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Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite
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Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite
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Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite
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Journal Article
Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite
2023
Overview
Zeolites containing Rh single sites stabilized by phosphorous were prepared through a one-pot synthesis method and are shown to have superior activity and selectivity for ethylene hydroformylation at low temperature (50 °C). Catalytic activity is ascribed to confined Rh
2
O
3
clusters in the zeolite which evolve under reaction conditions into single Rh
3+
sites. These Rh
3+
sites are effectively stabilized in a Rh-(O)-P structure by using tetraethylphosphonium hydroxide as a template, which generates in situ phosphate species after H
2
activation. In contrast to Rh
2
O
3
, confined Rh
0
clusters appear less active in propanal production and ultimately transform into Rh(I)(CO)
2
under similar reaction conditions. As a result, we show that it is possible to reduce the temperature of ethylene hydroformylation with a solid catalyst down to 50 °C, with good activity and high selectivity, by controlling the electronic and morphological properties of Rh species and the reaction conditions.
Isolated Rh
3+
sites are stabilized inside the MFI zeolite channels with phosphorous which is added during zeolite synthesis in the form of a phosphonium zeolite template. This Rh
3+
shows high activity in the low-temperature ethylene hydroformylation.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
