A key issue that researchers in the biomaterials field face today is biocompatibility of artificial implants in human bodies. Protein adsorption followed by cell adhesion and various undesirable biological responses occur when most foreign objects contact body fluid. Designing surfaces that proteins do not adsorb to is the primary approach in improving biocompatibility of biomaterials. Of the few existing biocompatible materials, poly(ethylene glycol) (PEG) and phosphorylcholine-containing molecules are the most well-recognized and studied. The exploration of new materials for potential biomedical applications is a responsibility that is imperative for materials scientists to address. In the proposed work, surface-initiated ring-opening metathesis polymerization (SiROMP) of cyclic olefins in the vapor phase and subsequent hydroxylation reaction will be assessed as an approach to tether new materials to silicon substrates. SiROMP is an effective method to covalently attach functionalized linear polymer chains to substrates, however, the reported monomers undergoing SiROMP in solution have been limited to norbornene and its derivatives. Vapor phase SiROMP of cyclic olefins of varying degrees of ring strain (cyclopentene, cycloheptene, and cyclooctene) and of different degrees of unsaturation (cyclooctene, cyclooctadiene, and cyclooctatetraene) will be carried out in the proposed work. The tethered unsaturated polymers will be hydroxylated to yield alcohol-functionalized polymers; the -OH group density will be controlled by the ring size and the degree of unsaturation of the cyclic olefins used. The molecular weight of the polymers will be tuned by grafting time. Wettability and protein adsorption characteristics will be correlated to the molecular weight and the -OH group density along the hydroxylated polymer chains. The protein adsorption characteristics of these new materials will be compared to those of well-recognized biomaterials, such as PEG. With the proposed research we hope to open up new opportunities for the design of bio-relevant materials. The exploration of new materials for potential biomedical applications is a responsibility that is imperative for materials scientists to address. Alcohol-functionalized linear polymers with varying alcohol group densities will be designed and tethered to solid substrates by a new synthetic tool, surface-initiated ring-opening metathesis polymerization in the vapor phase of low ring-strain cyclic olefins, followed by hydroxylation of the unsaturated polymers. Wettability and protein resistant characteristics of these new materials will be studied and correlated with their molecular weight and alcohol group densities. ? ? ?

Agency
National Institute of Health (NIH)
Institute
National Institute of Biomedical Imaging and Bioengineering (NIBIB)
Type
Academic Research Enhancement Awards (AREA) (R15)
Project #
2R15EB000139-02A1
Application #
7302999
Study Section
Biomaterials and Biointerfaces Study Section (BMBI)
Program Officer
Erim, Zeynep
Project Start
2002-06-01
Project End
2011-07-31
Budget Start
2007-08-01
Budget End
2011-07-31
Support Year
2
Fiscal Year
2007
Total Cost
$218,568
Indirect Cost
Name
Mount Holyoke College
Department
Chemistry
Type
Schools of Arts and Sciences
DUNS #
066985714
City
South Hadley
State
MA
Country
United States
Zip Code
01075
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Lerum, Maria Felisa Z; Chen, Wei (2011) Surface-initiated ring-opening metathesis polymerization in the vapor phase: an efficient method for grafting cyclic olefins with low strain energies. Langmuir 27:5403-9
Lerum, Maria Felisa Z; Chen, Wei (2009) Acute degradation of surface-bound unsaturated polyolefins in common solvents under ambient conditions. Langmuir 25:11250-4
Smith, Emily Asenath; Chen, Wei (2008) How to prevent the loss of surface functionality derived from aminosilanes. Langmuir 24:12405-9
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