Phosphorus coordinated Rh single-atom sites on nanodiamond as highly regioselective catalyst for hydroformylation of olefins

Peng Gao, Guanfeng Liang (), Tong Ru, Xiaoyan Liu, Haifeng Qi, Aiqin Wang and Fen-Er Chen ()
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Peng Gao: Fudan University
Guanfeng Liang: Fudan University
Tong Ru: Fudan University
Xiaoyan Liu: Chinese Academy of Sciences
Haifeng Qi: Chinese Academy of Sciences
Aiqin Wang: Chinese Academy of Sciences
Fen-Er Chen: Fudan University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-25061-0

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