences
Juncai Dong: Chinese Academy of Sciences
Jun Luo: Tianjin University of Technology
Chen Chen: Tsinghua University
Qing Peng: Tsinghua University
Claudia Draxl: Humboldt-Universität zu Berlin
Dingsheng Wang: Tsinghua University
Yadong Li: Tsinghua University

Nature Communications, 2018, vol. 9, issue 1, 1-7

Abstract: Abstract 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 Fe2 clusters that are supported on mesoporous carbon nitride (mpg-C3N4). The obtained Fe2/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 Fe2 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 Pd2 and Ir2, which lays the foundation for discovering diatomic cluster catalysts.

Date: 2018
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DOI: 10.1038/s41467-018-04845-x

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