High dispersion of heteropolyacid nanoparticles on hydrothermally Cs-modified three-dimensionally ordered macroporous SiO2 with excellent selectivity in methacrolein oxidation

doi:10.1016/j.cjche.2020.07.017

摘要/Abstract

摘要： Heteropolyacid nanoparticles (NPs) were supported on Cs-modified three-dimensionally ordered macroporous (3DOM) SiO₂ and used as the catalyst for the oxidation of methacrolein (MAL) to methacrylic acid (MAA). Hydrothermal treatment and incipient wetness impregnation were employed respectively for the Cs-modification. It was found that hydrothermal Cs-modification of 3DOM SiO₂ promoted the dispersion of the supported heteropolyacid, which showed an average particle size of 5.2 nm, much smaller than that (17.6 nm) on the Csmodified 3DOM SiO₂ prepared by incipient wetness impregnation. The effects of hydrothermal treatment on the structure and catalytic performance of the catalyst were investigated. Results showed that the ion exchange between Cs⁺ and the surface silanol groups on 3DOM SiO₂ was promoted with the increase of the hydrothermal temperature. Meanwhile, Cs-modification helped the heteropolyacid to retain intact Keggin structure, inhibiting the formation of MoO₃. Highly dispersed heteropolyacid NPs with enhanced structural stability exhibited excellent selectivity to MAA in the oxidation of MAL.

关键词: Catalyst support, Heteropolyacid, Nanoparticles, Oxidation, Methacrolein

Abstract: Heteropolyacid nanoparticles (NPs) were supported on Cs-modified three-dimensionally ordered macroporous (3DOM) SiO₂ and used as the catalyst for the oxidation of methacrolein (MAL) to methacrylic acid (MAA). Hydrothermal treatment and incipient wetness impregnation were employed respectively for the Cs-modification. It was found that hydrothermal Cs-modification of 3DOM SiO₂ promoted the dispersion of the supported heteropolyacid, which showed an average particle size of 5.2 nm, much smaller than that (17.6 nm) on the Csmodified 3DOM SiO₂ prepared by incipient wetness impregnation. The effects of hydrothermal treatment on the structure and catalytic performance of the catalyst were investigated. Results showed that the ion exchange between Cs⁺ and the surface silanol groups on 3DOM SiO₂ was promoted with the increase of the hydrothermal temperature. Meanwhile, Cs-modification helped the heteropolyacid to retain intact Keggin structure, inhibiting the formation of MoO₃. Highly dispersed heteropolyacid NPs with enhanced structural stability exhibited excellent selectivity to MAA in the oxidation of MAL.

Key words: Catalyst support, Heteropolyacid, Nanoparticles, Oxidation, Methacrolein

Heng Zhang, Junqi Liu, Chenyuan Liu, Tingting Wang, Wancheng Zhu. High dispersion of heteropolyacid nanoparticles on hydrothermally Cs-modified three-dimensionally ordered macroporous SiO₂ with excellent selectivity in methacrolein oxidation[J]. 中国化学工程学报, 2020, 28(11): 2785-2791.

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High dispersion of heteropolyacid nanoparticles on hydrothermally Cs-modified three-dimensionally ordered macroporous SiO₂ with excellent selectivity in methacrolein oxidation

High dispersion of heteropolyacid nanoparticles on hydrothermally Cs-modified three-dimensionally ordered macroporous SiO₂ with excellent selectivity in methacrolein oxidation

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