De Novo Design of Entropy-Driven Polymers Resistant to Bacterial Attachment via Multicomponent Reactions

Abstract

Nonbactericidal polymers that prevent bacterial attachment are important for public health, environmental protection, and avoiding the generation of superbugs. Here, inspired by the physical bactericidal process of carbon nanotubes and graphene derivatives, we develop nonbactericidal polymers resistant to bacterial attachment by using multicomponent reactions (MCRs) to introduce molecular “needles” (rigid aliphatic chains) and molecular “razors” (multicomponent structures) into polymer side chains. Computer simulation reveals the occurrence of spontaneous entropy-driven interactions between the bacterial bilayers and the “needles” and “razors” in polymer structures and provides guidance for the optimization of this type of polymers for enhanced resistibility to bacterial attachment. The blending of the optimized polymer with commercially available polyurethane produces a film with remarkably superior stability of the resistance to bacterial adhesion after wear compared with that of commercial mobile phone shells made by the Sharklet technology. This proof-of-concept study explores entropy-driven polymers resistant to bacterial attachment via a combination of MCRs, computer simulation, and polymer chemistry, paving the way for the de novo design of nonbactericidal polymers to prevent bacterial contamination.

Membrane-Specific Binding of 4 nm Lipid Nanoparticles Mediated by an Entropy-Driven Interaction Mechanism

“…To gain deep insights into the membrane-binding mechanism of cLNPs, the free energy change ( normalΔ G ) corresponding to the cLNP–membrane interaction was estimated by calculating the potential of mean force (PMF) as a function of the z -directional distance, italicZ (Figure a, inset). The entropic and enthalpic contributions ( T normalΔ S and normalΔ H , respectively, refer to Methods) to normalΔ G were also calculated. − Here, the results are discussed for the case of cLNPs with a C4 type core and DOTAP lipids as an example. As shown in Figure a and Figure S8, normalΔ G varies appreciably depending on the composition of the membrane system.…”

Understanding Interfacial Nanoparticle Organization through Simulation and Theory: A Review

“…The transport of nanoparticles at bionano interfaces is critical for various biomedical applications and cellular responses. , Many experiments and theoretical models have been prolifically proposed to explain the diffusive transport of spheres or other 3D nanoparticles on the cell membrane. However, little is known about the transport of 2D nanomaterials.…”

Antioxidant Polymers via the Ugi Reaction for In Vivo Protection of UV-Induced Oxidative Stress

“…Recently, multi-component reactions (MCRs) have been used in polymer chemistry to prepare many elegant polymers. These MCRs include Passerini, Biginelli, Kabachnik–Fields, Ugi, Hantzsch reactions, and metal-catalyzed, as well as alkyne-based MCRs. − Because many MCRs are compatible with antioxidant groups such as phenols and heterocyclic groups, they can introduce antioxidative groups into polymer structures with nearly intact antioxidant capability. Meanwhile, MCRs use three or more reactants to generate single compounds; thus, the number and molecular diversity of polymers can be easily increased by combining different reactants, increasing the probability of obtaining an applicable antioxidant polymer.…”