Spray-drying water-based assembly of hierarchical and ordered mesoporous silica microparticles with enhanced pore accessibility for efficient bio-adsorption

Zhangxiong Wu, Kathryn Waldron, Xiangcheng Zhang, Yunqing Li, Lei Wu, Winston Duo Wu, Xiao Dong Chen, Dongyuan Zhao, Cordelia Selomulya

Research output: Contribution to journalArticleResearchpeer-review

Abstract

The fast and scalable spray-drying-assisted evaporation-induced self-assembly (EISA) synthesis of hierarchically porous SBA-15-type silica microparticles from a water-based system is demonstrated. The SBA-15-type silica microparticles has bowl-like shapes, uniform micro-sizes (∼90 µm), large ordered mesopores (∼9.5 nm), hierarchical meso-/macropores (20–100 nm) and open surfaces. In the synthesis, soft- and hard-templating approaches are combined in a single rapid drying process with a non-ionic tri-block copolymer (F127) and a water-insoluble polymer colloid (Eudragit RS, 120 nm) as the co-templates. The RS polymer colloid plays three important roles. First, the RS nanoparticles can be partially dissolved by in-situ generated ethanol to form RS polymer chains. The RS chains swell and modulate the hydrophilic-hydrophobic balance of F127 micelles to allow the formation of an ordered mesostructure with large mesopore sizes. Without RS, only worm-like mesostructure with much smaller mesopore sizes can be formed. Second, part of the RS nanoparticles plays a role in templating the hierarchical pores distributed throughout the microparticles. Third, part of the RS polymer forms surface “skins” and “bumps”, which can be removed by calcination to enable a more open surface structure to overcome the low pore accessibility issue of spray-dried porous microparticles. The obtained materials have high surface areas (315–510 m2 g−1) and large pore volumes (0.64–1.0 cm3 g−1), which are dependent on RS concentration, HCl concentration, silica precursor hydrolysis time and drying temperature. The representative materials are promising for the adsorption of lysozyme. The adsorption occurs at a >three-fold faster rate, in a five-fold larger capacity (an increase from 20 to 100 mg g−1) and without pore blockage compared with the adsorption of lysozyme onto spray-dried microparticles of similar physicochemical properties obtained without the use of RS.

Original languageEnglish
Pages (from-to)529-540
Number of pages12
JournalJournal of Colloid and Interface Science
Volume556
DOIs
Publication statusPublished - 15 Nov 2019

Keywords

  • Bio-adsorption
  • Hierarchical structure
  • Particle processing
  • Porous silica
  • Spray drying

Cite this

@article{e4b198e1de534dcd9b3dd8c78a2ce4ef,
title = "Spray-drying water-based assembly of hierarchical and ordered mesoporous silica microparticles with enhanced pore accessibility for efficient bio-adsorption",
abstract = "The fast and scalable spray-drying-assisted evaporation-induced self-assembly (EISA) synthesis of hierarchically porous SBA-15-type silica microparticles from a water-based system is demonstrated. The SBA-15-type silica microparticles has bowl-like shapes, uniform micro-sizes (∼90 µm), large ordered mesopores (∼9.5 nm), hierarchical meso-/macropores (20–100 nm) and open surfaces. In the synthesis, soft- and hard-templating approaches are combined in a single rapid drying process with a non-ionic tri-block copolymer (F127) and a water-insoluble polymer colloid (Eudragit RS, 120 nm) as the co-templates. The RS polymer colloid plays three important roles. First, the RS nanoparticles can be partially dissolved by in-situ generated ethanol to form RS polymer chains. The RS chains swell and modulate the hydrophilic-hydrophobic balance of F127 micelles to allow the formation of an ordered mesostructure with large mesopore sizes. Without RS, only worm-like mesostructure with much smaller mesopore sizes can be formed. Second, part of the RS nanoparticles plays a role in templating the hierarchical pores distributed throughout the microparticles. Third, part of the RS polymer forms surface “skins” and “bumps”, which can be removed by calcination to enable a more open surface structure to overcome the low pore accessibility issue of spray-dried porous microparticles. The obtained materials have high surface areas (315–510 m2 g−1) and large pore volumes (0.64–1.0 cm3 g−1), which are dependent on RS concentration, HCl concentration, silica precursor hydrolysis time and drying temperature. The representative materials are promising for the adsorption of lysozyme. The adsorption occurs at a >three-fold faster rate, in a five-fold larger capacity (an increase from 20 to 100 mg g−1) and without pore blockage compared with the adsorption of lysozyme onto spray-dried microparticles of similar physicochemical properties obtained without the use of RS.",
keywords = "Bio-adsorption, Hierarchical structure, Particle processing, Porous silica, Spray drying",
author = "Zhangxiong Wu and Kathryn Waldron and Xiangcheng Zhang and Yunqing Li and Lei Wu and Wu, {Winston Duo} and Chen, {Xiao Dong} and Dongyuan Zhao and Cordelia Selomulya",
year = "2019",
month = "11",
day = "15",
doi = "10.1016/j.jcis.2019.08.084",
language = "English",
volume = "556",
pages = "529--540",
journal = "Journal of Colloid and Interface Science",
issn = "0021-9797",
publisher = "Elsevier",

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Spray-drying water-based assembly of hierarchical and ordered mesoporous silica microparticles with enhanced pore accessibility for efficient bio-adsorption. / Wu, Zhangxiong; Waldron, Kathryn; Zhang, Xiangcheng; Li, Yunqing; Wu, Lei; Wu, Winston Duo; Chen, Xiao Dong; Zhao, Dongyuan; Selomulya, Cordelia.

