Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs

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Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs. / Kissi, Eric Ofosu; Ruggiero, Michael T.; Hempel, Nele Johanna; Song, Zihui; Grohganz, Holger; Rades, Thomas; Löbmann, Korbinian.

In: Physical Chemistry Chemical Physics, Vol. 21, No. 35, 01.01.2019, p. 19686-19694.

Research output: Contribution to journalJournal articlepeer-review

Harvard

Kissi, EO, Ruggiero, MT, Hempel, NJ, Song, Z, Grohganz, H, Rades, T & Löbmann, K 2019, 'Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs', Physical Chemistry Chemical Physics, vol. 21, no. 35, pp. 19686-19694. https://doi.org/10.1039/c9cp01764j

APA

Kissi, E. O., Ruggiero, M. T., Hempel, N. J., Song, Z., Grohganz, H., Rades, T., & Löbmann, K. (2019). Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs. Physical Chemistry Chemical Physics, 21(35), 19686-19694. https://doi.org/10.1039/c9cp01764j

Vancouver

Kissi EO, Ruggiero MT, Hempel NJ, Song Z, Grohganz H, Rades T et al. Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs. Physical Chemistry Chemical Physics. 2019 Jan 1;21(35):19686-19694. https://doi.org/10.1039/c9cp01764j

Author

Kissi, Eric Ofosu ; Ruggiero, Michael T. ; Hempel, Nele Johanna ; Song, Zihui ; Grohganz, Holger ; Rades, Thomas ; Löbmann, Korbinian. / Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs. In: Physical Chemistry Chemical Physics. 2019 ; Vol. 21, No. 35. pp. 19686-19694.

Bibtex

@article{82979253ab104cabbfa8031c4f68bc4d,
title = "Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs",
abstract = "In this study the glass transition temperatures (Tgα and Tgβ) in mesoporous silica-based amorphous drugs were characterized. For this purpose, mesoporous silica Parteck SLC (MPS) was loaded with the drugs ibuprofen and carvedilol, either below, at, or above the monomolecular drug loading capacities, i.e. the concentration at which the entire MPS surface is covered with a monolayer of drug molecules. The resulting amorphous forms were analysed using X-ray powder diffraction and the thermal behaviour was characterised with differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA). The drug monolayer did not contribute to the thermal signal in DSC. Using DMA however, it could be shown that the monolayer indeed exhibited a very weak Tgα, and that the temperature range of this transition did not differ from that of the quench cooled amorphous drugs. Theoretical ab initio molecular dynamics simulations revealed that the nature of hydrogen bonding geometry of the functional groups interacting with the MPS surface were similar to that of the respective crystalline drugs, which results in restricted molecular motions for those functional groups. On the other hand, the non-interacting parts of the molecules exhibited molecular motions similar to what is observed in pure amorphous drugs. As a result of the interactions of the monolayer with the MPS surface, the monomolecular drug layer did not reveal a Tgβ. However, a Tgβ was found at any drug-MPS ratios above the monomolecular drug loading capacity as a result of the excess drug which forms a {"}true{"} amorphous phase. Overall, this study demonstrated that drug molecules forming an amorphous monolayer on the surfaces of a mesoporous silica particle, even though they are restricted in their mobility, exhibit a Tgα, but lack a Tgβ, whereas any excess drug confined in the MPS pores showed similar properties as the pure amorphous drug. These findings will help to increase the overall understanding of drug loaded MS systems, including their physical stability as well as release properties.",
author = "Kissi, {Eric Ofosu} and Ruggiero, {Michael T.} and Hempel, {Nele Johanna} and Zihui Song and Holger Grohganz and Thomas Rades and Korbinian L{\"o}bmann",
year = "2019",
month = jan,
day = "1",
doi = "10.1039/c9cp01764j",
language = "English",
volume = "21",
pages = "19686--19694",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Royal Society of Chemistry",
number = "35",

}

RIS

TY - JOUR

T1 - Characterising glass transition temperatures and glass dynamics in mesoporous silica-based amorphous drugs

AU - Kissi, Eric Ofosu

AU - Ruggiero, Michael T.

