Publications by authors named "Ben Zhong Tang"

775 Publications

NIR-II Aggregation-Induced Emission Luminogens for Tumor Phototheranostics.

Biosensors (Basel) 2022 Jan 17;12(1). Epub 2022 Jan 17.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518172, China.

As an emerging and powerful material, aggregation-induced emission luminogens (AIEgens), which could simultaneously provide a precise diagnosis and efficient therapeutics, have exhibited significant superiorities in the field of phototheranostics. Of particular interest is phototheranostics based on AIEgens with the emission in the range of second near-infrared (NIR-II) range (1000-1700 nm), which has promoted the feasibility of their clinical applications by virtue of numerous preponderances benefiting from the extremely long wavelength. In this minireview, we summarize the latest advances in the field of phototheranostics based on NIR-II AIEgens during the past 3 years, including the strategies of constructing NIR-II AIEgens and their applications in different theranostic modalities (FLI-guided PTT, PAI-guided PTT, and multimodal imaging-guided PDT-PTT synergistic therapy); in addition, a brief conclusion of perspectives and challenges in the field of phototheranostics is given at the end.
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http://dx.doi.org/10.3390/bios12010046DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8774032PMC
January 2022

Organic Long-Persistent Luminescence from a Single-Component Aggregate.

J Am Chem Soc 2022 Jan 20. Epub 2022 Jan 20.

Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon 999077, Hong Kong, China.

Long-persistent luminescence (LPL), also known as afterglow, is a phenomenon in which the material shows long-lasting luminescence after the cessation of the excitation source. The research of LPL continues to attract much interest due to its fundamental nature and its potential in the development of the next generation of functional materials. However, most of the current LPL materials are multicomponent inorganic systems obtained after harsh synthetic procedures and often use rare-earth metals. Recently, metal free organic long-persistent luminescence (OLPL) has gained much interest because it can bypass many of the disadvantages of inorganic systems. To date, the most successful method to generate OLPL systems is to access charge-separated states through binary donor-acceptor exciplex systems. However, it has been reported that the ratios of the binary systems affect OLPL properties, complicating the reproducibility and large-scale production of OLPL materials. Simpler OLPL systems can overcome these issues for the benefit of the development and adoption of OLPL systems. Here, we report on the rational design and synthesis of a single-component OLPL system with detectable afterglow for at least 12 min under ambient conditions. This work exemplifies an easy design principle for new OLPL materials. The investigation of the material provides valuable insights toward the generation of OLPL from a single-component system.
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http://dx.doi.org/10.1021/jacs.1c11480DOI Listing
January 2022

Room temperature synthesis of polythioamides from multicomponent polymerization of sulfur, pyridine-activated alkyne, and amines.

Chem Commun (Camb) 2022 Jan 20. Epub 2022 Jan 20.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, South China University of Technology, Guangzhou 510640, China.

Through the design of a pyridine-activated diyne monomer, the catalyst-free multicomponent polymerizations of sulfur, aromatic alkyne, and a group of commercially available primary and secondary diamines were realized at room temperature or 40 °C, affording functional polythioamides with well-defined structures, high yields (up to 98%), high molecular weights (95 100 g mol), improved mercury removal performance, and interesting photophysical and photochemical properties. This work not only demonstrated an advance in efficient and economic synthesis of polythioamides, but also revealed the structure-property relationship of these promising sulfur-containing polymer materials.
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http://dx.doi.org/10.1039/d1cc06448gDOI Listing
January 2022

Completely aqueous processable stimulus responsive organic room temperature phosphorescence materials with tunable afterglow color.

Nat Commun 2022 Jan 17;13(1):347. Epub 2022 Jan 17.

Institute of Molecular Aggregation Science, Tianjin University, 300072, Tianjin, China.

Many luminescent stimuli responsive materials are based on fluorescence emission, while stimuli-responsive room temperature phosphorescent materials are less explored. Here, we show a kind of stimulus-responsive room temperature phosphorescence materials by the covalent linkage of phosphorescent chromophore of arylboronic acid and polymer matrix of poly(vinylalcohol). Attributed to the rigid environment offered from hydrogen bond and B-O covalent bond between arylboronic acid and poly(vinylalcohol), the yielded polymer film exhibits ultralong room temperature phosphorescence with lifetime of 2.43 s and phosphorescence quantum yield of 7.51%. Interestingly, the RTP property of this film is sensitive to the water and heat stimuli, because water could destroy the hydrogen bonds between adjacent poly(vinylalcohol) polymers, then changing the rigidity of this system. Furthermore, by introducing another two fluorescent dyes to this system, the color of afterglow with stimulus response effect could be adjusted from blue to green to orange through triplet-to-singlet Förster-resonance energy-transfer. Finally, due to the water/heat-sensitive, multicolor and completely aqueous processable feature for these three afterglow hybrids, they are successfully applied in multifunctional ink for anti-counterfeit, screen printing and fingerprint record.
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http://dx.doi.org/10.1038/s41467-022-28011-6DOI Listing
January 2022

A ratiometric theranostic system for visualization of ONOO species and reduction of drug-induced hepatotoxicity.

Biomater Sci 2022 Jan 17. Epub 2022 Jan 17.

