Phosphorus coordinated Rh single-atom sites on nanodiamond as highly regioselective catalyst for hydroformylation of olefins.
Peng Gao,Peng Gao,Guanfeng Liang,Tong Ru,Xiaoyan Liu,Haifeng Qi,Aiqin Wang,Fener Chen,Fener Chen +8 more
TL;DR: In this article, a phosphorus-coordinated single-atom catalyst with nanodiamond as support was developed for branched aldehydes in hydroformylation of terminal olefins.
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Abstract: Single-atom Rh catalysts present superior activity relative to homogeneous catalyst in olefins hydroformylation, yet with limited success in regioselectivity control. In the present work, we develop a phosphorus coordinated Rh1 single-atom catalyst with nanodiamond as support. Benefiting from this unique structure, the catalyst exhibits excellent activity and regioselectivity in hydroformylation of arylethylenes with wide substrate generality, i.e., with high conversion (>99%) and high regioselectivity (>90%), which is comparable with the homogeneous counterparts. The coordination interaction between Rh1 and surface phosphorus species is clarified by 31P solid-state NMR and X-ray absorption spectroscopy (XAS). Rh single atoms are firmly anchored over nanodiamond through Rh-P bonds, guaranteeing good stability in the hydroformation of styrene even after six runs. Finally, by using this catalyst, two kinds of pharmaceutical molecules, Ibuprofen and Fendiline, are synthesized efficiently with high yields, demonstrating a new prospect of single-atom catalyst in pharmaceutical synthesis. Single-atom Rh catalysts present superior activity in olefins hydroformylation, yet with limited success in regioselectivity control. Here the authors develop a Rh1 single-atom catalyst with nanodiamond as support, with which good to excellent regioselectivities to branched aldehydes in hydroformylation of terminal olefins are achieved.
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