Latest ArticlesEngineering 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.
Organics present significant prospects as environmentally friendly and sustainable electrode materials for potassium ion batteries (PIBs) because of their abundant, recyclable and highly customizable characteristics. However, small molecular organics are easily solubilized in organic electrolytes, resulting in a low capacity and poor stability. Herein, the folic acid-based supermolecules (SM-FAs) are successfully prepared by a hydrothermal assisted self-assembly strategy. Due to multi-locus hydrogen bonds (HBs) and the cyclized π-conjugated interactions, the structural stability of SM-FAs has been significantly improved, and the solubility in carbonate electrolytes has been effectively inhibited. As an anode for PIB, the SM-FA-6 sample exhibits a large capacity (206 mAh/g at 50 mA/g) and an outstanding cycle stability (capacity retention of 91% after 1000 cycles at 50 mA/g). More impressively, an integrative storage mechanism which combines both the general enolization reaction between C=O groups and K+, and the atypical π–K+ interaction within the assembled conjugation framework, is unraveled for potassium ion accumulation. It is envisioned that this facile self-assemble strategy opens up a promising avenue to modulate the stability of small molecular organic electrodes with enhanced storage capacity.
Most porous conductive frameworks are highly anisotropic in their structures thus leading to anisotropic charge transport. Here we report a supramolecular self-assembly which is constructed by intermolecular hydrogen bonding and π···π interactions. This material features a chiral, porous, cubic framework structure with π-stacked helical columns along all of the three Cartesian coordinates. As a result, isotropic charge transport with an electrical conductivity (σ) of 2.1 × 10–7 S/cm is achieved. By achieving isotropic charge transport in a π-stacked supramolecular assembly, these results provide a new type of isotropic conductive framework materials alternative to conductive metal-organic frameworks (MOFs).
We report here a generic, green synthesis of 17 valuable syn-aryl-(2S,3R)-2–chloro-3–hydroxy esters (syn-(2S,3R)-1) in 73%-99% isolated yields along with 6.1:1–83:1 dr and 31%~ > 99% ee, through dynamic reductive kinetic resolution of racemic aryl α–chloro β-keto esters (2) catalyzed by an engineered ketoreductase which was obtained via epPCR-based directed evolution. The hectogram scale synthesis of syn-(2S,3R)-1b at a substrate concentration of 120 g/L showcased the application potential of the biocatalytic method developed presently.
In-depth exploration of the relationship among different adsorption sites is conducive to design of efficient adsorbents for target pollutants removal from water. In this study, the experiments, multivariate non-linear regression and density functional theory calculations are applied to explore the possible synergistic effects of three nitrogen (N)-containing sites on cow dung biochar surface for sulfamethoxazole (SMX) adsorption. Notably, a strong synergistic effect between pyridinic N and pyrrolic N sites was found for sulfamethoxazole adsorption. The adsorption energies of SMX on four pyrrolic N-coupled pyridinic N structures were −1.02, −0.41, −0.49 and −0.72 eV, much higher than the sum of adsorption energies (−0.31 eV) on pyrrolic N and pyridinic N. Besides, the alteration of Mulliken charge revealed that the simultaneous presence of pyridinic N and pyrrolic N improved the electron transfer remarkably from −0.459 e and 0.094 e to −0.649 e and 0.186 e, benefiting for SMX adsorption. This work firstly explored the possible synergies of adsorption sites on biochar surface for organic contaminants removal from water, which shed new lights on the adsorption mechanism and provided valuable information to design efficient adsorbents in the field of water treatment.
Hydrogen evolution from water electrolysis has become an important reaction for the green energy revolution. Traditional precious metals and their compounds are excellent catalysts for producing hydrogen; however, their high cost limits their large-scale practical application. Therefore, the development of affordable electrocatalysts to replace these precious metals is important. Transition metal phosphides (TMPs) have shown remarkable performance for hydrogen evolution and garnered considerable interest in the field of electrolysis. Based on the detailed introduction of TMPs in previous studies, we have systematically summarized the preparation methods, improvement methods, and development opportunities of TMPs and proposed “stimulatory factors” as a fundamental factor affecting the performance of TMPs herein. As the core of this research, “stimulatory factors” can provide numerous solutions to improve the performance of TMP materials and provide a good starting point for TMP research.
Most catalytic processes are achieved by heating the whole reaction systems including the entire reactor, substrate and solvent, which leads to energy loss and obvious heat transfer limits. In this study, induction heating was employed to boost the catalytic Suzuki-Miyaura cross-coupling reactions by using conductive superparamagnetic microspheres with loaded Pd nanoparticles as heterogeneous catalysts. It was found that, at the same apparent reaction temperatures, the reactions by adopting the induction heating all exhibit better catalytic performance with higher conversion and yield, as compared to the reactions using conventional joule heating. The improvement is mainly attributed to the localized heating effect endowed by high efficiency of the heat transfer from the heat source to catalytic sites, which dissipates the electromagnetic energy through Néel relaxation mechanism. Moreover, it has be found that the reactions have been largely accelerated, resulting in much shorter reaction time required to approach a given value of reactant conversion. These results indicate that the unique heating method based on the superparamagnetic nanomaterials as both the inductive component and catalyst support holds a promising application for fast and efficient heterogeneous catalytic process, and exhibits potential for improving energy transfer efficiency and reducing the side reactions attributed to the uneven temperature profile.
Integrating discrete plasmonic nanoparticles into assemblies can induce plasmonic coupling that produces collective plasmonic properties, which are not available for single nanoparticles. Theoretical analysis revealed that plasmonic coupling derived from assemblies could produce stronger electromagnetic field enhancement effects. Thus, plasmonic assemblies enable better performance in plasmon-based applications, such as enhanced fluorescence and Raman effects. This makes them hold great potential for trace analyte detection and nanomedicine. Herein, we focus on the recent advances in various plasmonic nanoassembles such as dimers, tetramers, and core-satellite structures, and discuss their applications in biosensing and cell imaging. The fabrication strategies for self-assembled plasmonic nanostructures are described, including top-down strategies, self-assembly methods linked by DNA, ligand, polymer, amino acid, or proteins, and chemical overgrowth methods. Thereafter, their applications in biosensor and cell imaging based on dark-field imaging, surface-enhanced Raman scattering, plasmonic circular dichroism, and fluorescence imaging are discussed. Finally, the remaining challenges and prospects are elucidated.
Macromolecular 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.
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