title: Biodegradable DNA-enabled poly(ethylene glycol) hydrogels prepared by copper-free click chemistry.
abstract: Significant research has focused on investigating the potential of hydrogels in various applications and, in particular, in medicine. Specifically, hydrogels that are biodegradable lend promise to many therapeutic and biosensing applications. Endonucleases are critical for mechanisms of DNA repair. However, they are also known to be overexpressed in cancer and to be present in wounds with bacterial contamination. In this work, we set out to demonstrate the preparation of DNA-enabled hydrogels that could be degraded by nucleases. Specifically, hydrogels were prepared through the reaction of dibenzocyclooctyne-functionalized multi-arm poly(ethylene glycol) with azide-functionalized single-stranded DNA in aqueous solutions via copper-free click chemistry. Through the use of this method, biodegradable hydrogels were formed at room temperature in buffered saline solutions that mimic physiological conditions, avoiding possible harmful effects associated with other polymerization techniques that can be detrimental to cells or other bioactive molecules. The degradation of these DNA-cross-linked hydrogels upon exposure to the model endonucleases Benzonase(®) and DNase I was studied. In addition, the ability of the hydrogels to act as depots for encapsulation and nuclease-controlled release of a model protein was demonstrated. This model has the potential to be tailored and expanded upon for use in a variety of applications where mild hydrogel preparation techniques and controlled material degradation are necessary including in drug delivery and wound healing systems.
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.
authors.forename: Karolyn
authors.initials: K
authors.lastname: Barker
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.
authors.forename: Shiva K
authors.initials: SK
authors.lastname: Rastogi
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.
authors.forename: Jose
authors.initials: J
authors.lastname: Dominguez
authors.affiliation: b Materials Science, Engineering, and Commercialization Program , Texas State University , San Marcos , TX , USA.
authors.forename: Travis
authors.initials: T
authors.lastname: Cantu
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.
authors.forename: William
authors.initials: W
authors.lastname: Brittain
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.|b Materials Science, Engineering, and Commercialization Program , Texas State University , San Marcos , TX , USA.
authors.forename: Jennifer
authors.initials: J
authors.lastname: Irvin
authors.affiliation: a Department of Chemistry and Biochemistry , Texas State University , San Marcos , TX , USA.|b Materials Science, Engineering, and Commercialization Program , Texas State University , San Marcos , TX , USA.
authors.forename: Tania
authors.initials: T
authors.lastname: Betancourt
mesh_terms: D020341:Absorbable Implants; D057930:Click Chemistry; D004277:DNA, Single-Stranded / Q000737:chemistry*; D003850:Deoxyribonuclease I / Q000737:chemistry; D004343:Drug Implants / Q000138:chemical synthesis / Q000737:chemistry; D004706:Endodeoxyribonucleases / Q000737:chemistry; D004722:Endoribonucleases / Q000737:chemistry; D016650:Fluorescein-5-isothiocyanate / Q000008:administration & dosage / Q000031:analogs & derivatives; D020100:Hydrogels / Q000138:chemical synthesis* / Q000737:chemistry*; D008422:Materials Testing; D008855:Microscopy, Electron, Scanning; D061848:Optical Imaging; D011092:Polyethylene Glycols / Q000737:chemistry*; D012710:Serum Albumin, Bovine / Q000008:administration & dosage; D012996:Solutions; D013057:Spectrum Analysis; D013696:Temperature; D014867:Water / Q000737:chemistry; D014945:Wound Healing
chemical_list: D004277:DNA, Single-Stranded; D004343:Drug Implants; D020100:Hydrogels; D012996:Solutions; C039217:fluorescein isothiocyanate bovine serum albumin; D014867:Water; D012710:Serum Albumin, Bovine; D011092:Polyethylene Glycols; D004706:Endodeoxyribonucleases; D004722:Endoribonucleases; D003850:Deoxyribonuclease I; C021835:Serratia marcescens nuclease; D016650:Fluorescein-5-isothiocyanate
keywords: Biodegradation; DNA; click chemistry; hydrogel; nuclease-mediated degradation; protein release; stimuli-responsive biomaterials