TY - JOUR
T1 - Green Light-Responsive CO-Releasing Polymeric Materials Derived from Ring-Opening Metathesis Polymerization
AU - Gandra, Upendar Reddy
AU - Sinopoli, Alessandro
AU - Moncho, Salvador
AU - Nandakumar, Manjula
AU - Ninković, Dragan B.
AU - Zarić, Snežana D.
AU - Sohail, Muhammad
AU - Al-Meer, Saeed
AU - Brothers, Edward N.
AU - Mazloum, Nayef A.
AU - Al-Hashimi, Mohammed
AU - Bazzi, Hassan S.
N1 - Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/9/18
Y1 - 2019/9/18
N2 - Carbon monoxide (CO) is an important biological gasotransmitter in living cells. Precise spatial and temporal control over release of CO is a major requirement for clinical application. To date, the most reported carbon monoxide releasing materials use expensive fabrication methods and require harmful and poorly designed tissue-penetrating UV irradiation to initiate the CO release precisely at infected sites. Herein, we report the first example of utilizing a green light-responsive CO-releasing polymer P synthesized via ring-opening metathesis polymerization. Both monomer M and polymer P were very stable under dark conditions and CO release was effectively triggered using minimal power and low energy wavelength irradiation (550 nm, ≤28 mW). Time-dependent density functional theory (TD-DFT) calculations were carried out to simulate the electronic transition and insight into the nature of the excitations for both L and M. TD-DFT calculations indicate that the absorption peak of M is mainly due to the excitation of the seventh singlet excited state, S7. Furthermore, stretchable materials using polytetrafluoroethylene (PTFE) strips based on P were fabricated to afford P-PTFE, which can be used as a simple, inexpensive, and portable CO storage bandage. Insignificant cytotoxicity as well as cell permeability was found for M and P against human embryonic kidney cells.
AB - Carbon monoxide (CO) is an important biological gasotransmitter in living cells. Precise spatial and temporal control over release of CO is a major requirement for clinical application. To date, the most reported carbon monoxide releasing materials use expensive fabrication methods and require harmful and poorly designed tissue-penetrating UV irradiation to initiate the CO release precisely at infected sites. Herein, we report the first example of utilizing a green light-responsive CO-releasing polymer P synthesized via ring-opening metathesis polymerization. Both monomer M and polymer P were very stable under dark conditions and CO release was effectively triggered using minimal power and low energy wavelength irradiation (550 nm, ≤28 mW). Time-dependent density functional theory (TD-DFT) calculations were carried out to simulate the electronic transition and insight into the nature of the excitations for both L and M. TD-DFT calculations indicate that the absorption peak of M is mainly due to the excitation of the seventh singlet excited state, S7. Furthermore, stretchable materials using polytetrafluoroethylene (PTFE) strips based on P were fabricated to afford P-PTFE, which can be used as a simple, inexpensive, and portable CO storage bandage. Insignificant cytotoxicity as well as cell permeability was found for M and P against human embryonic kidney cells.
KW - CO-releasing material (CORMat)
KW - carbon monoxide (CO)
KW - light-responsive
KW - polymer conjugates
KW - portable CO storage and CO release bandage
UR - http://www.scopus.com/inward/record.url?scp=85072508757&partnerID=8YFLogxK
U2 - 10.1021/acsami.9b12628
DO - 10.1021/acsami.9b12628
M3 - Article
C2 - 31490644
AN - SCOPUS:85072508757
SN - 1944-8244
VL - 11
SP - 34376
EP - 34384
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 37
ER -