Haotian Bai

Supramolecular Conjugated Polymer Systems with Controlled Antibacterial Activity

Infections of antibiotic-resistant pathogens have caused a series of public health crises across the world. According to the latest published reports, an antibiotic switch has been recognized as a potential strategy to control antibacterial activity for combating this serious drug resistance. Thus, it is anticipated that more effective antibiotic switches should be obtained by further exploring the developed strategies. Here, we report an improved pretreatment strategy using a surfactant (Triton X-100) for constructing an effective supramolecular antibiotic switch based on a poly(fluorene-co-phenylene) derivative (PFP) and cucurbit[7]uril (CB[7]), which can regulate the aggregation state of polymers before the supramolecular self-assembly process occurs. Triton X-100 can regulate the aggregation states of conjugated polymers, which is used to successfully realize the reversible control of bactericidal activity of PFP in the dark and under white light irradiation by supramolecular assembly/disassembly between PFP and CB[7]. Specialized antibiotic switches are significantly important to fight pathogenic infections and solve the drug resistance crisis in the future.

Photothermal‐Responsive Conjugated Polymer Nanoparticles for Remote Control of Gene Expression in Living Cells

Remote control and noninvasive manipulation of cellular bioprocess has received intensive attention as a powerful technology to control cell functions. Here, a strategy is developed to remotely control intracellular gene expression with high spatial and temporal resolutions by using photothermal-responsive conjugated polymer nanoparticles (CPNs) as the transducer under near-infrared light irradiation. After being modified with positive charged peptide, the CPNs with superior photothermal conversion capacity could effectively coat on the surface of living cells and generate localized heat to trigger target gene expression. The heat-inducible heat shock protein-70 promoter starts transcription of downstream EGFP gene in response to heat shock, thus producing green fluorescent protein in the living cells. The combination of heat-inducible gene promoter and photothermal-responsive CPNs provides a method for the development of thermogenetics.

Electrochemiluminescence for Electric-Driven Antibacterial Therapeutics

The employment of physical light sources in clinical photodynamic therapy (PDT) system endows it with a crucial defect in the treatment of deeper tissue lesions due to the limited penetration depth of light in biological tissues. In this work, we constructed for the first time an electric driven luminous system based on electrochemiluminescence (ECL) for killing pathogenic bacteria, where ECL is used for the excitation of photosensitizer instead of a physical light source to produce reactive oxygen species (ROS). We named this new strategy as ECL-therapeutics. The mechanism for the ECL-therapeutics is dependent on the perfect spectral overlap and energy transfer from the ECL generated by luminol to photosensitizer, cationic oligo(p-phenylenevinylene) (OPV), to sensitize the surrounding oxygen molecule into ROS. Furthermore, taking into account the practical application of our ECL-therapeutics, we used flexible hydrogel to replace the liquid system to develop hydrogel antibacterial device. Because the chemical reaction is a slow process in the hydrogel, the luminescence could last for more than 10 min after only electrifying for five seconds. This unique persistent luminescence characteristic with long afterglow life makes them suitable for persistent antibacterial applications. Thus, stretchable and persistent hydrogel devices are designed by integrating stretchable hydrogel, persistent ECL and antibacterial function into hydrogel matrices. This novel strategy avoids the employment of external light source, making it simple, convenient and controllable, which exploits a new field for ECL beyond sensors and also opens up a new model for PDT.

Tuning Antibacterial Activity of Cyclodextrin-Attached Cationic Ammonium Surfactants by A Supramolecular Approach

Two β-cyclodextrin-attached cationic ammonium surfactants bearing a dodecyl chain (APDB) and a hexadecyl chain (APCB) were synthesized to reduce the cytotoxicity of cationic surfactants to mammalian cells and endow the surfactants with host-guest recognition sites, and three kinds of guest molecules were utilized to improve the antibacterial ability of APDB and APCB via host-guest interaction by regulating the electrostatic or hydrophobic interaction of APDB or APCB with bacteria. The guest molecules include AD-NH3+ carrying one positive charge, DB with a benzene ring group and a dodecyl chain, and single chain cationic ammonium surfactant DTAB or CTAB. Either AD-NH3+ or DB increases the killing efficacy of APCB against S. aureus at 50 μM from 59% to about 75%, while DTAB or CTAB improves the killing efficacy of APCB to more than 90%. In particular, only a very small amount CTAB can improve the antibacterial activity of APCB to a very high level, but keeps very low cytotoxicity. However, the mixtures of the guest molecules with APDB are devoid of any activity against S. aureus. This is mainly attributed to the fact that APCB and its mixtures with the guest molecules form 100-200 nm spherical aggregates, while the mixtures of APDB with the guest molecules cannot form aggregates at lower concentration. It is revealed that the three kinds of guest molecules trapped in the APCB spherical aggregates lead to diverse interaction modes of the APCB spherical aggregates with S. aureus, accounting for the different killing efficacy of the APCB/guest molecule mixtures. This supramolecular strategy provides an effective approach for the construction of highly efficient antibacterial agents with low cytotoxicity.

Supramolecular Strategy Based on Conjugated Polymers for Discrimination of Virus and Pathogens

A conjugated polymer-based supramolecular system is designed for discrimination of virus and microbes. The supramolecular system is composed of cationic polythiophene derivative (PT) and barrel-shaped macrocyclic molecular cucurbit[7]uril (CB[7]). Because PT and PT/CB[7] complexes possess different interaction manners toward virus and microbes, the rapid and simple discrimination of virus and microbes was realized through polymer fluorescence intensity change assisting with standard linear discriminant analysis (LDA). The supramolecular strategy would expand the idea of designing biological probes and further promote the extensive application of conjugated polymer materials in biosensor field.