Department of Chemical and Biological Engineering and Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, Division of Life Science and State Key Laboratory of Molecular Neuroscience, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

Peroxynitrite (ONOO) is a potent reactive nitrogen species that plays a role as a critical mediator in liver injury elicited by drugs such as acetaminophen (APAP). At a therapeutic dosage, most APAP is metabolized by liver cells and then excreted in the urine. However, excessive APAP intake can cause an acute production of ONOO, which induces mitochondrial oxidative stress and necrosis of the liver cells. Therefore, the ONOO levels in hepatocytes have been considered as an early sign of hepatotoxicity associated with drug overdosage. Herein, a ratiometric theranostic system based on aggregation-induced emission luminogens (AIEgens) for the visualization of ONOO and reduction of drug-induced hepatotoxicity is developed. The AIEgen ATV-PPB shows a ratiometric fluorescence response from red to green upon cleavage of arylboronic ester moieties by ONOO with high sensitivity and selectivity. Meanwhile, experiments reveal that ATV-PPB not only acts as a fluorescent probe for ONOO but also as an intracellular ONOO scavenger to reduce the hepatotoxicity under overdose APAP treatment.
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http://dx.doi.org/10.1039/d1bm01675jDOI Listing
January 2022

Novel Quinolizine AIE System: Visualization of Molecular Motion and Elaborate Tailoring for Biological Application.

Angew Chem Int Ed Engl 2022 Jan 12. Epub 2022 Jan 12.

The Chinese University of Hong Kong, Shenzhen, School of Science and Engineering, 2001 Longxiang Boulevard, Longgang District, 518172, Shenzhen, CHINA.

Molecular motions are ubiquitous in nature and they immutably play intrinsic roles in all actions. However, exploring appropriate models to decipher molecular motions is an extremely important but very challenging task for researchers. Considering aggregation-induced emission (AIE) luminogens possess their unique merits to visualize molecular motions, it is particularly fascinating to construct new AIE systems as model to study molecular motion. Herein, a novel quinolizine (QLZ) AIE system was constructed based on the restriction intramolecular vibration mechanism. It was demonstrated that QLZ could act as an ideal model to visualize single-molecule motion and macroscopic molecular motion via fluorescence change. Additionally, further elaborate tailoring of this impressive core achieved highly efficient reactive oxygen species production and realized fluorescence imaging-guided photodynamic therapy applications, which confirms the great application potential of this new AIE-active QLZ core. Therefore, this work not only provides an ideal model to visualize molecular motion but also opens a new way for the application of AIEgens.
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http://dx.doi.org/10.1002/anie.202117709DOI Listing
January 2022

Bringing Inherent Charges into Aggregation-Induced Emission Research.

Acc Chem Res 2022 Jan 5;55(2):197-208. Epub 2022 Jan 5.

Department of Chemistry, the Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, and Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China.

ConspectusCharged organic molecules, such as DNA, RNA, proteins, and polysaccharides, are ubiquitous and indispensable in natural living systems, which possess specific biological functions to interact with oppositely charged species via electrostatic attraction. The molecules with inherent charges typically differentiate themselves from the neutral ones with unique attributes (e.g., ionic interactions and high polarity), thereby playing a pivotal role in a broad spectrum of areas, including supramolecular chemistry, structural biology, and materials science. It is thus of great importance to explore and develop various charged organic systems for biomimicry and the creation of functional materials. In 2001, our group reported a peculiar luminogen that exhibited weak emission in solution but had significantly enhanced emission in aggregates, and we, for the first time, coined this phenomenon as aggregation-induced emission (AIE). The AIE concept significantly changes the cognition of the scientific community toward classic photophysical phenomena. Since the discovery of this unusual luminescence phenomenon, AIE luminogens (AIEgens) have attracted extensive attention from researchers in a plethora of disciplines because of their high brightness in aggregates, large Stokes shift, excellent photostability, and good biocompatibility. In the past 10 years, our laboratory has expended a great amount of effort to bring inherent charges into AIE research and acquired fruitful achievements.In this Account, we summarize the progress of charged AIE systems primarily made by our laboratory. We start with a brief introduction to charged AIEgens and then discuss their design strategies from molecular and topological perspectives, respectively. Next, we review the unique properties of charged AIEgens, including D-A interactions, anion-π interactions, and intermolecular electrostatic interactions, with an emphasis on how they differentiate themselves from the neutral analogs. On the one hand, positively charged AIEgens exhibit unique photophysical properties by forming typical donor-acceptor structures to manipulate the emission wavelength or initiate ultralong persistent luminescence. On the other hand, positively charged AIEgens exhibit unique physiochemical properties, such as an adjustable targeting capability toward biological targets and a strong capability for the generation of reactive oxygen species. Furthermore, we showcase the applications of charged AIEgens in imaging and diagnosis, photodynamic therapy, gas separation, and solar desalination. Finally, we conclude this Account with a summary and some perspectives regarding the existing challenges and future directions. We hope that this Account can spark new ideas and inspire scientists from different disciplines to explore this nascent yet promising research area.
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http://dx.doi.org/10.1021/acs.accounts.1c00630DOI Listing
January 2022

Robust Luminescent Molecules with High-Level Reverse Intersystem Crossing for Efficient Near Ultraviolet Organic Light-Emitting Diodes.