AU - Hempel, Nele Johanna

AU - Song, Zihui

AU - Grohganz, Holger

AU - Rades, Thomas

AU - Löbmann, Korbinian

PY - 2019/1/1

Y1 - 2019/1/1

N2 - In this study the glass transition temperatures (Tgα and Tgβ) in mesoporous silica-based amorphous drugs were characterized. For this purpose, mesoporous silica Parteck SLC (MPS) was loaded with the drugs ibuprofen and carvedilol, either below, at, or above the monomolecular drug loading capacities, i.e. the concentration at which the entire MPS surface is covered with a monolayer of drug molecules. The resulting amorphous forms were analysed using X-ray powder diffraction and the thermal behaviour was characterised with differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA). The drug monolayer did not contribute to the thermal signal in DSC. Using DMA however, it could be shown that the monolayer indeed exhibited a very weak Tgα, and that the temperature range of this transition did not differ from that of the quench cooled amorphous drugs. Theoretical ab initio molecular dynamics simulations revealed that the nature of hydrogen bonding geometry of the functional groups interacting with the MPS surface were similar to that of the respective crystalline drugs, which results in restricted molecular motions for those functional groups. On the other hand, the non-interacting parts of the molecules exhibited molecular motions similar to what is observed in pure amorphous drugs. As a result of the interactions of the monolayer with the MPS surface, the monomolecular drug layer did not reveal a Tgβ. However, a Tgβ was found at any drug-MPS ratios above the monomolecular drug loading capacity as a result of the excess drug which forms a "true" amorphous phase. Overall, this study demonstrated that drug molecules forming an amorphous monolayer on the surfaces of a mesoporous silica particle, even though they are restricted in their mobility, exhibit a Tgα, but lack a Tgβ, whereas any excess drug confined in the MPS pores showed similar properties as the pure amorphous drug. These findings will help to increase the overall understanding of drug loaded MS systems, including their physical stability as well as release properties.

AB - In this study the glass transition temperatures (Tgα and Tgβ) in mesoporous silica-based amorphous drugs were characterized. For this purpose, mesoporous silica Parteck SLC (MPS) was loaded with the drugs ibuprofen and carvedilol, either below, at, or above the monomolecular drug loading capacities, i.e. the concentration at which the entire MPS surface is covered with a monolayer of drug molecules. The resulting amorphous forms were analysed using X-ray powder diffraction and the thermal behaviour was characterised with differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA). The drug monolayer did not contribute to the thermal signal in DSC. Using DMA however, it could be shown that the monolayer indeed exhibited a very weak Tgα, and that the temperature range of this transition did not differ from that of the quench cooled amorphous drugs. Theoretical ab initio molecular dynamics simulations revealed that the nature of hydrogen bonding geometry of the functional groups interacting with the MPS surface were similar to that of the respective crystalline drugs, which results in restricted molecular motions for those functional groups. On the other hand, the non-interacting parts of the molecules exhibited molecular motions similar to what is observed in pure amorphous drugs. As a result of the interactions of the monolayer with the MPS surface, the monomolecular drug layer did not reveal a Tgβ. However, a Tgβ was found at any drug-MPS ratios above the monomolecular drug loading capacity as a result of the excess drug which forms a "true" amorphous phase. Overall, this study demonstrated that drug molecules forming an amorphous monolayer on the surfaces of a mesoporous silica particle, even though they are restricted in their mobility, exhibit a Tgα, but lack a Tgβ, whereas any excess drug confined in the MPS pores showed similar properties as the pure amorphous drug. These findings will help to increase the overall understanding of drug loaded MS systems, including their physical stability as well as release properties.

U2 - 10.1039/c9cp01764j

DO - 10.1039/c9cp01764j

M3 - Journal article

C2 - 31469369

AN - SCOPUS:85072057533

VL - 21

SP - 19686

EP - 19694

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 35

ER -

ID: 236717311