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Title: Adsorption and Recovery of Polyphenolic Flavonoids Using TiO 2-Functionalized Mesoporous Silica Nanoparticles

Exploiting specific interactions with titania (TiO 2) has been proposed for the separation and recovery of a broad range of biomolecules and natural products, including therapeutic polyphenolic flavonoids which are susceptible to degradation, such as quercetin. Functionalizing mesoporous silica with TiO 2 has many potential advantages over bulk and mesoporous TiO 2 as an adsorbent for natural products, including robust synthetic approaches leading to high surface area, stable separation platforms. Here, TiO 2 surface functionalized mesoporous silica nanoparticles (MSNPs) are synthesized and characterized as a function of TiO 2 content (up to 636 mg TiO2/g). The adsorption isotherms of two polyphenolic flavonoids, quercetin and rutin, were determined (0.05-10 mg/ml in ethanol), and a 100-fold increase in the adsorption capacity was observed relative to functionalized nonporous particles with similar TiO 2 surface coverage. An optimum extent of functionalization (approximately 440 mg TiO 2/g particles) is interpreted from characterization techniques including grazing incidence x-ray scattering (GIXS), high resolution transmission electron microscopy (HRTEM) and nitrogen adsorption, which examined the interplay between the extent of TiO 2 functionalization and the accessibility of the porous structures. The recovery of flavonoids is demonstrated using ligand displacement in ethanolic citric acid solution (20% w/v), in which greatermore » than 90% recovery can be achieved in a multistep extraction process. The radical scavenging activity (RSA) of the recovered and particle-bound quercetin as measured by 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical scavenging assay demonstrates greater than 80% retention of antioxidant activity by both particle-bound and recovered quercetin. In conclusion, these mesoporous titanosilicate materials can serve as a synthetic platform to isolate, recover, and potentially deliver degradation-sensitive natural products to biological systems.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Univ. of Kentucky, Lexington, KY (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Naprogenix Inc., Lexington, KY (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 37; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; adsorption; flavonoid; functionalization; silica nanoparticles; stability
OSTI Identifier:
1395148

Khan, M. Arif, Wallace, William T., Islam, Syed Z., Nagpure, Suraj, Strzalka, Joseph, Littleton, John M., Rankin, Stephen E., and Knutson, Barbara L.. Adsorption and Recovery of Polyphenolic Flavonoids Using TiO2-Functionalized Mesoporous Silica Nanoparticles. United States: N. p., Web. doi:10.1021/acsami.7b09510.
Khan, M. Arif, Wallace, William T., Islam, Syed Z., Nagpure, Suraj, Strzalka, Joseph, Littleton, John M., Rankin, Stephen E., & Knutson, Barbara L.. Adsorption and Recovery of Polyphenolic Flavonoids Using TiO2-Functionalized Mesoporous Silica Nanoparticles. United States. doi:10.1021/acsami.7b09510.
Khan, M. Arif, Wallace, William T., Islam, Syed Z., Nagpure, Suraj, Strzalka, Joseph, Littleton, John M., Rankin, Stephen E., and Knutson, Barbara L.. 2017. "Adsorption and Recovery of Polyphenolic Flavonoids Using TiO2-Functionalized Mesoporous Silica Nanoparticles". United States. doi:10.1021/acsami.7b09510. https://www.osti.gov/servlets/purl/1395148.
@article{osti_1395148,
title = {Adsorption and Recovery of Polyphenolic Flavonoids Using TiO2-Functionalized Mesoporous Silica Nanoparticles},
author = {Khan, M. Arif and Wallace, William T. and Islam, Syed Z. and Nagpure, Suraj and Strzalka, Joseph and Littleton, John M. and Rankin, Stephen E. and Knutson, Barbara L.},
abstractNote = {Exploiting specific interactions with titania (TiO2) has been proposed for the separation and recovery of a broad range of biomolecules and natural products, including therapeutic polyphenolic flavonoids which are susceptible to degradation, such as quercetin. Functionalizing mesoporous silica with TiO2 has many potential advantages over bulk and mesoporous TiO2 as an adsorbent for natural products, including robust synthetic approaches leading to high surface area, stable separation platforms. Here, TiO2 surface functionalized mesoporous silica nanoparticles (MSNPs) are synthesized and characterized as a function of TiO2 content (up to 636 mg TiO2/g). The adsorption isotherms of two polyphenolic flavonoids, quercetin and rutin, were determined (0.05-10 mg/ml in ethanol), and a 100-fold increase in the adsorption capacity was observed relative to functionalized nonporous particles with similar TiO2 surface coverage. An optimum extent of functionalization (approximately 440 mg TiO2/g particles) is interpreted from characterization techniques including grazing incidence x-ray scattering (GIXS), high resolution transmission electron microscopy (HRTEM) and nitrogen adsorption, which examined the interplay between the extent of TiO2 functionalization and the accessibility of the porous structures. The recovery of flavonoids is demonstrated using ligand displacement in ethanolic citric acid solution (20% w/v), in which greater than 90% recovery can be achieved in a multistep extraction process. The radical scavenging activity (RSA) of the recovered and particle-bound quercetin as measured by 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical scavenging assay demonstrates greater than 80% retention of antioxidant activity by both particle-bound and recovered quercetin. In conclusion, these mesoporous titanosilicate materials can serve as a synthetic platform to isolate, recover, and potentially deliver degradation-sensitive natural products to biological systems.},
doi = {10.1021/acsami.7b09510},
journal = {ACS Applied Materials and Interfaces},
number = 37,
volume = 9,
place = {United States},
year = {2017},
month = {8}
}