Angew Chem Int Ed Engl 2022 Jan 3:e202116810. Epub 2022 Jan 3.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, South China University of Technology, Guangzhou, 510640, China.

Organic light-emitting diodes (OLEDs) radiating near ultraviolet (NUV) light are of high importance but rarely reported due to the lack of robust organic short-wavelength emitters. Here, we report a short π-conjugated molecule (POPCN-2CP) with high thermal and morphological stabilities and strong NUV photoluminescence. Its neat film exhibits an electroluminescence (EL) peak at 404 nm with a maximum external quantum efficiency (η ) of 7.5 % and small efficiency roll-off. The doped films of POPCN-2CP in both non-polar and polar hosts at a wide doping concentration range (10-80 wt%) achieve high-purity NUV light (388-404 nm) and excellent η s of up to 8.2 %. The high-level reverse intersystem crossing improves exciton utilization and accounts for the superb η s. POPCN-2CP can also serve as an efficient host for blue fluorescence, thermally activated delayed fluorescence and phosphorescence emitters, providing excellent EL performance via Förster energy transfer.
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http://dx.doi.org/10.1002/anie.202116810DOI Listing
January 2022

Combining Hydroxyl-Yne and Thiol-Ene Click Reactions to Facilely Access Sequence-Defined Macromolecules for High-Density Data Storage.

J Am Chem Soc 2021 Dec 27. Epub 2021 Dec 27.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, AIE Institute, Center for Aggregation-Induced Emission, South China University of Technology, Guangzhou 510640, People's Republic of China.

Through mimicking the synthesis of hereditary-information-containing nucleic acids, scientists are committed to synthesizing sequence-defined macromolecules. Herein, a protecting-group-free, metal-free, and atom-economical chemistry combining hydroxyl-yne and thiol-ene click reactions was developed to efficiently synthesize sequence-defined oligo(monothioacetals) (overall yield of 54% for an 11-step synthesis) from readily available starting compounds and monomers under ambient conditions. The sequences of linear oligo(monothioacetals) could be easily decoded via a tandem ESI-MS/MS technique, making them new kinds of digital macromolecules with a high data storage density (0.013 bit/Da). Moreover, star oligo(monothioacetals) could also be facilely generated through divergent and convergent strategies and their combination. An unprecedented sequence-defined miktoarm star oligo(monothioacetal) was obtained, which could serve as a new nonlinear digital macromolecule to achieve 2D information matrix encoding and hold great potential to be applied for information encryption, anticouterfeiting, secret communication, etc. Thus, this work provides a powerful stepwise iterative approach to facilely access sequence-defined linear and topological oligo(monothioacetals) for high-density data storage.
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http://dx.doi.org/10.1021/jacs.1c10612DOI Listing
December 2021

Porphyrin-Based Two-Dimensional Layered Metal-Organic Framework with Sono-/Photocatalytic Activity for Water Decontamination.

ACS Nano 2021 Dec 27. Epub 2021 Dec 27.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, School of Materials Science and Engineering, South China University of Technology, Guangzhou, Guangdong 510640, China.

Water treatment is crucial to improve the water quality and reduce diarrheal and chronological diseases caused by excessive discharge of organic dyes and other waste. The development and expansion of efficient catalysts for the degradation and sterilization of organic dyes has attracted widespread attention. Herein, we report an example of a porphyrin-based two-dimensional layered metal-organic framework (MOF) (2DZnTcpp) and its efficient sono-/photocatalytic degradation of organic dyes and bactericidal activity. The dislocated layers effectively avoid close π-π stacking and provide a porous space for oxygen/water/dye contact. The introduction of Zn ions increases the spin orbital coupling through the heavy atom effect and promotes the intersystem crossing process for singlet oxygen generation. The effective ligand-to-metal charge transfer and the excessive open Zn catalytic sites also facilitate water splitting for hydroxyl radical generation. These features together promote the reactive oxygen species (ROS) generation of 2DZnTcpp under light illumination or ultrasound sonication. It is worth noting that the 2DZnTcpp with a high specific surface area and porosity shows efficient sono-/photocatalytic degradation of organic dye waste. Moreover, 2DZnTcpp could also largely inactivate under light irradiation (the light power of 1 sun) or ultrasound sonication for 30 min with efficiencies over 99.99999%. This work provides an approach for the design and synthesis of MOF-based sono-/photocatalysts used in the purification and treatment of textile wastewater and is committed to the establishment of a more efficient, fast, and environmentally friendly catalytic system.
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http://dx.doi.org/10.1021/acsnano.1c09301DOI Listing
December 2021

A Class of Biocompatible Dye-Protein Complex Optical Nanoprobes.

ACS Nano 2021 Dec 23. Epub 2021 Dec 23.

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering & Key Laboratory of Micro-systems and Micro-structures, Ministry of Education, Harbin Institute of Technology, 150001 Harbin, P. R. China.

