Supramolecular Assembly of β-Cyclodextrin-Modified Polymer by Electrospinning with Sustained Antibacterial Activity

Abstract

Supramolecular assembly loading drug as biomedical materials is a research hotspot. Herein, we reported a supramolecular electrospun assembly constructed via the hydrophobic and hydrogen bonding interaction. The obtained results showed that the assembly by supramolecular electrospinning not only increased the interactions of multiple antibacterial active species including antibiotics, cationic polymers, and silver to form a flexible membrane with good mechanical strength but also indicated the dual effects of rapid doxycycline and polyethyleneimine release as well as a sustained Ag release. Interestingly, the assembly showed not only good degradability but also a high bacteriostatic efficacy toward Escherichia coli (E. coli) up to 99.9%. More importantly, the in vivo wound healing assay indicated that the assembly could promote the healing of uninfected, E. coli-infected, and even methicillin-resistant staphylococcus aureus-infected wounds. The current research provides a novel approach to construct a supramolecular assembly by electrospinning mechanically induced strong noncovalent interaction.

Multicharged cyclodextrin supramolecular assemblies

“…Although the literature contains numerous reviews covering the diverse applications of CDs and CD-based assemblies, including metal complexation, 11,41,161,162 cyclodextrin metal–organic frameworks, 163 cyclodextrin covalent organic frameworks, 164–167 supramolecular catalysis and synthesis, 168–170 multistimuli-responsive materials, 15,171–173 polymer materials, 13,24,174–181 self-healing materials, 182 amphiphilic materials, 90,183 crystalline organic materials, 184 liquid crystal materials, 14 rotaxanes/polypseudorotaxanes/catenanes/polyrotaxanes, 185–190 drug/protein/gene delivery, 16,19,23,191–194 molecular recognition and imaging, 1,195–199 molecular machines, 200 thiolated cyclodextrins, 201 cyclodextrin–porphyrinoid systems, 202 foods and antioxidants, 203,204 electrochemical analysis, 5 and chiral analysis, 205 to the best of our knowledge, multicharged CDs as an important building block have not been comprehensively reviewed. Multilevel supramolecular assembly based on electrostatic interactions between opposite charges, including parent CDs modified with multiple charges or encapsulating charged guest molecules, has enabled the construction of a diverse variety of multifunctional materials, and these have been widely applied in drug delivery, 206–214 bioimaging, 215–218 molecular recognition, 219–231 nanochannels, 232,233 molecular switches, 26,234 adsorbents and enrichment, 235–237 surfactants, 238 electrospinning supramolecular systems, 239,240 supercapacitors, 241 CD–polyoxometalate complexes, 242–245 liquid crystal materials, 246 multistimuli-responsive materials, 247–252 pseudorotaxanes, 253 conductive polymers, 254 photodynamic/chemotherapy, 255 molecular shuttles, 256,257 etc. Therefore, CD-based multicharged supramolecular assemblies are anticipated to attract even more attention in the future.…”

Physical Contact-Triggered In Situ Reactivation of Antibacterial Hydrogels

“…Certain recent microbial infections arising from emerging and re-emerging pathogens have posed an extremely serious threat to global healthcare, raising grave fears about emerging infectious diseases (EIDs). , Because of the widespread multidrug resistance that many pathogens have developed through self-mutation due to the overuse of antibiotics, the so-called “superbugs” have emerged . As the traditionally effective antibiotics no longer work against these pathogens, developing new ways to kill them has become an unprecedented and urgent global challenge in antibacterial research and technology. − The emergence of antibacterial hydrogels with high-specific, on-demand bactericidal capabilities offers a potential option for combating EIDs and thereby mitigating the present pathogen-associated healthcare crisis. − …”

Secondary Ammonium-Based Hyperbranched Poly(amidoamine) with Excellent Membrane-Active Property for Multidrug-Resistant Bacterial Infection

“…Compared with a polymer that is functionalized with neutral or negatively charged groups, a polymer with cationic surfaces generally showed higher cell-membrane affinity and penetration. − Cationic polymers with long hydrophobic chains and positively charged functional groups have attracted increasing attention due to their structural similarity to antimicrobial peptides (AMPs), which exhibit excellent antimicrobial activity. − The mechanism of synthetic cationic polymers is the interaction with the negatively charged bacteria membrane through electrostatic interaction, followed by insertion into the phospholipid layers of bacteria, thus disrupting cell membranes and ultimately killing the bacteria fast and efficiently. , Unlike a significant number of known cationic quaternary ammonium compounds (QACs) and polymeric quaternary ammonium compounds (PQACs), , the secondary/tertiary diallylammonium-based polyelectrolytes (PDAAs) that are defined as the representatives of a new family of synthetic polyelectrolytes also exhibited high biocidal activity. − Furthermore, benefiting from the formation of hydrogen bonds, these ammonium/amine groups may impart novel properties to the polymers that are distinct from their quaternary ammonium counterparts . Water-soluble cationic nonquaternary PDAAs, secondary poly­(diallylammonium trifluoroacetate) (PDAATFA), and tertiary poly­(diallylmethylammonium trifluoroacetate) (PDAMATFA) exhibited a strong biocidal effect on Mycobacteriaceae smegmatis and Mycobacterium tuberculosis .…”