Latest ArticlesPolyimide-linkage covalent organic frameworks (PI-COFs), as a subclass of the COFs material family, featuring the unique combination of excellent thermal stability of polyimide, tunable pore sizes, as well as high crystallinity and surface area of COFs, are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation, catalysis, chemical sensing, and energy storage. Therefore, it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development. In this review, we offer a comprehensive overview of recent advancements in PI-COFs, emphasizing their synthesis methods, design principles and applications. Finally, our brief outlooks on the current challenges and future developments of PI-COFs are provided. Overall, this review aims to guide the recent and future development of PI-COFs.
Although the combination of chemotherapy and immunotherapy can improve the treatment of breast cancer, traditional drugs are highly toxic because they do not specifically target tumors. In this study, we developed a self-driving bacteria/nanoparticle biohybrid called Bif@PDA-aPD1/DOX-Lip by attaching polydopamine (PDA) coated doxorubicin (DOX) liposomes and the immune checkpoint inhibitor anti-programmed cell death protein 1 antibody (aPD-1) to Bifidobacterium infantis (B. infantis, Bif). Using the homing abilities of bacteria, Bif@PDA-aPD1/DOX-Lip could actively accumulate in tumor tissue, releasing DOX and aPD-1 in the acidic environment to have a synergistic anti-tumor effect. Results show that the concentration of DOX in tumors of the Bif@PDA-aPD1/DOX-Lip group was 6.31 times higher than in the free DOX group. The combination of DOX and aPD-1 not only killed tumor cells but also promoted immune normalization by maturing dendritic cells (DCs), increasing M1 macrophage ratio, and enhancing infiltration of CD8+ and CD4+ T cells in tumors and spleen. Therefore, Bif@PDA-aPD1/DOX-Lip therapy significantly inhibited tumor growth and increased the average survival time of mice to over 80 days. The Bif@PDA-aPD1/DOX-Lip biomotors offer a highly effective method for enhancing chemo-immunotherapy in solid tumors.
Adjuvants enhance and prolong the immune response to therapeutic agents, such as drugs and vaccines. However, conventional adjuvants have limitations in terms of immune specificity and duration. Nanoadjuvants can leverage their nanoscale size to increase the capture efficacy of antigens by antigen-presenting cells and improve immunogen presentation for targeted delivery. Furthermore, noninvasive visualization of bifunctional nanoadjuvants with integrated efficacy and imaging postdelivery can provide insights into in vivo distribution and performance, aiding in the optimization and design of new dosage forms. This review systematically summarizes the structure, assembly, and function of nanoadjuvants alongside contrast agents. It delves into the impact of complex structures formed by nanoadjuvant-contrast agent interactions on antigen presentation, migration, imaging tracking, and visualization of immune cell recruitment. It also discusses how imaging can determine optimal immune intervals, vaccine safety, and toxicity while enabling diagnostic and therapeutic integration. Moreover, this paper discusses potential applications of novel adjuvants and promising imaging technologies that could have implications for future vaccine and drug development endeavors.
Organic ambipolar emitting materials hold immense potential for application in integrated optoelectrical devices yet challenging to design and synthesize. Cocrystals exhibit significant superiority in designing such materials because the properties of emission and transport can be flexibly tailored through the strategic pairing of donor and acceptor units. In this study, we report a new cocrystal system, DPA-5FDPA, derived from two high-mobility emissive molecules, 2,6-diphenylanthracene (DPA) and 2,6-diperfluorophenyl anthracene (5FDPA). This cocrystal system exhibits outstanding emission and ambipolar semiconducting properties. Notably, the single-crystal field-effect transistor devices based on DPA-5FDPA achieve maximum hole and electron mobilities of 0.298 cm2 V-1 s-1 and 0.009 cm2 V-1 s-1, respectively. In comparison, the reference compound of 2-perfluorophenyl-6-phenylanthracene (5FBA) exhibits unipolar p-type transport with the hole mobility of 0.008 cm2 V-1 s-1. In addition, DPA-5FDPA exhibits excellent optical waveguide behavior with a small optical loss coefficient of 0.079 dB/µm at 508 nm, which is lower than most reported cocrystal systems. These results underscore the promise of co-crystallization as a versatile strategy for developing advanced ambipolar emissive semiconductors and provide deeper insights into the relationships among molecular structures, packing modes, intermolecular interactions, and charge-transport properties.
Carbon-rich cycloarene macrocycles can adopt multiple atropisomeric forms due to steric hindrance restricting σ-bond rotation. These distinct conformations exhibit variations in cavity structure, electronic properties, and functional site distribution, leading to diverse molecular recognition and self-assembly behaviors. In recent years, research on carbon-rich cycloarene macrocyclic compounds has emerged as a cutting-edge and interdisciplinary focus in the fields of carbon-rich functional molecules and macrocyclic chemistry. This review provides a comprehensive overview of the development of atropisomers in carbon-rich cycloarene macrocycles, spanning their design and synthesis, optoelectronic properties, and supramolecular chemistry.
Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics. To tune the emission behavior and mechanical property of molecular crystals simultaneously via supramolecular salt strategy is rarely reported, which is very important to improve their photophysical behavior and softness for the fabrication of flexible light-emitting device. Herein, supramolecular salt approach has been successfully applied to synthesize two elastic organic fluorescent crystals (CMOH-Py-Cl and CMOH-Py-Br) derived from non-emissive and brittle pyridine-substituted coumarin derivative (CMOH-Py). Their elastic properties can be attributed to the prevalent presence of numerous weak interactions introduced by halogen atoms, which are beneficial to the absorption and release of mechanical energy. Furthermore, density functional theory (DFT) calculations demonstrated a narrowing of the HOMO–LUMO energy gaps from CMOH-Py to CMOH-Py-Cl/CMOH-Py-Br via supramolecular salt approach. Finally, the application of flexible crystal materials in the field of optical waveguides has been investigated. The transformation of crystals in terms of photophysical and mechanical properties, achieved by the supramolecular salt approach, offers novel insights into the design and construction of flexible crystalline materials, providing a new path for the development of next-generation smart materials.
Possessing excellent mechanical properties, a high-coverage slide-ring conductive gel is constructed by in situ polymerization of α-cyclodextrin (α-CD) polyrotaxane (PR) and 1-vinyl-3-ethylimidazolium bromide ([VEIM]Br) ionic liquid (IL), using 1-ethyl-3-methylimidazolium bromide ([EMIM]Br) IL as solvent. Benefiting from the compatibility of ILs and alkene-PR, the cross-linked network slide-ring gel not only maintains excellent conductivity (1.52 × 10−2 S/m), but also has effectively improved mechanical properties (513% fracture strain, 0.713 MPa fracture stress, 211 kPa elastic modulus and 1366 kJ/m3 toughness) and adhesive properties (472.3 ± 25.9 kPa). The supramolecular gel can be used as a strain sensor to efficiently monitor deformation signals in real-time at least 200 times. Especially, the slide-ring gel can self-power generated by triboelectric effect and electrostatic induction between the skin layer and the polydimethylsiloxane (PDMS) layer that encapsulates the gel, achieving reversible and durable motion sensing, which provides a convenient pathway for constructing supramolecular self-powered flexible electronic materials.
Boron (B) doping serves as a promising strategy to enhance the quantum yield, photostability and environmental robustness of graphene quantum dots (GQDs). In this study, we reported a light-driven strategy for the facile synthesis of boron-doped graphene quantum dots (B-GQDs). Specifically, under continuous stirring at room temperature, ultraviolet irradiation induces the progressive polymerization of o-phenylenediamine (o-PDA) precursors, resulting in the formation of GQDs; meanwhile, 2-hydroxyphenylboronic acid (2-HPBA), acting as the B source, participates in the polymerization reaction with o-PDA intermediates, ultimately yielding B-GQDs. This approach significantly improves the technology of preparing QDs, yielding B-GQDs with a remarkably high fluorescence quantum yield of 71.2%. Detailed investigations reveal that the abundant surface functional groups on B-GQDs facilitate hydrogen-bonding interactions with water molecules, enabling their application as fluorescent probes for the quantitative detection of water content in various organic solvents. By integrating B-GQDs, a paper-based fluorescent sensor was successfully designed, achieving ultra-portable water content detection with excellent performance (0%-100%).
Peptides play important roles in chemistry, medicinal chemistry and life science, due to their high efficiency and specificity, unusual biological and therapeutic properties. As naturally occurring peptides often face with their intrinsic limitations including metabolic instability and low membrane permeability, the strategies for synthesizing unnatural amino acids and peptides are explored. Among the methods for modifying amino acids and peptides, chemo- and site-selective approaches are preferred because of the ability to fine-tuning structural features. Recently, transition metal-catalyzed C-H activation has been employed for the functionalization of amino acids and peptides. Through domino C-H activation/annulation, a series of structurally complex and diverse amino acids and peptides is constructed. This review highlights recent advances in the synthesis of unnatural amino acids and peptides via transition metal-catalyzed C-H activation/annulation.
Azobenzene-winged phenanthrolines (L1 and L2) were designed, synthesized, and fully characterized. Ligand L1 forms an in-situ cobalt complex, which has been effectively employed as a circular dichroism (CD)-active chiral sensor. The resulting ternary complex (L1–Co2+–amino alcohol) exhibits pronounced exciton-coupled circular dichroism (ECCD) signals at the characteristic azobenzene absorption bands. These signals arise from efficient chirality transfer from the chiral amino alcohol to the azobenzene chromophores, enabling the determination of the absolute configuration of chiral amino alcohols. Accordingly, the L1–Co2+ coordination system demonstrates considerably potential in chirality sensing applications. Remarkably, the induced ECCD signals are highly responsive to multiple external stimuli, including photoirradiation, solvent polarity, temperature, and redox conditions. In particular, temperature and redox changes can induce a reversible inversion of the ECCD signal, thereby establishing this system as a multifunctional, stimuli-responsive chiroptical molecular switch.
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