Molecular organic dyes are classic fluorescent nanoprobes finding tremendous uses in biological and life sciences. Yet, they suffer from low brightness, poor photostability, and lack of functional groups for bioconjugation. Here, we describe a class of biocompatible dye-protein optical nanoprobes, which show long-time photostability, superbrightness, and enriched functional groups. These nanoprobes utilize apoferritin (an intracellular protein for iron stores and release) to encase appropriate molecular organic dyes to produce on-demand fluorescence in aqueous solution. A pH-driven dissociation-reconstitution process of apoferritin subunits allows substantial incorporation of hydrophilic (aggregation caused quenching, ACQ) or hydrophobic (aggregation induced enhancement, AIE) dye molecules into the protein nanocavity (8 nm), producing monodispersed dye-apoferritin nanoparticles (apo-dye-NPs, ∼12 nm). As compared with single dye monomer, single apo-dye-NPs possess hundreds of times larger molar extinction coefficient and 2 orders of magnitude higher absolute luminescence quantum yield (up to 45-fold), multiplying fluorescence brightness up to 2778-fold. We show that varying the type of incorporated dyes entails a precise control over nanoprobe emission profile tunable in a broad spectral range of 370-1300 nm. Mechanical investigations indicate that the diversified microstructures of nanocavity inner surface are able to conform ACQ dyes at reasonable space interval while providing protein-guided-stacking for AIE dyes, thus enhancing fluorescence quantum yield through confining intermolecular quenching and intramolecular rotation. Moreover, apo-dye-NPs are able to emit stable fluorescence (over 13 min) without quenching in confocal imaging of HepG2 cancer cell under ultrahigh laser irradiance (1.3 × 10 W/cm). These superb properties make them suitable, as demonstrated in this work, for long-term super-resolved structured illumination microscopic cell imaging (spatial resolution, 117 nm) over 48 h, near-infrared (NIR) fluorescence angiography imaging of whole-body blood vessels (spatial resolution, 380 μm), and NIR photoacoustic imaging of liver .
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http://dx.doi.org/10.1021/acsnano.1c06536DOI Listing
December 2021

Advances in Improving Healthcare with Aggregation-Induced Emission.

Adv Healthc Mater 2021 12;10(24):e2102499

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, 2001 Longxiang Boulevard, Longgang District, Shenzhen City, Shenzhen, Guangdong, 518172, China.

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http://dx.doi.org/10.1002/adhm.202102499DOI Listing
December 2021

Precise Molecular Engineering of Type I Photosensitizers with Near-Infrared Aggregation-Induced Emission for Image-Guided Photodynamic Killing of Multidrug-Resistant Bacteria.

Adv Sci (Weinh) 2021 Dec 19:e2104079. Epub 2021 Dec 19.

Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, 999077, China.

Multidrug resistance (MDR) bacteria pose a serious threat to human health. The development of alternative treatment modalities and therapeutic agents for treating MDR bacteria-caused infections remains a global challenge. Herein, a series of near-infrared (NIR) anion-π photosensitizers featuring aggregation-induced emission (AIE-PSs) are rationally designed and successfully developed for broad-spectrum MDR bacteria eradication. Due to the strong intramolecular charge transfer (ICT) and enhanced highly efficient intersystem crossing (ISC), these electron-rich anion-π AIE-PSs show boosted type I reactive oxygen species (ROS) generation capability involving hydroxyl radicals and superoxide anion radicals, and up to 99% photodynamic killing efficacy is achieved for both Methicillin-resistant Staphylococcus aureus (MRSA) and multidrug resistant Escherichia coli (MDR E. coli) under a low dose white light irradiation (16 mW cm ). In vivo experiments confirm that one of these AIE-PSs exhibit excellent therapeutic performance in curing MRSA or MDR E. coli-infected wounds with negligible side-effects. The study would thus provide useful guidance for the rational design of high-performance type I AIE-PSs to overcome antibiotic resistance.
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http://dx.doi.org/10.1002/advs.202104079DOI Listing
December 2021

High-Performance Orange-Red Organic Light-Emitting Diodes with External Quantum Efficiencies Reaching 33.5% based on Carbonyl-Containing Delayed Fluorescence Molecules.

Adv Sci (Weinh) 2021 Dec 19:e2104435. Epub 2021 Dec 19.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, South China University of Technology, Guangzhou, 510640, China.

Developing orange to red purely organic luminescent materials having external quantum efficiencies (η s) exceeding 30% is challenging because it generally requires strong intramolecular charge transfer, efficient reverse intersystem crossing (RISC), high photoluminescence quantum yield (Φ ), and large optical outcoupling efficiency (Φ ) simultaneously. Herein, by introducing benzoyl to dibenzo[a,c]phenazine acceptor, a stronger electron acceptor, dibenzo[a,c]phenazin-11-yl(phenyl)methanone, is created and employed for constructing orange-red delayed fluorescence molecules with various acridine-based electron donors. The incorporation of benzoyl leads to red-shifted photoluminescence with accelerated RISC, reduced delayed lifetimes, and increased Φ s, and the adoption of spiro-structured acridine donors promotes horizontal dipole orientation and thus renders high Φ s. Consequently, the state-of-the-art orange-red organic light-emitting diodes are achieved, providing record-high electroluminescence (EL) efficiencies of 33.5%, 95.3 cd A , and 93.5 lm W . By referring the control molecule without benzoyl, it is demonstrated that the presence of benzoyl can exert significant positive effect over improving delayed fluorescence and enhancing EL efficiencies, which can be a feasible design for robust organic luminescent materials.
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http://dx.doi.org/10.1002/advs.202104435DOI Listing
December 2021

Diradical-Featured Organic Small-Molecule Photothermal Material with High-Spin State in Dimers for Ultra-Broadband Solar Energy Harvesting.

