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Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation
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Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation
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Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation
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Journal Article
Carbon nitride supported Fe2 cluster catalysts with superior performance for alkene epoxidation
2018
Overview
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-C
3
N
4
). The obtained Fe
2
/mpg-C
3
N
4
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.
Sub-nano clusters with atomic precision provide a compelling platform for bridging heterogeneous and homogeneous catalysis, but their synthesis remains a great challenge. Here, the authors report a precursor-preselected wet-chemistry strategy to synthesize highly dispersed Fe
2
clusters supported on mesoporous carbon nitride.
