TY - JOUR
T1 - Impact of PEGylation on the degradation and pore organization in mesoporous silica nanoparticles
T2 - A study of the inner mesoporous structure in physiologically relevant ionic conditions
AU - Ramírez, María de los Ángeles
AU - Bindini, Elisa
AU - Moretti, Paolo
AU - Soler Illia, Galo J.A.A.
AU - Amenitsch, Heinz
AU - Andreozzi, Patrizia
AU - Ortore, Maria Grazia
AU - Moya, Sergio E.
N1 - Funding Information:
The authors thank Elettra Synchrotron for beamtime allocation and acknowledge the CERIC-ERIC Consortium for the access (20192044 proposal code) to experimental facilities. S.E.M. thanks the PID2020-114356RB-I00 project from the Ministry of Science and Innovation of the Government of Spain. G.S.I. acknowledges support from ANPCyT (PICT 2015-2526 and PICT 2018-4651). This work was performed under the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency - Grant no. MDM-2017-0720. P.A. acknowledges MIUR-Italy (“Progetto Dipartimenti di Eccellenza 2018-2022” funding allocated to the Department of Chemistry “Ugo Schiff”). We acknowledge Julia Cope, PhD from CIC biomaGUNE for kindly revising the manuscript.
Funding Information:
The authors thank Elettra Synchrotron for beamtime allocation and acknowledge the CERIC-ERIC Consortium for the access (20192044 proposal code) to experimental facilities. S.E.M. thanks the PID2020-114356RB-I00 project from the Ministry of Science and Innovation of the Government of Spain. G.S.I. acknowledges support from ANPCyT (PICT 2015-2526 and PICT 2018-4651 ). This work was performed under the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency - Grant no. MDM-2017-0720 . P.A. acknowledges MIUR-Italy (“Progetto Dipartimenti di Eccellenza 2018-2022” funding allocated to the Department of Chemistry “Ugo Schiff”). We acknowledge Julia Cope, PhD from CIC biomaGUNE for kindly revising the manuscript.
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/11
Y1 - 2022/11
N2 - The degradation of mesoporous silica nanoparticles (MSNs) in the biological milieu due to silica hydrolysis plays a fundamental role for the delivery of encapsulated drugs and therapeutics. However, little is known on the evolution of the pore arrangement in the MSNs in biologically relevant conditions. Small Angle X-ray scattering (SAXS) studies were performed on unmodified and PEGylated MSNs with a MCM-48 pore structure and average sizes of 140 nm, exposed to simulated body fluid solution (SBF) at pH 7.4 for different time intervals from 30 min to 24 h. Experiments were performed with silica concentrations below, at and over 0.14 mg/mL, the saturation concentration of silica in water at physiological temperature. At silica concentrations of 1 mg/mL (oversaturation), unmodified MSNs show variation in interpore distances over 6 h exposure to SBF, remaining constant thereafter. A decrease in radius of gyration is observed over the same time. Mesoporosity and radius of gyration of unmodified MSNs remain then unchanged up to 24 h. PEGylated MSNs at 1 mg/mL concentration show a broader diffraction peak but no change in the position of the peak is observed following 24 h exposure to SBF. PEGylated MSNs at 0.01 mg/mL show no diffraction peaks already after 30 min exposure to SBF, while at 0.14 mg/mL a small diffraction peak is present after 30 min exposure but disappears after 1 h.
AB - The degradation of mesoporous silica nanoparticles (MSNs) in the biological milieu due to silica hydrolysis plays a fundamental role for the delivery of encapsulated drugs and therapeutics. However, little is known on the evolution of the pore arrangement in the MSNs in biologically relevant conditions. Small Angle X-ray scattering (SAXS) studies were performed on unmodified and PEGylated MSNs with a MCM-48 pore structure and average sizes of 140 nm, exposed to simulated body fluid solution (SBF) at pH 7.4 for different time intervals from 30 min to 24 h. Experiments were performed with silica concentrations below, at and over 0.14 mg/mL, the saturation concentration of silica in water at physiological temperature. At silica concentrations of 1 mg/mL (oversaturation), unmodified MSNs show variation in interpore distances over 6 h exposure to SBF, remaining constant thereafter. A decrease in radius of gyration is observed over the same time. Mesoporosity and radius of gyration of unmodified MSNs remain then unchanged up to 24 h. PEGylated MSNs at 1 mg/mL concentration show a broader diffraction peak but no change in the position of the peak is observed following 24 h exposure to SBF. PEGylated MSNs at 0.01 mg/mL show no diffraction peaks already after 30 min exposure to SBF, while at 0.14 mg/mL a small diffraction peak is present after 30 min exposure but disappears after 1 h.
KW - Degradation
KW - Mesoporous silica nanoparticles
KW - PEGylation
KW - SAXS
KW - Simulated body fluid
UR - http://www.scopus.com/inward/record.url?scp=85137153296&partnerID=8YFLogxK
U2 - 10.1016/j.colsurfb.2022.112797
DO - 10.1016/j.colsurfb.2022.112797
M3 - Article
C2 - 36063718
AN - SCOPUS:85137153296
VL - 219
JO - Colloids and Surfaces / B
JF - Colloids and Surfaces / B
SN - 0927-7765
M1 - 112797
ER -