Shengliang Li

An Optical Nanoruler Based on a Conjugated Polymer−Silver Nanoprism Pair for Label‐Free Protein Detection

An optical nanoruler system based on a conjugated polyelectrolyte-silver nanoprism pair is developed for label-free protein detection by taking advantage of the metal-enhanced fluorescence effect of silver nanostructures. Antibody-antigen interactions induce a change in the metal-fluorophore distance, followed by the response of a fluorescent signal of the conjugated polyelectrolyte. The system is used to detect target antigens sensitively and selectively.

Preparation of Conjugated Polymer Grafted with H2O2-Sensitive Prodrug for Cell Imaging and Tumor Cell Killing

In this work, a new conjugated polymer poly(fluorene-co-phenylene) derivative containing pendent quaternized chlormethine (PFP-Chl) was synthesized by covalent linking small molecular prodrug groups onto conjugated polymer side chains. H2O2-sensitive prodrug with an eight-member-cyclic boronate ester structure could suffer from H2O2-triggered nitrogen mustard release and further DNA cross-linking and alkylation. PFP-Chl combines therapeutic characteristic with excellent optical property of conjugated polymers. It is found that PFP-Chl could enter into cells by endocytosis to simultaneously exhibit abilities of fluorescent imaging and tumor cell inhibition.

Fluorescence Ratiometric Assay Strategy for Chemical Transmitter of Living Cells Using H2O2-Sensitive Conjugated Polymers

A new water-soluble conjugated poly(fluorene-co-phenylene) derivative (PFP-FB) modified with boronate-protected fluorescein (peroxyfluor-1) via PEG linker has been designed and synthesized. In the presence of H2O2, the peroxyfluor-1 group can transform into green fluorescent fluorescein by deprotecting the boronate protecting groups. In this case, upon selective excitation of PFP-FB backbone at 380 nm, efficient fluorescence resonance energy transfer (FRET) from PFP-FB backbone to fluorescein occurs, and accordingly, the fluorescence color of PFP-FB changes from blue to green. Furthermore, the emission color of PFP-FB and the FRET ratio change in a concentration-dependent manner. By taking advantage of PFP-FB, ratiometric detection of choline and acetylcholine (ACh) through cascade enzymatic reactions and further dynamic monitoring of the choline consumption process of cancer cells have been successfully realized. Thus, this new polymer probe promotes the development of enzymatic biosensors and provides a simpler and more effective way for detecting the chemical transmitter of living cells.

Conjugated Polymer Nanoparticles to Augment Photosynthesis of Chloroplasts

By coating chloroplasts with conjugated polymer nanoparticles (CPNs), a new bio-optical hybrid photosynthesis system (chloroplast/CPNs) is developed. Since CPNs possess unique light harvesting ability, including the ultraviolet part that chloroplasts absorb less, chloroplast/CPN complexes can capture broader range of light to accelerate the electron transport rates in photosystem II (PS II), the critical protein complex in chloroplasts, and augment photosynthesis beyond natural chloroplasts. The degree of spectral overlay between emission of CPNs and absorption of chloroplasts is critical for the enhanced photosynthesis. This work exhibits good potential to explore new and facile nanoengineering strategy for reforming chloroplast with light-harvesting nanomaterials to enhance solar energy conversion.

Biofilm Inhibition and Elimination Regulated by Cationic Conjugated Polymers

In this work, we demonstrate that water-soluble conjugated polymers (PFP) have the ability to inhibit biofilm formation and eradicate mature established biofilm using reactive oxygen species (ROS) produced by PFP under white light irradiation. Upon addition of PFP to planktonic Staphylococcus aureus (S. aureus), electrostatic interactions bring cationic PFP to the surface of S. aureus, which possesses negative charges. As the amount of PFP coated on S. aureus becomes saturated, the interactions of bacteria to bacteria and bacteria to surface may be disrupted, resulting in reduced biofilm formation. After the biofilm matures, those PFP on the surface of the biofilm can generate ROS under white light irradiation, which has the ability to inactivate bacteria nearby. Once the biofilm is broken, PFP can penetrate throughthe biofilm and continuously generate ROS under irradiation, resulting in biofilm disruption. As a consequence, this makes conjugated polymers a very promising material for the disruption of biofilm in biomedical and industrial applications.

Preparation of Reactive Oligo(p‐Phenylene Vinylene) Materials for Spatial Profiling of the Chemical Reactivity of Intracellular Compartments

An oligo(p-phenylene vinylene) derivative (OPV-pfp) functionalized with pentafluorophenol active ester is designed and synthesized. The high reactivity of OPV-pfp with biological small molecules or macromolecules containing amino groups under physiological conditions leads to spectral changes of OPV-pfp; thus, spatial reactivity discrimination for different subcellular structures inside cells is realized by triggering and imaging the fluorescence signal change of the OPV-pfp.

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.

ROS self-scavenging polythiophene materials for cell imaging

A conjugated polymer (PTDHP) was synthesized by modifying the side chain of cationic polythiophene (PT) with a dihydropyridine (DHP) group via a click reaction. PTDHP has a unique ROS self-scavenging ability through the oxidation of the DHP into a pyridine structure upon light irradiation. Thus, PTDHP achieves cell imaging with good photo-stability and low photo-cytotoxicity.

Cationic Poly(p-phenylene vinylene) Materials as a Multifunctional Platform for Light-Enhanced siRNA Delivery

In this work, a multifunctional platform based on the versatile function of cationic poly(p-phenylene vinylene) (PPV) derivative has been developed for white light-enhanced siRNA delivery in a remote control manner. Conjugated polyelectrolyte PPV, which possesses cationic and amphipathic features, can effectively self-assemble with siRNA and deliver siRNA into living cells. More importantly, PPV can sensitize surrounding oxygen into reactive oxygen species (ROS) upon exposure to white light and disrupt the endosomal membrane, and the resulting enhanced endosomal escape increases the gene silencing ability of siRNA. Besides, due to high fluorescent emission, PPV can also be used to image the siRNA delivery and intracelluar location. Therefore, by taking full advantage of PPV, this strategy provides a new enhanced siRNA delivery in a non-invasive and spatiotemporal photochemical manner.

Regulation of excitation transitions by molecular design endowing full-color-tunable emissions with unexpected high quantum yields for bioimaging application

Organic fluorophores are indispensible in chemical/biological imaging. The conjugated fluorescent molecules simultaneously possessing highly tunable emission, high quantum yield in solvents of different polarities, and large Stokes shift are quite rare. Herein, we report a new category of fluorophores based on diarylated thieno[3,4-b]thiophenes efficiently synthesized by direct C–H arylation reaction. TbT-Fluors showed full-color-tunable emissions with large Stokes shifts. Intriguingly, the fluorescence quantum yields of TbT-Fluors are barely sensitive to solvent polarities, approaching 100%. Based on photophysical and theoretical investigations, we found that the enhanced oscillator strength of the S1-S0 transition and increased T2-S1 energy difference can sufficiently compensate the negative effect from the decreased energy gap and increased reorganization energy in dimethyl sulfoxide (DMSO). Bioimaging applications revealed that some TbT-Fluors can penetrate the cell membrane and are superior for imaging in terms of high photochemical stability and low cytotoxicity. Furthermore, TbT-PhF exhibits specific colocalization with mitochondria in living cells.