[en] An original experimental set-up combining a FTIR microscope with a high pressure cell has been built in order to analyze in-situ the impregnation of solute into microscopic polymer samples, such as fibers or films, subjected to supercritical CO2. Thanks to this experimental set-up, key factors governing the impregnation process can be simultaneously followed such as the swelling of the polymeric matrix, the CO2 sorption, the kinetic of impregnation and the drug loading into the matrix. Moreover, the solute/polymer interactions and the speciation of the solute can be analyzed. We have monitored in situ the impregnation of aspirin and ketoprofen into PEO (Polyethylene Oxide) platelets at T=40°C and P=5; 10 and 15 MPa. The kinetic of impregnation of aspirin was quicker than the one of ketoprofen and the final drug loading was also higher in case of aspirin. Whereas the CO2 sorption and the PEO swelling remain constant when PEO is just subjected to CO2 under isobaric conditions, we noticed that both parameters can increase while the drug impregnates PEO. Coupling these results with DSC measurements, we underlined the plasticizing effect of the drug that also leads to decrease the crystallinity of PEO in situ thus favoring the sorption of CO2 molecules into the matrix and the swelling of the matrix. The plasticizing effect increases with the drug loading. Finally, the speciation of drug was investigated considering the shift of the carboxyl bands of the drugs. Both drugs were found to be mainly homogeneously dispersed into PEO.
Research center :
Center for Education and Research on Macromolecules (CERM)
Disciplines :
Materials science & engineering Chemistry
Author, co-author :
Champeau, Mathilde ; University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Thomassin, Jean-Michel ; University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Jérôme, Christine ; University of Liège - ULiège > Department of Chemistry > Center for Education and Research on Macromolecules (CERM)
Tassaing, Thierry; University of Bordeaux, Institute of Molecular Sciences, France
Language :
English
Title :
In situ investigation of scCO2 assisted impregnation of drug into polymer by high pressure FTIR micro-spectroscopy
Publication date :
07 February 2015
Journal title :
Analyst
ISSN :
0003-2654
eISSN :
1364-5528
Publisher :
Royal Society of Chemistry, Cambridge, United Kingdom
Volume :
140
Issue :
3
Pages :
869-879
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
Conseil Général d'Aquitaine [FR] The International Doctoral School IDS-Funmat
B. Bonavoglia, G. Storti, M. Morbidelli, A. Rajendran and M. Mazzotti, J. Polym. Sci., Part B: Polym. Phys., 2006, 44, 1531-1546.
Z. Lei, H. Ohyabu, Y. Sato, H. Inomata and R. L. Smith Jr, J. Supercrit. Fluids, 2007, 40, 452-461.
R. G. Wissinger and M. E. Paulaitis, J. Polym. Sci., Part B: Polym. Phys., 1991, 29, 631-633.
A. R. Berens, G. S. Huvard, R. W. Korsmeyer and F. W. Kunig, J. Appl. Polym. Sci., 1992, 46, 231-242.
A. I. Cooper, S. G. Kazarian and M. Poliakoff, Chem. Phys. Lett., 1993, 206, 175-180.
S. G. Kazarian, N. H. Brantley, B. L. West, M. F. Vincent and C. A. Eckert, Appl. Spectrosc., 1997, 51, 491-494.
N. H. Brantley, D. Bush, S. G. Kazarian and C. A. Eckert, J. Phys. Chem. B, 1999, 103, 10007-10016.
S. Ugaonkar, T. E. Needham and G. D. Bothun, Int. J. Pharm., 2011, 403, 96-100.
C. Zhao, S. Okubayashi, T. Suzuma, K. Hirogaki, I. Tabata and T. Hori, Sen'i Gakkaishi, 2011, 67, 34-39.
M. Banchero, Color. Technol., 2013, 129, 2-17.
D. Li and B. Han, Ind. Eng. Chem. Res., 2000, 39, 4506-4509.
O. Muth, T. Hirth and H. Vogel, J. Supercrit. Fluids, 2000, 17, 65-72.
A. R. C. Duarte, J. F. Mano and R. L. Reis, Eur. Polym. J., 2009, 45, 141-148.
M. E. M. Braga, V. P. Costa, M. J. T. Pereira, P. T. Fiadeiro, A. P. A. R. Gomes, C. M. M. Duarte and H. C. De Sousa, Int. J. Pharm., 2011, 420, 231-243.
