Mesoporous Methyl-Functionalized Sn-Silicates Generated by the Aerosol Process for the Sustainable Production of Ethyl Lactate

Research output: Contribution to journalArticle

Abstract

The aerosol-assisted sol−gel process was used to synthesize in a straightforward one-pot procedure a series of methyl-functionalized tin silicates with different degrees of methylation. The successful incorporation of isolated Sn as single site within the silica framework was confirmed via Sn solid-state NMR measurements, while Si and C solid-state magic-angle-spinning NMR experiments revealed a degree of methylation close to the theoretical value, hence proving the efficacy of the adopted cosynthetic approach. These materials were tested as catalysts in the synthesis of ethyl lactate from dihydroxyacetone and ethanol. The methylated solids display enhanced performances in terms of both activity and selectivity compared to the nonmethylated analogues, highlighting a strong beneficial role of surface hydrophobicity. Under proper conditions a total conversion and a selectivity higher than 95% were achieved. Moreover, the efficient separation and reuse of the heterogeneous catalyst as well as the possibility of an easily recover of the reaction solvent result in a very low waste production protocol with an exceptionally low E-factor.
Original languageEnglish
Pages (from-to)14095-14103
Number of pages9
JournalACS Sustainable Chemistry and Engineering
Volume6
Issue number11
DOIs
Publication statusPublished - 5 Nov 2018

Fingerprint

Silicates
methylation
Aerosols
nuclear magnetic resonance
Methylation
silicate
catalyst
aerosol
hydrophobicity
tin
Dihydroxyacetone
Nuclear magnetic resonance
ethanol
Catalysts
Magic angle spinning
Tin
silica
Hydrophobicity
Silicon Dioxide
Ethanol

Keywords

  • Mesoporuos metallosilicate
  • hybrid mateirals
  • hydrophobicity
  • biorefinery
  • spray drying

Cite this

@article{d2cb53303cd14a67ba1116287b192185,
title = "Mesoporous Methyl-Functionalized Sn-Silicates Generated by the Aerosol Process for the Sustainable Production of Ethyl Lactate",
abstract = "The aerosol-assisted sol−gel process was used to synthesize in a straightforward one-pot procedure a series of methyl-functionalized tin silicates with different degrees of methylation. The successful incorporation of isolated Sn as single site within the silica framework was confirmed via Sn solid-state NMR measurements, while Si and C solid-state magic-angle-spinning NMR experiments revealed a degree of methylation close to the theoretical value, hence proving the efficacy of the adopted cosynthetic approach. These materials were tested as catalysts in the synthesis of ethyl lactate from dihydroxyacetone and ethanol. The methylated solids display enhanced performances in terms of both activity and selectivity compared to the nonmethylated analogues, highlighting a strong beneficial role of surface hydrophobicity. Under proper conditions a total conversion and a selectivity higher than 95{\%} were achieved. Moreover, the efficient separation and reuse of the heterogeneous catalyst as well as the possibility of an easily recover of the reaction solvent result in a very low waste production protocol with an exceptionally low E-factor.",
keywords = "Mesoporuos metallosilicate, hybrid mateirals, hydrophobicity, biorefinery, spray drying",
author = "Alvise Vivian and Luca Fusaro and Debecker, {Damien P.} and Carmela Aprile",
note = "doi: 10.1021/acssuschemeng.8b02623",
year = "2018",
month = "11",
day = "5",
doi = "10.1021/acssuschemeng.8b02623",
language = "English",
volume = "6",
pages = "14095--14103",
journal = "ACS Sustainable Chemistry and Engineering",
issn = "2168-0485",
publisher = "American Chemical Society",
number = "11",

}

TY - JOUR

T1 - Mesoporous Methyl-Functionalized Sn-Silicates Generated by the Aerosol Process for the Sustainable Production of Ethyl Lactate

AU - Vivian, Alvise

AU - Fusaro, Luca

AU - Debecker, Damien P.

AU - Aprile, Carmela

N1 - doi: 10.1021/acssuschemeng.8b02623

PY - 2018/11/5

Y1 - 2018/11/5

N2 - The aerosol-assisted sol−gel process was used to synthesize in a straightforward one-pot procedure a series of methyl-functionalized tin silicates with different degrees of methylation. The successful incorporation of isolated Sn as single site within the silica framework was confirmed via Sn solid-state NMR measurements, while Si and C solid-state magic-angle-spinning NMR experiments revealed a degree of methylation close to the theoretical value, hence proving the efficacy of the adopted cosynthetic approach. These materials were tested as catalysts in the synthesis of ethyl lactate from dihydroxyacetone and ethanol. The methylated solids display enhanced performances in terms of both activity and selectivity compared to the nonmethylated analogues, highlighting a strong beneficial role of surface hydrophobicity. Under proper conditions a total conversion and a selectivity higher than 95% were achieved. Moreover, the efficient separation and reuse of the heterogeneous catalyst as well as the possibility of an easily recover of the reaction solvent result in a very low waste production protocol with an exceptionally low E-factor.

AB - The aerosol-assisted sol−gel process was used to synthesize in a straightforward one-pot procedure a series of methyl-functionalized tin silicates with different degrees of methylation. The successful incorporation of isolated Sn as single site within the silica framework was confirmed via Sn solid-state NMR measurements, while Si and C solid-state magic-angle-spinning NMR experiments revealed a degree of methylation close to the theoretical value, hence proving the efficacy of the adopted cosynthetic approach. These materials were tested as catalysts in the synthesis of ethyl lactate from dihydroxyacetone and ethanol. The methylated solids display enhanced performances in terms of both activity and selectivity compared to the nonmethylated analogues, highlighting a strong beneficial role of surface hydrophobicity. Under proper conditions a total conversion and a selectivity higher than 95% were achieved. Moreover, the efficient separation and reuse of the heterogeneous catalyst as well as the possibility of an easily recover of the reaction solvent result in a very low waste production protocol with an exceptionally low E-factor.

KW - Mesoporuos metallosilicate

KW - hybrid mateirals

KW - hydrophobicity

KW - biorefinery

KW - spray drying

U2 - 10.1021/acssuschemeng.8b02623

DO - 10.1021/acssuschemeng.8b02623

M3 - Article

VL - 6

SP - 14095

EP - 14103

JO - ACS Sustainable Chemistry and Engineering

JF - ACS Sustainable Chemistry and Engineering

SN - 2168-0485

IS - 11

ER -