Journal
ACS OMEGA
Volume 6, Issue 9, Pages 6466-6473Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsomega.1c00176
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Funding
- National Natural Science Foundation of China [82004208]
- Postdoctoral Science Foundation of China [2020M681948]
- Zhejiang Provincial Postdoctoral Science Foundation [ZJ2020104]
- Scientific Research Fund of Zhejiang Provincial Education Department [Y201942316]
- Scientific Research and Innovation Fund of Zhejiang Chinese Medical University [KC201915]
- Research Project of Zhejiang Chinese Medical University [BZXCG-2020-11, 2020ZZ07, 2019ZG36, SZZ201816]
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A novel metal-free, reusable, and green catalytic system comprising hydrothermal carbon microspheres supporting N-hydroxyphthalimide was developed and successfully employed in the aerobic oxidation of alcohol, achieving superior performance and versatile catalytic effect for diversified alcohols.
A novel metal-free, reusable, and green catalytic system comprising hydrothermal carbon microspheres (HCMSs) supporting N-hydroxyphthalimide (NHPI) was developed and employed in the aerobic oxidation of alcohol. Hierarchically porous HCMSs with good monodispersity were produced by the hydrothermal carbonization of sucrose and designed NaOH-impregnated calcination under a static air atmosphere. The meso- and macroporous pores on HCMSs make up 71% of the total pore volume. The covalent immobilization of NHPI onto HCMSs was first accomplished by grafting hyperbranched polyquaternary amine via repetitive ring-opening reactions of diglycidyl ether and subsequent amidation with 4-carboxy-NHPI. Owing to the cocatalysis of grafted quaternary ammonium salt, a designed heterogeneous catalyst has superior performance to free NHPI in the oxidation of 2-phenylethanol. The established catalytic system achieved 42% conversion and up to 96% selectivity of acetophenone at 90 degrees C under 1 atm O-2 for 20 h and presented a versatile catalytic effect for diversified alcohols. Immobilized NHPI could be facilely recycled via simple filtration and displayed good stability for six cycles without a discernible decrease of reactivity or damage of catalyst morphology in repeated oxidation test.
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