Adv Mater 2021 Dec 9:e2108048. Epub 2021 Dec 9.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong (Shenzhen), Shenzhen, 518172, China.

Organic materials with radical characteristics are gaining increasing attention, due to their potential implications in highly efficient utilization of solar energy. Manipulating intermolecular interactions is crucial for tuning radical properties, as well as regulating their absorption bands, and thus improving the photothermal conversion efficiency. Herein, a diradical-featured organic small-molecule croconium derivative, CR-DPA-T, is reported for highly efficient utilization of solar energy. Upon aggregation, CR-DPA-T exists in dimer form, stabilized by the strong intermolecular π-π interactions, and exhibits a rarely reported high-spin state. Benefiting from the synergic effects of radical characteristics and strong intermolecular π-π interactions, CR-DPA-T powder absorbs broadly from 300 to 2000 nm. In-depth investigations with transient absorption analysis reveal that the strong intermolecular π-π interactions can promote nonradiative relaxation by accelerating internal conversion and facilitating intermolecular charge transfer (ICT) between dimeric molecules to open up faster internal conversion pathways. Remarkably, CR-DPA-T powder demonstrates a high photothermal efficiency of 79.5% under 808 nm laser irradiation. By employing CR-DPA-T as a solar harvester, a CR-DPA-T-loaded flexible self-healing poly(dimethylsiloxane) (H-PDMS) film, named as H-PDMS/CR-DPA-T self-healing film, is fabricated and employed for solar-thermal applications. These findings provide a feasible guideline for developing highly efficient diradical-featured organic photothermal materials.
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http://dx.doi.org/10.1002/adma.202108048DOI Listing
December 2021

A Universal Boronate-Affinity Crosslinking-Amplified Dynamic Light Scattering Immunoassay for Point-of-Care Glycoprotein Detection.

Angew Chem Int Ed Engl 2021 Dec 8:e202112031. Epub 2021 Dec 8.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, Guangdong, 518172, China.

Herein, we report a universal boronate-affinity crosslinking-amplified dynamic light scattering (DLS) immunoassay for point-of-care (POC) glycoprotein detection in complex samples. This enhanced DLS immunoassay consists of two elements, i.e., antibody-coated magnetic nanoparticles ([email protected]) for target capture and DLS signal transduction, and phenylboronic acid-based boronate-affinity materials as crosslinking amplifiers. Upon the addition of targets, glycoproteins are first captured by [email protected] and amplified by target-induced crosslinking stemming from the selective binding between the boronic acid ligand and cis-diol-containing glycoprotein, thereby resulting in a remarkably increased DLS signal in the average nanoparticle size. Benefiting from the multivalent binding and fast boronate-affinity reaction between glycoproteins and crosslinkers, the proposed immunosensing strategy has achieved the ultrasensitive and rapid quantitative assay of glycoproteins at the fM level within 15 min. Overall, this work provides a promising and versatile design strategy for extending the DLS technique to detect glycoproteins even in the field or at POC.
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http://dx.doi.org/10.1002/anie.202112031DOI Listing
December 2021

A biocompatible dual-AIEgen system without spectral overlap for quantitation of microbial viability and monitoring of biofilm formation.

Mater Horiz 2021 Jun 23;8(6):1816-1824. Epub 2021 Apr 23.

Department of Chemistry, Department of Chemical and Biological Engineering, Hong Kong Branch of Chinese Nation-al Engineering Research Center for Tissue Restoration and Reconstruction, Institute of Advanced Study and Division of Life Science The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

The lack of rapid and reliable microbial detection and sensing platforms and insufficient understanding of microbial behavior may delay precautions that could be made, which is a great threat to human life and increases the heavy financial burden on society. In this contribution, a dual-aggregation-induced emission luminogen (AIEgen) system is successfully developed for microbial imaging and metabolic status sensing. This system consists of two AIEgens (DCQA and TPE-2BA) that bear positively charged groups or boronic acid groups, providing universal microbial staining ability and specific affinity for dead microbes, respectively. Based on the distinctive fluorescence response produced by the diverse interaction of AIEgens with live or dead microbes, this dual-AIEgen system can detect all the microbes and identify their viabilities. Furthermore, the morphology and metabolic status of a sessile biofilm can also be imaged and monitored. The system exhibits rapid labelling properties that suitable for various microbes, and good biocompatibilities.
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http://dx.doi.org/10.1039/d1mh00149cDOI Listing
June 2021

Augmenting photosynthesis through facile AIEgen-chloroplast conjugation and efficient solar energy utilization.

Mater Horiz 2021 May 26;8(5):1433-1438. Epub 2021 Apr 26.

