Dissertation (Ph.D.)--Auburn University,2006. / Abstract. Vita. Includes bibliographic references (p.138-140).

Thesis--Auburn University, 2008. / Abstract. Vita. Includes bibliographical references (p. 85-90).

Microbial cross-contamination remains an on-going challenge in the food sector despite implemented sanitation programs. Antimicrobial coatings with inherent self-sanitizing properties have been explored to enhance current cleaning practice and support food safety. Prior work has demonstrated successful incorporation of dual antimicrobial characters, cationic polymers and N-halamines, into one coating system. In addition to the rechargeable nature of N-halamines, the coating was reported to exhibit biocidal effects due to the inherently antimicrobial cationic moieties and the chlorinated N-halamines. However, while these polymer coatings were able to retain antimicrobial activity after repeated chlorination, signs of hydrolysis was observed for the N-halamine bonds, indicating potential issues for long-term usage. Herein, we introduced varied molecular weight cross-linkers in an adaption of the established fabrication method to evaluate cross-linker molecular weight (styrene maleic anhydride (SMA) of 6, 8, 120, 250 kDa) influence on surface properties of the coating. All antimicrobial polymer coatings exhibited similar FTIR spectra, with a prominent absorption band at ~1650 cm-1 suggesting successful cross-link of the polyethyleneimine and SMA. Surface concentration of primary amines ranged from 350-900 nmol/cm2, and N-halamines from 90-130 nmol/cm2. Surface energy decreased with increasing molecular weight of SMA, but were not statistically different from one another. In the end, optimal cross-linker molecular weight was determined based on antimicrobial performance, where the coated PPs with 6 kDa SMAs demonstrated enhanced biocidal effects against E. coli O157:H7 in its chlorinated form. Further, the antimicrobial coating demonstrated efficacy of ~3 to >5 log reductions of microbial load in its unchlorinated and chlorinated form against E. coli O157:H7, L. monocytogenes, and P. fluorescens. Storage studies support the stability of the chlorinated halamines, with full retention of chlorinated N-halamines over a 24 h study (representative of time between sanitation cycles). These results support the potential application of this antimicrobial polymer coating in food processing and handling operations, in support of reducing cross-contamination of spoilage and pathogenic microorganisms.

Antimicrobial coatings in which the active agent (e.g. N-halamine) can regenerate activity represent a promising way to prevent microbial cross-contamination. A reported method for applying coatings containing antimicrobial N-halamines is layer-by-layer (LbL) application of polyelectrolytes, which form N-halamines upon cross-linking. Prior reports on dip layer-by-layer (LbL) fabrication have demonstrated the potential of this coating technology; however, spray LbL fabrication would enable more rapid coating and represents a more commercially translatable application technique. In this work, dip and spray LbL methods were used to coat polypropylene (PP) with N-halamine containing bilayers consisting of cross-linked polyethylenimine (PEI) and poly(acrylic acid) (PAA). Further experimentation with spray LbL fabrication used naturally occurring polyelectrolytes, chitosan and alginate. Materials were characterized using atomic force microscopy (AFM), ellipsometry, contact angle, fourier transform infrared spectroscopy, a chlorine content assay, and a dye assay for amine quantification. All methods of coating application exhibited a 99.999% (5-log) reduction against Listeria monocytogenes with application time for spray LbL taking less than 10% of the time required for dip LbL. Spray LbL fabrication of N-halamines is a rapid and inexpensive method to fabricate rechargeable antimicrobial surfaces.