Enhanced Biphasic Reactions in Amphiphilic Silica Mesopores
© 2024 The Authors. Published by American Chemical Society..
In this study, we investigated the effect of the pore volume and mesopore size of surface-active catalytic organosilicas on the genesis of particle-stabilized (Pickering) emulsions for the dodecanal/ethylene glycol system and their reactivity for the acid-catalyzed biphasic acetalization reaction. To this aim, we functionalized a series of fumed silica superparticles (size 100-300 nm) displaying an average mesopore size in the range of 11-14 nm and variable mesopore volume, with a similar surface density of octyl and propylsulfonic acid groups. The modified silica superparticles were characterized in detail using different techniques, including acid-base titration, thermogravimetric analysis, TEM, and dynamic light scattering. The pore volume of the particles impacts their self-assembly and coverage at the dodecanal/ethylene glycol (DA/EG) interface. This affects the stability and the average droplet size of emulsions and conditions of the available interfacial surface area for reaction. The maximum DA-EG productivity is observed for A200 super-SiNPs with a pore volume of 0.39 cm3·g-1 with an interfacial coverage by particles lower than 1 (i.e., submonolayer). Using dissipative particle dynamics and all-atom grand canonical Monte Carlo simulations, we unveil a stabilizing role of the pore volume of porous silica superparticles for generating emulsions and local micromixing of immiscible dodecanal and ethylene glycol, allowing fast and efficient solvent-free acetalization in the presence of Pickering emulsions. The micromixing level is interrelated to the adsorption energy of self-assembled particles at the DA/EG interface.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:128 |
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| Enthalten in: |
The journal of physical chemistry. C, Nanomaterials and interfaces - 128(2024), 4 vom: 01. Feb., Seite 1644-1653 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Zhao, Guolin [VerfasserIn] |
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| Links: |
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| Themen: |
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| Anmerkungen: |
Date Revised 10.02.2024 published: Electronic-eCollection Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/acs.jpcc.3c07477 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM368119750 |
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| 520 | |a © 2024 The Authors. Published by American Chemical Society. | ||
| 520 | |a In this study, we investigated the effect of the pore volume and mesopore size of surface-active catalytic organosilicas on the genesis of particle-stabilized (Pickering) emulsions for the dodecanal/ethylene glycol system and their reactivity for the acid-catalyzed biphasic acetalization reaction. To this aim, we functionalized a series of fumed silica superparticles (size 100-300 nm) displaying an average mesopore size in the range of 11-14 nm and variable mesopore volume, with a similar surface density of octyl and propylsulfonic acid groups. The modified silica superparticles were characterized in detail using different techniques, including acid-base titration, thermogravimetric analysis, TEM, and dynamic light scattering. The pore volume of the particles impacts their self-assembly and coverage at the dodecanal/ethylene glycol (DA/EG) interface. This affects the stability and the average droplet size of emulsions and conditions of the available interfacial surface area for reaction. The maximum DA-EG productivity is observed for A200 super-SiNPs with a pore volume of 0.39 cm3·g-1 with an interfacial coverage by particles lower than 1 (i.e., submonolayer). Using dissipative particle dynamics and all-atom grand canonical Monte Carlo simulations, we unveil a stabilizing role of the pore volume of porous silica superparticles for generating emulsions and local micromixing of immiscible dodecanal and ethylene glycol, allowing fast and efficient solvent-free acetalization in the presence of Pickering emulsions. The micromixing level is interrelated to the adsorption energy of self-assembled particles at the DA/EG interface | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Li, Yao |e verfasserin |4 aut | |
| 700 | 1 | |a Zhen, Wen |e verfasserin |4 aut | |
| 700 | 1 | |a Gao, Jie |e verfasserin |4 aut | |
| 700 | 1 | |a Gu, Yunjiao |e verfasserin |4 aut | |
| 700 | 1 | |a Hong, Bing |e verfasserin |4 aut | |
| 700 | 1 | |a Han, Xia |e verfasserin |4 aut | |
| 700 | 1 | |a Zhao, Shuangliang |e verfasserin |4 aut | |
| 700 | 1 | |a Pera-Titus, Marc |e verfasserin |4 aut | |
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