Department of Chemical and Biological Engineering, Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, Division of Life Science and Institute of Advanced Study, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

Photosynthesis is regarded as the foundation for sustaining life on our planet. Light-harvesting is the initial step that activates the subsequent photochemical reactions. In the photosystems, chloroplast is the basic light-driven metabolic factory of higher plant cells. However, there is an incomplete match between the solar radiation spectrum and absorption profile of chloroplasts. It is hard for the photosynthetic pigments to fully utilize the sunlight energy. Here, we designed two new aggregation-induced emission (AIE) molecules with activated alkyl groups (TPE-PPO and TPA-TPO). Via a facile metal-free "Click" reaction, we realized the substantial manipulation of live chloroplasts with the AIE luminogens (AIEgens). Owing to the matched photophysical properties, the AIEgens could harvest harmful ultraviolet radiation (HUVR) and photosynthetically inefficient radiation (PIR), and further convert them into photosynthetically active radiation (PAR) for chloroplast absorption. As a result, the conjugated AIEgen-chloroplast exhibited better capability of water splitting and electron separation. It promoted the generation of adenosine triphosphate (ATP), which is an important product of photosynthesis. This work provides an effective strategy for improving plant photosynthesis.
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http://dx.doi.org/10.1039/d1mh00012hDOI Listing
May 2021

9,10-Phenanthrenequinone: A Promising Kernel to Develop Multifunctional Antitumor Systems for Efficient Type I Photodynamic and Photothermal Synergistic Therapy.

ACS Nano 2021 12 30;15(12):20042-20055. Epub 2021 Nov 30.

State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, South China University of Technology, Guangzhou 510640, China.

Synergistic phototherapy provides a promising strategy to conquer the hypoxia and heterogeneity of tumors and realize a better therapeutic effect than monomodal photodynamic therapy (PDT) or photothermal therapy (PTT). The development of efficient multifunctional organic phototheranostic systems still remains a challenging task. Herein, 9,10-phenanthrenequinone (PQ) with strong electron-withdrawing ability is conjugated with the rotor-type electron-donating triphenylamine derivatives to create a series of tailor-made photosensitizers. The highly efficient Type I reactive oxygen species generation and outstanding photothermal conversion capacity are tactfully integrated into these PQ-cored photosensitizers. The underlying photophysical and photochemical mechanisms of the combined photothermal and Type I photodynamic effects are deciphered by experimental and theoretical methods and are closely associated with the active intramolecular bond stretching vibration, facilitated intersystem crossing, and specific redox cycling activity of the PQ core. Both and evaluations demonstrate that the nanoagents fabricated by these PQ-based photosensitizers are excellent candidates for Type I photodynamic and photothermal combined antitumor therapy. This study thus broadens the horizon for the development of high-performance PTT/Type I PDT nanoagents for synergistic phototheranostic treatments.
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http://dx.doi.org/10.1021/acsnano.1c07730DOI Listing
December 2021

High-Performance Near-Infrared Aggregation-Induced Emission Luminogen with Mitophagy Regulating Capability for Multimodal Cancer Theranostics.

ACS Nano 2021 12 29;15(12):20453-20465. Epub 2021 Nov 29.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, 2001 Longxiang Boulevard, Longgang District, Shenzhen 518172, China.

The construction of intelligent near-infrared (NIR) fluorophores for high specificity to cancer cells and application in multiple therapeutic modalities is crucial for precise cancer diagnostic and therapy. In this study, an aggregation-induced emission-active NIR fluorophore (TACQ) with mitophagy-modulating activity was synthesized and developed for mitochondrial targeting multimodal cancer theranostics. The strengthened push-pull interaction extended the emission of TACQ into the NIR-II region (>1000 nm). Further, the rotor structure and twisted molecular conformation enables nanoaggregates of TACQ to balance the radiative and nonradiative decays to simultaneously exhibit bright NIR emission, high photothermal conversion efficiency (55%), and efficient generation of reactive oxygen species. The lipocationic property of TACQ allows it to selectively accumulate in the mitochondria of cancer cells. TACQ can induce mitophagy and block mitophagic flux facilitating cancer cell apoptosis. Both and evaluations revealed that TACQ is an efficient theranostic agent for NIR fluorescence and photothermal imaging-guided synergistic chemo-photothermal and photodynamic therapy.
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http://dx.doi.org/10.1021/acsnano.1c08928DOI Listing
December 2021

Through-Space Interactions in Clusteroluminescence.

JACS Au 2021 Nov 30;1(11):1805-1814. Epub 2021 Sep 30.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518172, China.

Conventional π-conjugated luminophores suffer from problems such as emission quenching, biotoxicity, environmental pollution, etc. The emerging nonconjugated and nonaromatic clusteroluminogens (CLgens) are expected to overcome these stubborn drawbacks, so research of CLgens shows great significance not only for practical application but also for the construction of fundamental photophysical theories. This perspective summarizes the unusual features of CLgens in comparison to traditional chromophores, such as nonconjugated molecular structures, unmatched absorption and excitation, excitation-dependent luminescence, multiple emission peaks, and room-temperature phosphorescence. Different from the theory of through-bond conjugation in π-conjugated luminophores, through-space interactions, including through-space n···n interaction and through-space n···π interaction, are regarded as the emitting sources of nonconjugated CLgens. In addition, the formation of network clusters is proposed as an efficient strategy to improve the performance of CLgens, and their potential applications of anticounterfeiting, photoelectronic devices, and bioimaging are prospected.
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http://dx.doi.org/10.1021/jacsau.1c00311DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8611663PMC
November 2021

Metal-Based Aggregation-Induced Emission Theranostic Systems.

