Latest ArticlesThe precise synthesis of polymer with narrow molecular weight distribution (Đ) and well-defined architectures is very essential to exploring the functions and properties of polymer materials. Here, a universal polymerization method capable of low Đ and reactive hydrogen compatibility is reported by introducing super-Grignard reagents (R2Mg·LiCl) into polymer chemistry. Under mild conditions, various monomers, including nonpolar polystyrene and 4-methoxystyrene that cannot be initiated by Grignard reagents, and polar methacrylate, are successfully polymerized with full monomer conversion and low Đ. This approach is amenable to wide varieties of initiators, polymerization temperature, and feed ratio, which makes it attractive for applications in polymer synthesis. By adding methanol and water during the polymerization process, the reactive hydrogen compatibility of this method is confirmed, which makes this method avoid the rigorous restriction on polymerization conditions of anionic polymerization. Moreover, chain extension polymerization and block copolymerization are achieved and demonstrate the livingness of chain propagation, enabling the facile synthesis of well-defined macromolecular architectures. This work therefore expands the methodology libraries of living polymerization, which may cause inspirations to polymer science.
Forming J-aggregates by organic monomer is a fascinating strategy to urge spectroscopic redshift with respect to that of the monomer. Herein, we designed 1,7-diphenyl-substituted meso–CF3-BDP monomer confirmed by X-ray crystallographic analysis. The low-barrier rotation of the –CF3 group in meso–CF3-BDP 1 significantly enhances the non-radiative efficiency, and the photothermal conversion efficiency (PCE) of the self-assembled nanoparticles (1-NPs: λabs = 746 nm) by J-aggregates was 82%. 1-NPs could effectively block cell cycle progression, inhibit cancer cell proliferation and trigger cell apoptosis under low power laser irradiation (0.2 W/cm2). This study proposes an alternate molecular design platform by J-aggregates to promote PCE through the insertion of rotating segment and trigger the cancer cells apoptosis in photothermal therapy at low power laser density.
Photoimmunotherapy is an emerging treatment modality that uses photothermal, photodynamic and photochemical processes to fight against cancer by eliciting a robust host immune response. Recently, various nanoformulations of biomaterials have been rationally designed as highly effective photosensitive agents, immunoadjuvants or carriers to enhance phototherapeutic efficacy, boost immune stimulation, amplify nano-permeability and monitor cancer progression in situ. Nevertheless, relying solely on a single-modality therapy may not completely ablate primary tumors, and the metastasis and recurrence of tumors remain a serious challenge. To solve this issue, the strategy of combining photoimmunotherapy with other immunotherapies, such as immune checkpoint blockade, chimeric antigen receptor-T cell or cytokine therapy, can greatly enhance the effectiveness of oncology treatment and reduce the traditional adverse effects. Thus, it is very valuable to summarize the research progress in biomaterial-assisted combination photoimmunotherapy for clinical translation. In this review, the recent advances in constructing multifunctional nano-biomaterials for combinatorial photoimmunotherapy of cancer are summarized. Furthermore, the opportunities, challenges, future trends and prospects in this field are also analyzed to pave the way for advancing the next generation of clinical cancer management strategies.
Applying the fluorescent carbon dots as smart materials in anticancer therapy is of great interest. However, carbon dots for multimodal synergistic anticancer therapy, especially for the triple modality, is rarely reported. Herein, we successfully synthesized OCDs by citric acid and (1R, 2S)-2-amino-1,2-diphenylethan-1-ol, which show aggregation-induced emission property and two-photon fluorescence imaging. Meanwhile, OCDs are ideal photosensitizers for photothermal therapy under 808 nm and Type Ⅰ photodynamic therapy with white light. Hydroxyl radicals, generated by Type Ⅰ photodynamic therapy based on OCDs can transform protumoral M2 macrophages into antitumoral M1 macrophages, which exhibited immunotherapy ability. The synergism trimodal of OCDs results in potent anticancer efficacy, showing great potential in cancer therapy.
The cancer cells realize their proliferation and metastasis activities based on the special redox adaptation to increased reactive oxygen species (ROS) level, which inversely makes them sensitive to external interference with their redox state. In view of this, in recent decades, researchers have made great efforts to construct a series of novel nanoplatform-based ROS-mediated cancer therapies through increasing ROS generation and inhibiting the ROS elimination. Besides, the multidrug resistance and thermoresistance of tumor are closely related to tumor redox state. Recently, numerous works have shown that ROS regulation in cancer cells can intervene in the expression, function and stability of related proteins to achieve reversal of tumor resistance. In this review, the recent researches about ROS-regulating nanoagents on cancer therapy and tumor resistance alleviation have been well summarized. Finally, the challenges and research directions of ROS-regulating nanoagents for future clinical translation are also discussed.
