Latest ArticlesMacromolecular drugs have attracted great interest as biotherapy to cure previously untreatable diseases. For clinical translation, biomacromolecules encounter several common druggability difficulties, such as in vivo instability and poor penetration to cross physiologic barriers, thus requiring sophisticated systems for drug delivery. Inspired by the natural biomineralization via interaction between inorganic ions and biomacromolecules, herein we rationally screened biocompatible transition metals to biomineralize with carbonate for macromolecules loading. Among the metal ions, Cu2+ was found to be the best candidate, and its superiority over the widely studied Ca2+ minerals was also demonstrated. Capitalized on this finding, copper carbonate nanoparticles were prepared via a simple mixing process to co-load glucose oxidase (GOx) and a HIF-α DNAzyme (DZ), achieving ultra-high loading capacity of 61%. Upon encapsulation into nanoparticles, enzymatic activity of both drugs was passivated to avoid potential side-effects during circulation, while the drugs could be rapidly released within 1 h in response to acidic pH to fully recover their activities. The nanoparticles could accumulate into tumor via intravenous injection, facilitate the cell membrane penetration, and release the payloads of GOx, DZ and Cu2+ inside cells to exert a series of anti-tumor effects. GOx caused tumor starvation by catalytic glucose consumption, and the concomitantly generated H2O2 byproduct boosted the Cu2+-mediated chemodynamic therapy (CDT). Meanwhile, the DZ silenced HIF-α expression to sensitize both starvation therapy and CDT. As a result, a synergistic tumor growth inhibition was achieved. This work provides a simple method to prepare biomineralized nanoparticles, and offers a general approach for macromolecular drugs delivery via Cu2+-based biomineralization.
Compared with other types of breast cancer, triple-negative breast cancer (TNBC) has the characteristics of a high degree of malignancy and poor prognosis. Early diagnosis of TNBC through biological markers and timely development of effective treatment methods can reduce its mortality. Many Research experiments have confirmed that some specific miRNA expression profiles in TNBC can used as markers for early diagnosis. However, detecting the expression profiles of multiple groups of miRNAs according to traditional detection methods is complicated and consumes many samples. To address this issue, we developed a method for high-throughput, high-sensitivity quantitative detection of multiple sets of miRNAs (including miR-16, miR-21, miR-92, miR-199, and miR-342) specifically expressed in TNBC by rolling circle amplification (RCA) on fluorescence-encoded microspheres. Through the optimization of reaction system conditions, the developed method showed an extensive linear dynamic range and high sensitivity for all five miRNAs with the lowest limit of detection of 2 fmol/L. Meanwhile, this high-throughput detection method also appeared reasonable specificity. Only in the presence of a specific target miRNA, the fluorescence signal on the correspondingly encoded microspheres is significantly increased, while the fluorescence signal on other non-correspondingly encoded microspheres is almost negligible. Furthermore, this process exhibited good recovery and reproducibility in serum. The advantages of this method allow us to more conveniently obtain the expression profiles of multiple groups of TNBC-associated miRNAs, which is beneficial for the early detection of TNBC.
Bioorthogonal reactions can take place in biological environments without interfering with biochemical processes. In this study, Pd(PPh3)2Cl2 was used as a bioorthogonal catalyst to in situ transform the stable N-heterocyclic carbene (NHC)-gold(I)-alkyne complex 5 to its active species which can effectively inhibit thioredoxin reductase (TrxR) and exhibit significant anticancer bioactivity in hepatocellular carcinoma (HCC).
Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy. In detail, H2 production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents. In this work, CdS quantum dots (CdS QDs) were successfully loaded onto the surface of a porphyrinic metal-organic framework (Pd-PCN-222) by the electrostatic self-assembly at room temperature. The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation, achieving a H2 production and benzylamine oxidation rate of 5069 and 3717 µmol g−1 h−1 with > 99% selectivity in 3 h. There is no noticeable loss of catalytic capability during three successive runs. Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6 clusters under visible-light irradiation, and thus CdS QDs and Zr6 clusters behave as the photocatalytic oxidation and reduction centers, respectively.
Metal-support interaction (MSI) is an efficient way in heterogeneous catalysis and electrocatalysis to modulate the electronic structure of metal for enhanced catalytic activity. However, there are still great challenges in promoting the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) simultaneously by this way. Herein, Fe-doped Co3O4 supported Ru (Ru/FeCo) catalysts are synthesized by MSI strategies to further improve the electrocatalytic activity and stability of the catalysts. The results show that the optimized Ru/FeCo catalyst exhibits the best catalytic performance. The HER and OER tests at 10 mA/cm2 in 1 mol/L KOH solution show excellent overpotentials of 155 mV and 283 mV, respectively. The activity and stability enhancement can be attributed to the MSI that effectively modify the electronic structure and improve interfacial electron transfer between Ru and Fe-doped Co3O4 (FeCo). This work provides an innovative direction for the design of high-efficiency bifunctional electrocatalysts by virtue of the MSI.
Multifunctional switchable materials are attracting tremendous interest because of their great application potential in signal processing, information encryption, and smart devices. Here, we reported an organic-inorganic hybrid thermochromic ferroelastic crystal, [TMIm][CuCl4] (TMIm = 1,1,3,3-tetramethylimidazolidinium), which undergoes two reversible phase transitions at 333 K and 419 K, respectively. Intriguingly, these three phases experience a remarkable ferroelastic-paraelastic-ferroelastic (2/m-mmm-2/m) transition, which remains relatively unexplored in ferroelastics. Moreover, the ferroelastic domains can be simultaneously switched under temperature and stress stimuli. Meanwhile, [TMIm][CuCl4] exhibits thermochromic phenomenon, endowing it with extra spectral encryption possibilities during information processing. Combined with dielectric switching behavior, [TMIm][CuCl4] are promising for practical applications in memory devices, next-generation sensors, and encryption technology.
Functional carbon nanomaterials have become the stars of many active research fields, such as electronics, energy, catalysis, imaging, sensing and biomedicine. Herein, a facile and one-pot strategy for generating ferromagnetic nanoparticles loaded on N-doped carbon nanosheets (Fe-N-CNS) is presented by salt-assisted high-temperature carbonization of natural silk proteins. Due to their graphitic structures, N-doping and ferromagnetic nanoparticles (FeNx, FeOy, FeCz), the silk-derived Fe-N-CNS can act as excellent mimics of both peroxidase and oxidase. Benefiting from the combined character of the graphene-like structures and enzyme-like activities, Fe-N-CNS can be further applied to highly efficient dye removal via synergistic adsorption and degradation. Meanwhile, the as-prepared Fe-N-CNS with intrinsic magnetism and electrical conductivity can also serve as an efficient electromagnetic wave absorption agent. The broadest effective absorption bandwidth (EAB) of as-obtained absorbing material yields a 6.73 GHz with 1 mm thickness, with a maximum reflection loss of −37.33 dB (11.41 GHz). The EAB can cover 2~18 GHz with a tunable absorber thickness from 1.0 mm to 5.0 mm. Collectively, Fe-N-CNS, as a dual-functional material, can tackle the aggravating environmental pollution issues of both dyes and electromagnetic waves.
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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