ChemMedChem 2021 Nov 27:e202100578. Epub 2021 Nov 27.

Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Guangdong-Hong Kong-Macau Joint Laboratory of Optoelectronic and Magnetic Functional Materials, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

Efficient theranostic systems can realize better outcomes in disease treatment because of precise diagnosis and the concomitant effective therapy. Aggregation-induced emission luminogens (AIEgens) are a unique type of organic emitters with intriguing photophysical properties in the aggregate state. Among the AIEgens studied for biomedical applications, so far, metal-based AIE systems have shown great potential in theranostics due to the enhanced multimodal bioimaging ability and therapeutic effect. This research field has been growing rapidly, and many rationally designed systems with promising activities to cancer and other diseases have been reported recently. In this review, we summarized the recent progress of metal-based AIE materials in bioimaging and biological theranostics, and deciphered the pertinent design strategies. We hope that this review can offer new insights into the development of this growing field.
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http://dx.doi.org/10.1002/cmdc.202100578DOI Listing
November 2021

A synergy between the push-pull electronic effect and twisted conformation for high-contrast mechanochromic AIEgens.

Mater Horiz 2021 Feb 15;8(2):630-638. Epub 2020 Dec 15.

AIE Research Center, Shaanxi Key Laboratory of Phytochemistry, College of Chemistry and Chemical Engineering, Baoji University of Arts and Sciences, Baoji 721013, China.

Mechanochromic (MC) luminogens in response to external stimulus have shown promising applications as pressure sensors and memory devices. Meanwhile, research on their underlying mechanism is still in the initial stage. Here, three pyridinium-functionalized tetraphenylethylenes bearing n-pentyloxy, hydrogen and nitro groups, namely TPE-OP, TPE-H and TPE-NO, are designed to systematically investigate the influence of the push-pull electronic effect and molecular conformation on MC luminescence. Upon anisotropic grinding and isotropic hydrostatic compression, TPE-OP with strong intramolecular charge transfer (ICT) affords the best MC behavior among them. Analysis of three polymorphs of TPE-H clearly indicates that planarization of the molecular conformation plays an important role in their bathochromic shifts under mechanical stimuli. Theoretical calculations also verify that high twisting stress of AIEgens can be released under high pressure. This study presents a mechanistic insight into MC behaviour and an effective strategy to achieve high-contrast MC luminescence.
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http://dx.doi.org/10.1039/d0mh01251cDOI Listing
February 2021

Altering Chain Flexibility of Aliphatic Polyesters for Yellow-Green Clusteroluminescence in 38 % Quantum Yield.

Angew Chem Int Ed Engl 2021 Nov 25. Epub 2021 Nov 25.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, 518172, China.

Preparation of non-conjugated polymers with long-wavelength emission and high quantum yield (QY) is still a huge challenge. Herein, we report the first example of linear non-conjugated polyester exhibiting yellow-green clusteroluminescence (CL) and a high QY of 38 %. We discovered that the polyester P3 with balanced flexibility and rigidity showed the longest CL wavelength and highest QY. Systematically photophysical characterization unravel the key role of ester cluster in the CL and the cluster formation via the aggregate of ester units was visualized. Moreover, P3 was demonstrated to be a highly selective, quick-responsive (ca. 1.2 min) and sensitive detector (detection limit is 0.78 μM) for irons owing to the fast disassociation of clusters by irons. This work not only gains further mechanistic insight into CL but also provides a new strategy to design high-efficiency and long-wavelength CL, meanwhile, enlightens the glorious application prospect of luminescent polyester.
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http://dx.doi.org/10.1002/anie.202114117DOI Listing
November 2021

Enantioselective recognition of chiral acids by supramolecular interactions with chiral AIEgens.

Chem Commun (Camb) 2021 Dec 9;57(98):13321-13324. Epub 2021 Dec 9.

Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, Guangdong 518172, China.

Novel chiral AIEgens bearing optically pure amino groups were synthesized and showed excellent discrimination for a series of chiral acidic compounds and amino acids. Interestingly, after supramolecular assembly with 4-sulfocalix[4]arene, the obtained complexes showed enhanced enantioselectivity for chiral acids.
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http://dx.doi.org/10.1039/d1cc05618bDOI Listing
December 2021

Cationization to boost both type I and type II ROS generation for photodynamic therapy.

Biomaterials 2022 Jan 17;280:121255. Epub 2021 Nov 17.

AIE Institute, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, School of Materials Science and Engineering, South China University of Technology, Guangzhou, 510640, China; Shenzhen Institute of Aggregate Science and Technology, School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, 2001 Longxiang Boulevard, Longgang District, Shenzhen City, Guangdong, 518172, China.

