BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Lecture 6: Programmed/Pulsed Drug Delivery and Drug Delivery in Tissue
Engineering
Last time: principles of controlled release from solid polymers
Today: Pulsatile/regulated/multifactor controlled release:
3 case studies of controlled release
Reading: ‘Polymeric system for dual growth factor delivery,’ T.P. Richardson et al., Nat. Biotech.
19, 1029-1034 (2001)
‘Microchips as controlled drug-delivery devices,’ J.T. Santini et al., Andegwandte Chemie
Intl. Ed. 39, 2396-2047 (2000)
Regulated controlled release
Applications of regulated and pulsatile release
? Definition: release of cargo in bursts followed by periods of little/no release in a defined temporal pattern
1
? Many applications would be best-served by non-monotonic and multi-cargo release profiles
o Motivation:
null Single injection delivery of ‘booster’ for vaccination
null Mimic natural secretion patterns of hormones
null Provide optimal therapy for tolerance-inducing drugs
? Constant drug levels cause receptor down-regulation
Vaccine boosting hormone release patterns in vivo
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
null Example: HIV-1 DNA vaccine delivered with boosters to elevate Ab titers
2
:
o Mechanical and electrical devices that can provide digitized release typically require larger devices and
surgical implantation (e.g. Pharm. Res. 1, 237 (1984)); also have high cost
null Show an example
o Degradable polymers allow submicron, injectable devices
? Two types
o Pre-programmed
null Release profile is encoded in structure and composition of device
o Triggered
null External signal drives release
Multilayer surface-eroding delivery devices
Case study: multilayered delivery devices
3
Fast-degrading Polyanhydride block
Hydrophilic PEG block
polyphosphazene
slow-degrading
polylactide block
? Polyphosphazene:
o Base-catalyzed degradation, acid-inhibited degradation
? PEG-b-Polyanhydride:
o Rapid bulk erosion- use hydrophilic block to make hrs-long degradation time for mm-thick caps (very fast)
o …becomes porous during erosion, so need a means to prevent next layer from starting to degrade as
water reaches drug-containing layer
o creates acidic byproducts as it degrades
? Function of complete device:
o First polyphosphazene layer: degrades quickly (first burst release)
o Polyanhydride layer: degrades quickly, acidifies internal environment
null Even though water penetrates the polyanhydride, no degradation of polyphosphazene begins and
no drug is released from the polyphosphazene layer until the polyanhydride has completely
eroded and acidic products are removed from microenvironment
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Polyanhydride layer acidifies
Water penetrates into device
Model drug release profiles:
environment as it degrades:
COO-
C
O
O
-
COO-
C
O
O-
COO-
C
O
O
-
Low pH
Polyphosphazene only degrades
quickly at neutral/basic pH :
? refs for theory: J Contr Rel 20, 201 (1992); J Cont Rel 18, 159 (1992)
Regulated release devices: case example- drug delivery microchips
? work from M. Cima and R. Langer labs:
4
Lecture 5 – Programmed Drug Delivery 3 of 12
BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
? Principle of a gold electrochemical cell in the presence of aqueous chloride solution:
o ON BOARD:
H
2
O, Na
+
Cl
-
Au cathode
Au anode
4 Cl
-
+ Au
[AuCl4]
-
3 e-
[AuCl4]
-
Au + 4 Cl
-
[AuCl4]
-
e-
3 e-
reduction oxidation
? In reality, multiple reactions occur simultaneously at the anode under an applied voltage in the ‘passive and
transpassive’ regime
5
:
o Au + 4Cl- -> [AuCl4]- + 3 e-
o Au + mH
2
O -> Au(H2O)
m
3+
+ 3 e-
o 2 Au + 3H
2
O -> Au
2
O
3
+ 6H
+
+ 6e-
o 2Cl
-
-> Cl
2
+ 2e-
o Au
2
O
3
+ 8Cl
-
+ 6H
+
-> 2[AuCl
4
]
-
+ 3H
2
O
? Design of anode:
o Need a material that is:
null stable in the presence of chloride ions in the absence of a potential
? many metals corrode with 0 applied potential in vivo
? many metals spontaneously form an oxide layer by reaction with water/O
2
in
physiological conditions
? in presence of potential, reacts to form a biocompatible soluble compound
? Pourbaix diagram: shows thermodynamically favored species under applied potential at varying pH
? Evans diagram: shows current produced due to electrochemical dissolution of the anode; the current is a
measure of the rate of electrons being produced and thus measures the kinetics of the reaction
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
o Shows that gold membranes corrode quickly
? Structure of the controlled release microchip:
o anode is a gold membrane 0.3 μm thick
o current limitation in design is size of battery needed to operate the device: ~ 1 cm
2
null microchip itself could be reduced to ~ 2 mmx 2mm
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Pourbaix diagram:
thermodynamic stability
1.6
1.2
0.8
E/V0.4
0.0
-0.4
-0.8
-1.2
[AuCl
4
]
Au(OH)
3
2 4 6 8 10 12
Au
pH
? WHY DOES GOLD DISSOLVE AT PH 7? POURBAIX DIAGRAM SHOWS OXIDE IS STABLE FORM
(Cima work)
6
? Release properties:
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Controlled Release in Tissue Engineering
Tissue Engineering/Regenerative Medicine
? 2 major approaches for regenerative medicine
o In vitro tissue genesis → in vivo application
o In vivo tissue genesis → in vivo application
Schematic comparison of in vitro and in vivo tissue engineering approaches
7
:
Skin: bone:
? Role of scaffold:
o Provide functions of native ECM
o Create a space for new tissue development
o Deliver cells to site
o Direct macroscopic size/shape of new tissue
? roles for soluble factor delivery in TE:
o chemoattractant gradients used to draw desired cell types into structure
o growth factors provided to induce cell proliferation to regenerate tissue
o cytokines to induce tissue-specific cell functions
Cytokine delivery from scaffolds
Case Study: Induction of vascularization in TE scaffolds
? Challenge of providing nutrients and oxygen to large tissue constructs
o Constructs ~500 μm thick or greater cannot be supported by diffusive transport- need vascularization
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Lecture 5 – Programmed Drug Delivery 8 of 12
? Structure of vasculature
O
2
O
2
O
2
z
pO
2
Blood flow
blood vessel structure:
Intima
(supportive ECM
layer)
Endothelial cell lining
Smooth muscle
cells
Extensive cell death
in center of construct
? Angiogenesis
8
Steps in angiogenesis:
1.