Fluorescence-guided surgery calls for development of near-infrared fluorophores. Despite the wide-spread application and a safe clinical record of Indocyanine Green (ICG), its maximal absorption wavelength at 780 nm is rather short and longer-wavelength dyes are desired to exploit such benefits as low photo-toxicity and deep penetration depth. Here, we report ECY, a stable deep near-infrared (NIR) fluorochromic scaffold absorbing/emitting at 836/871 nm with a fluorescence quantum yield of 16% in CH2Cl2. ECY was further rationally engineered for biological distribution specificity. Analogous bearing different numbers of sulfonate group or a polyethylene glycol chain were synthesized. By screening this focused library upon intravenous injection to BALB/c mice, ECYS2 was identified to be a suitable candidate for bioimaging of organs involved in hepatobiliary excretion, and ECYPEG was found to be a superior candidate for vasculature imaging. They have potentials in intraoperative imaging.
Photothermal therapy (PTT) induces thermoresistance through cellular heat shock response, which impairs the therapeutic efficacy of the PTT. To resolve this problem, we developed a photothermal theranostics (denoted as PMH), which integrated the photothermal conversion agent of PdMo bimetallene with histone deacetylase 6 (HDAC6) selected inhibitor (ACY-1215), showing the synergistic antitumor effect both in vitro and in vivo. Mechanistically, under the photoacoustic imaging (PA) navigation, the released ACY-1215 triggered by NIR laser irradiation decrease the heat shock proteins (HSPs) expression and weaken the HDAC6-regulated HSP90 deacetylation, thus hindering the degradation of PTT-induced misfolded or unfold proteins through proteasome dependent pathway. Moreover, mild photothermal therapy (mPTT) treatment compromised the autophagy, which induced by HDAC6 inhibition, leading to mPTT-induced misfolded or unfold proteins further accumulation. Given that inhibition of HDAC6 plus mPTT contribute to tumor eradication. This study develops a promising combination strategy based on mPTT for future cancer treatment.
A phytochemical investigation on Isodon flavidus led to the isolation of flavidanolide A (1), a rearranged diterpenoid featuring a six/seven/five-membered tricyclic skeleton, together with flavidanolide B (2), an uncommon heterodimeric diterpenoid consisting of a norabietane and a seco-isopimarane monomeric units. Their structures were elucidated by extensive spectroscopic data and single-crystal X-ray diffraction analyses. Their plausible biosynthetic routes were also proposed. In the bioassay, flavidanolide B was found to exhibit good inhibitory effect against lipopolysaccharide (LPS)-induced nitric oxide (NO) production in RAW264.7 cells comparable to positive control pyrrolidinedithiocarbamate ammonium (PDTC), which provided evidence for the medicinal value of I. flavidus as a folk medicine for treating inflammatory diseases.
An amphiphilic AIE photosensitizer has been successfully developed, which allows for easily inserting into the bacterial membranes. Binding experiments with phospholipid preliminary demonstrates its membrane specificity. As expected, it is proved to possess a broad-spectrum bacterial staining performance and photodynamic antibacterial activity toward S. aureus and E. coli.
Engineering small-molecule drugs into nanoparticulate formulations provides an unprecedented opportunity to improve the performance of traditional chemo drugs, but suffers from poor compatibility between drugs and nanocarriers. Stimuli-responsive mPEG-PDLLA–drug conjugate-based nanomedicines can facilitate the exploitation of beneficial properties of the carrier and enable the practical fabrication of highly efficacious self-assembled nanomedicines. However, the influence of hydrophobic length on the performance of this type of nanomedicine is little known. Here we synthesized two acid-sensitive ketal-linked mPEG-PDLLA–docetaxel prodrugs with different lengths of PDLLA, and engineered them into self-assembled sub-20 nm micellar nanomedicines for breast cancer chemotherapy. We found that the nanomedicine consisting of a mPEG-PDLLA–docetaxel prodrug with the shorter length of PDLLA stood out due to its potent cytotoxicity, deep penetration into multicellular spheroids, and improved in vivo anticancer performance. Additionally, our prodrug-based nanomedicines outperformed the generic formulation of commercial Nanoxel in terms of safety profile, tolerated doses, and tumor suppression. Our findings indicate that the hydrophobic content of a polymeric prodrug nanomedicine plays an important role in the performance of the nanomedicine, and should be instructive for developing polymeric prodrug-based nanomedicines with clinical translational potential.
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