C. González-Chomón, M. E. M. Braga, H. C. De Sousa, A. Concheiro and C. Alvarez-Lorenzo, Eur. J. Pharm. Biopharm., 2012, 82, 383-391.
Y. A. Hussain and C. S. Grant, J. Supercrit. Fluids, 2012, 71, 127-135.
S. L. Ma, Z. W. Lu, Y. T. Wu and Z. B. Zhang, J. Supercrit. Fluids, 2010, 54, 129-136.
Y. Masmoudi, L. Ben Azzouk, O. Forzano, J. M. Andre and E. Badens, J. Supercrit. Fluids, 2011, 60, 98-105.
A. R. C. Duarte, L. E. Anderson, C. M. M. Duarte and S. G. Kazarian, J. Supercrit. Fluids, 2005, 36, 160-165.
W. Saus, D. Knittel and E. Schollmeyer, Text. Res. J., 1993, 63, 135-142.
Z. Shen, G. S. Huvard, C. S. Warriner, M. Mc Hugh, J. L. Banyasz and M. K. Mishra, Polymer, 2008, 49, 1579-1586.
P. Vitoux, T. Tassaing, F. Cansell, S. Marre and C. Aymonier, J. Phys. Chem. B, 2009, 113, 897-905.
T. Guadagno and S. G. Kazarian, J. Phys. Chem. B, 2004, 108, 13995-13999.
M. Champeau, J. M. Thomassin, C. Jérôme and T. Tassaing, J. Supercrit. Fluids, 2014, 90, 44-52.
Z. Huang, W. D. Lu, S. Kawi and Y. C. Chiew, J. Chem. Eng. Data, 2004, 49, 1323-1327.
A. Stassi, R. Bettini, A. Gazzaniga, F. Giordano and A. Schiraldi, J. Chem. Eng. Data, 2000, 45, 161-165.
L. Manna, M. Banchero, D. Sola, A. Ferri, S. Ronchetti and S. Sicardi, J. Supercrit. Fluids, 2007, 42, 378-384.
G. Herzberg, Molecular Spectra and Molecular Structure: Infrared and Raman Spectra of Polyatomic Molecules, D. Van Nostrand Company, Inc., Princeton, New Jersey, 1956.
N. H. Brantley, S. G. Kazarian and C. A. Eckert, J. Appl. Polym. Sci., 2000, 77, 764-775.
K. L. A. Chan and S. G. Kazarian, Anal. Chem., 2013, 85, 1029-1036.
NIST, http://webbook.nist.gov/chemistry/.
S. Foltran, E. Cloutet, H. Cramail and T. Tassaing, J. Supercrit. Fluids, 2012, 63, 52-58.
S. Foltran, L. Maisonneuve, E. Cloutet, B. Gadenne, C. Alfos, T. Tassaing and H. Cramail, Polym. Chem., 2012, 3, 525-532.
R. Oparin, T. Tassaing, Y. Danten and M. Besnard, J. Chem. Phys., 2005, 122, 94505-94512.
S. Üzer, U. Akman and O. Hortac¸su, J. Supercrit. Fluids, 2006, 38, 119-128.
A. López-Periago, A. Argemi, J. M. Andanson, V. Fernandez, C. A. Garcia-Gonzalez, S. G. Kazarian, J. Saurina and C. Domingo, J. Supercrit. Fluids, 2009, 48, 56-63.
S. Yoda, K. Sato and H. T. Oyama, RSC Adv., 2011, 1, 156-162.
M. F. Vincent, S. G. Kazarian, B. L. West, J. A. Berkner, F. V. Bright, C. L. Liotta and C. A. Eckert, J. Phys. Chem. B, 1998, 102, 2176-2186.
J. Ke, S. Jin, B. Han, H. Yan and D. Shen, J. Supercrit. Fluids, 1997, 11, 53-60.
K. L. A. Chan and S. G. Kazarian, J. Comb. Chem., 2006, 8, 26-31.
A. Cortesi, P. Alessi, I. Kikic, S. Kirchmayer and F. Vecchione, J. Supercrit. Fluids, 2000, 19, 61-68.
S. G. Kazarian and G. G. Martirosyan, Int. J. Pharm., 2002, 232, 81-90.