-attracts endothelial cells, induces proliferation
-induces tube formation
2.
-attracts smooth muscle cells, stabilizes new vessels
VEGF (vascular endothelial growth factor)
PDGF (platelet-derived growth factor)
BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
Lecture 5 – Programmed Drug Delivery 9 of 12
? Dual growth factor delivery from degradable scaffolds for de novo blood vessel synthesis
9
:
Compression
mold
PLGA particles
Lyophilized VEGF
PDGF-containing microspheres
NaCl particles
? Fabrication process:
10
o PDGF encapsulated in PLGA microspheres by double emulsion approach
o Microspheres (5-50 μm) mixed with PLGA particles (150-250 μm), NaCl particles (250-500 μm), and
lyophilized VEGF particles (5-50 μm) in mold and compression molded to form a solid disk
o Disk equilibrated with CO
2
at 800 psi 48hrs
o Pressure rapidly dropped to ambient (14 psi)
o Salt leached by soaking in distilled water 48 hrs
1. Fill with high-pressure CO
2
2. Rapidly depressurize
Soak with water to leach out NaCl
BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
? In vivo experiments:
o Scaffolds implanted subcutaneously in Lewis rats, examined histologically at 2 weeks and 4 weeks
o Comparisons:
null Free cytokine injections with scaffolds vs. controlled release scaffolds
null Dual vs. single factor controlled release scaffolds
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
o Bolus injection of free cytokines is ineffective:
blank
VEGF
VEGF +
PDGF
PDGF
2 weeks 4 weeks
o controlled release scaffolds induce formation of more blood vessels with larger diameters:
VEGF
VEGF +
PDGF
PDGF
2 weeks 4 weeks
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BEH.462/3.962J Molecular Principles of Biomaterials Spring 2003
o vessels formed in controlled release systems show smooth muscle actin staining indicative of mature
vessel formation:
400X 1,000X
blank
VEGF
VEGF +
PDGF
PDGF
References
1. Medlicott, N. J. & Tucker, I. G. Pulsatile release from subcutaneous implants. Adv Drug Deliv Rev 38, 139-149
(1999).
2. Robinson, H. L. et al. Neutralizing antibody-independent containment of immunodeficiency virus challenges by
DNA priming and recombinant pox virus booster immunizations. Nat Med 5, 526-34 (1999).
3. Qiu, L. Y. & Zhu, K. J. Design of a core-shelled polymer cylinder for potential programmable drug delivery. Int J
Pharm 219, 151-60 (2001).
4. Santini, J. T., Jr., Cima, M. J. & Langer, R. A controlled-release microchip. Nature 397, 335-8 (1999).
5. Frankenthal, R. P. & Siconolfi, D. J. The anodic corrosion of gold in concentrated chloride solutions. J.
Electrochem. Soc. 129, 1192-1196 (1982).
6. Santini Jr, J. T., Richards, A. C., Scheidt, R., Cima, M. J. & Langer, R. Microchips as Controlled Drug-Delivery
Devices. Angew Chem Int Ed Engl 39, 2396-2407 (2000).
7. Yannas, I. V. Tissue and Organ Regeneration in Adults (Springer, New York, 2001).
8. Darland, D. C. & D'Amore, P. A. Blood vessel maturation: vascular development comes of age. J Clin Invest 103,
157-8 (1999).
9. Richardson, T. P., Peters, M. C., Ennett, A. B. & Mooney, D. J. Polymeric system for dual growth factor delivery.
Nat Biotechnol 19, 1029-34 (2001).
10. Harris, L. D., Kim, B. S. & Mooney, D. J. Open pore biodegradable matrices formed with gas foaming. J Biomed
Mater Res 42, 396-402 (1998).
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