In: Journal of Colloid and Interface Science, Vol. 556, 15.11.2019, p. 529-540.

Research output: Contribution to journalArticleResearchpeer-review

TY - JOUR

T1 - Spray-drying water-based assembly of hierarchical and ordered mesoporous silica microparticles with enhanced pore accessibility for efficient bio-adsorption

AU - Wu, Zhangxiong

AU - Waldron, Kathryn

AU - Zhang, Xiangcheng

AU - Li, Yunqing

AU - Wu, Lei

AU - Wu, Winston Duo

AU - Chen, Xiao Dong

AU - Zhao, Dongyuan

AU - Selomulya, Cordelia

PY - 2019/11/15

Y1 - 2019/11/15

N2 - The fast and scalable spray-drying-assisted evaporation-induced self-assembly (EISA) synthesis of hierarchically porous SBA-15-type silica microparticles from a water-based system is demonstrated. The SBA-15-type silica microparticles has bowl-like shapes, uniform micro-sizes (∼90 µm), large ordered mesopores (∼9.5 nm), hierarchical meso-/macropores (20–100 nm) and open surfaces. In the synthesis, soft- and hard-templating approaches are combined in a single rapid drying process with a non-ionic tri-block copolymer (F127) and a water-insoluble polymer colloid (Eudragit RS, 120 nm) as the co-templates. The RS polymer colloid plays three important roles. First, the RS nanoparticles can be partially dissolved by in-situ generated ethanol to form RS polymer chains. The RS chains swell and modulate the hydrophilic-hydrophobic balance of F127 micelles to allow the formation of an ordered mesostructure with large mesopore sizes. Without RS, only worm-like mesostructure with much smaller mesopore sizes can be formed. Second, part of the RS nanoparticles plays a role in templating the hierarchical pores distributed throughout the microparticles. Third, part of the RS polymer forms surface “skins” and “bumps”, which can be removed by calcination to enable a more open surface structure to overcome the low pore accessibility issue of spray-dried porous microparticles. The obtained materials have high surface areas (315–510 m2 g−1) and large pore volumes (0.64–1.0 cm3 g−1), which are dependent on RS concentration, HCl concentration, silica precursor hydrolysis time and drying temperature. The representative materials are promising for the adsorption of lysozyme. The adsorption occurs at a >three-fold faster rate, in a five-fold larger capacity (an increase from 20 to 100 mg g−1) and without pore blockage compared with the adsorption of lysozyme onto spray-dried microparticles of similar physicochemical properties obtained without the use of RS.

AB - The fast and scalable spray-drying-assisted evaporation-induced self-assembly (EISA) synthesis of hierarchically porous SBA-15-type silica microparticles from a water-based system is demonstrated. The SBA-15-type silica microparticles has bowl-like shapes, uniform micro-sizes (∼90 µm), large ordered mesopores (∼9.5 nm), hierarchical meso-/macropores (20–100 nm) and open surfaces. In the synthesis, soft- and hard-templating approaches are combined in a single rapid drying process with a non-ionic tri-block copolymer (F127) and a water-insoluble polymer colloid (Eudragit RS, 120 nm) as the co-templates. The RS polymer colloid plays three important roles. First, the RS nanoparticles can be partially dissolved by in-situ generated ethanol to form RS polymer chains. The RS chains swell and modulate the hydrophilic-hydrophobic balance of F127 micelles to allow the formation of an ordered mesostructure with large mesopore sizes. Without RS, only worm-like mesostructure with much smaller mesopore sizes can be formed. Second, part of the RS nanoparticles plays a role in templating the hierarchical pores distributed throughout the microparticles. Third, part of the RS polymer forms surface “skins” and “bumps”, which can be removed by calcination to enable a more open surface structure to overcome the low pore accessibility issue of spray-dried porous microparticles. The obtained materials have high surface areas (315–510 m2 g−1) and large pore volumes (0.64–1.0 cm3 g−1), which are dependent on RS concentration, HCl concentration, silica precursor hydrolysis time and drying temperature. The representative materials are promising for the adsorption of lysozyme. The adsorption occurs at a >three-fold faster rate, in a five-fold larger capacity (an increase from 20 to 100 mg g−1) and without pore blockage compared with the adsorption of lysozyme onto spray-dried microparticles of similar physicochemical properties obtained without the use of RS.

KW - Bio-adsorption

KW - Hierarchical structure

KW - Particle processing

KW - Porous silica

KW - Spray drying

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