The pursuing of photosensitizers (PSs) with efficient reactive oxygen species (ROS) especially type I ROS generation in aggregate is always in high demand for photodynamic therapy (PDT) and photoimmunotherapy but remains to be a big challenge. Herein, we report a cationization molecular engineering strategy to boost both singlet oxygen and radical generation for PDT. Cationization could convert the neutral donor-acceptor (D-A) typed molecules with the dicyanoisophorone-triphenylamine core (DTPAN, DTPAPy) to their A-D-A' typed cationic counterparts (DTPANPF and DTPAPyPF). Our experiment and simulation results reveal that such cationization could enhance the aggregation-induced emission (AIE) feature, promote the intersystem crossing (ISC) processes, and increase the charge transfer and separation ability, all of which work collaboratively to promote the efficient generation of ROS especially hydroxyl and superoxide radicals in aggregates. Moreover, these cationic AIE PSs also possess specific cancer cell mitochondrial targeting capability, which could further promote the PDT efficacy both in vitro and in vivo. Therefore, we expect this delicate molecular design represents an attractive paradigm to guide the design of type I AIE PSs for the further development of PDT.
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http://dx.doi.org/10.1016/j.biomaterials.2021.121255DOI Listing
January 2022

Aggregation-induced delayed fluorescence luminogens: the innovation of purely organic emitters for aqueous electrochemiluminescence.

Chem Sci 2021 Oct 7;12(40):13283-13291. Epub 2021 Sep 7.

Centre for Advanced Analytical Science, c/o School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou Key Laboratory of Sensing Materials & Devices Guangzhou 510006 P. R. China

Due to overcoming the limitation of aggregation caused quenching (ACQ) of solid-state emitters, aggregation-induced emission (AIE) organic luminogens have become a promising candidate in aqueous electrochemiluminescence (ECL). However, restricted by the physical nature of fluorescence, current organic AIE luminogen-based ECL (AIECL) faces the bottleneck of low ECL efficiency. Here, we propose to construct aqueous ECL based on aggregation-induced delayed fluorescence (AIDF) luminogens, called AIDF-ECL. Compared with the previous organic AIE luminogens, purely organic AIDF luminogens integrate the superiorities of both AIE and the utilization of dark triplets thermal-activated spin up-conversion properties, thereby possessing the capability of close-to-unity exciton utilization for ECL. The results show that the ECL characteristics using AIDF luminogens are directly related to their AIDF properties. Compared with an AIECL control sample based on a tetraphenylethylene AIE moiety, the ECL efficiency of our AIDF-ECL model system is improved by 5.4 times, confirming the excellent effectiveness of this innovative strategy.
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http://dx.doi.org/10.1039/d1sc02918eDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8528032PMC
October 2021

An aggregation-induced emission platform for efficient Golgi apparatus and endoplasmic reticulum specific imaging.

Chem Sci 2021 Oct 5;12(41):13949-13957. Epub 2021 Oct 5.

Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research, Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong 999077 China

As two important subcellular organelles in eukaryotic cells, the Golgi apparatus (GA) and endoplasmic reticulum (ER) have recently captivated much interest due to their considerable importance in many biofunctions and role as critical biomarkers for various diseases. The development of efficient GA- and ER-specific probes is of great significance, but remains an appealing yet significantly challenging task. Herein, we reported for the first time the construction of an aggregation-induced emission (AIE) platform for GA and ER fluorescent probes, termed as AIE-GA and AIE-ER, by facile synthesis and simple functionalization. Their excellent targeting specificity to GA or ER, remarkable photostability, high brightness, and low working concentration make AIE-GA and AIE-ER significantly impressive and superior to commercially available probes. Moreover, molecular docking calculations are performed to validate the targeting mechanism of the two AIE probes.
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http://dx.doi.org/10.1039/d1sc03932fDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8549777PMC
October 2021

Near-infrared luminescent probes for bioimaging and biosensing.

Chem Sci 2021 Mar 17;12(10):3377-3378. Epub 2021 Mar 17.

Department of Chemistry, The Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, Institute for Advanced Study, Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China

Fan Zhang and Ben Zhong Tang introduce the themed issue on Near-infrared luminescent probes for bioimaging and biosensing.
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http://dx.doi.org/10.1039/d1sc90046cDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8562496PMC
March 2021

Aggregation-induced emission luminogens for image-guided surgery in non-human primates.

Nat Commun 2021 11 10;12(1):6485. Epub 2021 Nov 10.

Eye Center, the Second Affiliated Hospital, Zhejiang University School of Medicine, Hangzhou, 310009, China.

During the past two decades, aggregation-induced emission luminogens (AIEgens) have been intensively exploited for biological and biomedical applications. Although a series of investigations have been performed in non-primate animal models, there is few pilot studies in non-human primate animal models, strongly hindering the clinical translation of AIE luminogens (AIEgens). Herein, we present a systemic and multifaceted demonstration of an optical imaging-guided surgical operation via AIEgens from small animals (e.g., mice and rabbits) to rhesus macaque, the typical non-human primate animal model. Specifically, the folic conjugated-AIE luminogen (folic-AIEgen) generates strong and stable fluorescence for the detection and surgical excision of sentinel lymph nodes (SLNs). Moreover, with the superior tumor/normal tissue ratio and rapid tumor accumulation, folic-AIEgen successfully images and guides the precise resection of invisible cancerous metastases. Taken together, the presented strategies of folic-AIEgen based fluorescence intraoperative imaging and visualization-guided surgery show potential for clinical applications.
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http://dx.doi.org/10.1038/s41467-021-26417-2DOI Listing
November 2021
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