Latest ArticlesTherapeutic cancer vaccines have undergone a resurgence in the past decade. Because of the high level of immune cell accumulation and abundant capillary lymphatic system in the dermis, percutaneous vaccination is considered to be an ideal treatment route. For convenient administration, the recent development of microneedles (MNs) provides a safe, painless, and low-cost transdermal delivery strategy, which could bypass the first-pass metabolism of vaccines for enhanced stability and bioavailability. However, the therapeutic effect of MNs-based cancer vaccines is not optimal, which is limited by the complex set of host, tumor, and environmental factors, as well as the limited vaccine loading capacity. Therefore, further improvements are still required to push their clinical translation. In this critical review, we deliberate on how to improve the therapeutic effect of MNs-based vaccines for cancer immunotherapy, summarize the recent advances in MNs-based cancer vaccination, and provide an overview of various design strategies and mechanisms for active or passive targeting delivery, aiming to develop safer, more effective, and more stable MNs-based cancer vaccines. Finally, we briefly describe the potential of vaccine platforms in combination with other therapies, suggest the need to design vaccines according to specific circumstances, and discuss the biosafety of repeated administration for enhancing clinical efficacy.
Geminal diboronates and diarylmethyl boronates are versatile building blocks in synthetic chemistry. We here reported a highly efficient approach for the synthesis of gem-bisborylalkanes and diarylmethyl boronates via cobalt-catalyzed deoxygenative borylation of diaryl ketones. This borylation protocol is compatible with a broad range of functionalized aryl groups, providing access to a wide array of boronic esters. The resulting boronic esters can be further transformed to various cross-coupling products and TPEs that represent important structural motifs in organic chemistry and materials science.
Accurate detection of uric acid (UA) is crucial for diagnosing gout, yet traditional sweat-based UA sensors continue to face challenges posed by complex and costly electrode fabrication methods, as well as weakly hydrophilic substrates. Here, we designed and developed simple, low-cost, and hydrophilic sweat UA detection sensors constructed by carbon electrodes and cellulose paper substrates. The carbon electrodes were made by carbonized polyimide films through a simple, one-step laser engraving method. Our electrodes are porous, possess a large specific surface area, and are flexible and conductive. The substrates were composed of highly hydrophilic cellulose paper that can effectively collect, store, and transport sweat. The constructed electrodes demonstrate high sensitivity of 0.4 µA L µmol−1 cm−2, wide linear range of 2–100 µmol/L. In addition, our electrodes demonstrate high selectivity, excellent reproducibility, high flexibility, and outstanding stability against mechanical bending, temperature variations, and extended storage periods. Furthermore, our sensors have been proven to provide reliable results when detecting UA levels in real sweat and on real human skin. We envision that these sensors hold enormous potential for use in the prognosis, diagnosis, and treatment of gout.
The efficient production of high-quality scintillators with long radioluminescence afterglow is crucial for high-performance X-ray luminescence extension imaging. However, scaling-up the synthesis of ligand-free scintillators to fabricate large-area X-ray imaging screens for industrial applications remains a challenge. In this study, we report an efficient method to synthesize ligand-free, lanthanide-doped microscintillators by a one-pot reaction via the concentrated hydrothermal method. The as-synthesized microscintillators exhibit prolonged persistent radioluminescence for up to 30 days after X-ray exposure and remain high stability in air or water for more than 18 months without deterioration. Monte Carlo simulations indicate that the size effect is responsible for the excellent afterglow performance of the microscintillators. We employ these high-quality lanthanide-doped microscintillators to fabricate a large-area X-ray imaging detector using a blade-coating method, a spatial resolution of 24.9 lp/mm for X-ray imaging. Our study offers a solution for scaling-up the synthesis of low-cost microscintillators for practical applications.
Pretreatment of the carrier for supported catalysts can effectively improve the strong metal-support interaction (SMSI) and increase the dispersion of precious metals, which are critical to many important catalytic reactions. In this work, we tuned SMSI on Pd/TiO2 catalysts through inducing surface defects of TiO2 by pretreated with different atmospheres (H2/N2, N2, O2/N2) at the high temperature (800 ℃). Multiple characterization results illustrated that surface defects anchored Pd species and thus enhanced their dispersion. During reduction, Ti3+ species formed and transferred onto the metallic Pd species and then induced SMSI, which effectively stabilize Pd species in the metallic state. The stronger MSI, the more stability of Pd species. As a case, Pd/TiO2–800H2, with strongest MSI, displayed the best HCHO oxidation performance at low temperature (10 ℃).
The design and syntheses of metal-organic cages (MOCs) based on polyoxometalates (POMs) building blocks have attracted increasing attention due to their intriguing molecular architectures and physicochemical properties. In this work, we have successfully synthesized and systematically characterized a tetrahedral polyoxometalate-based organic cage (POC), K3Na17H12[(C4H6O6)6[Ni4(OH)3(A-α-SiW9O34)]4]·96H2O (Ni16L6(SiW9)4), using tritopic Ni4-substituted Keggin cluster (Ni4SiW9) as nodes and flexible L-(+)-tartaric acid ligands as linkers. The resulting POC tetrahedron has been firstly investigated as efficient catalyst for visible-light-driven hydrogen production, achieving a turnover number of 15,500 after 96-h photocatalysis. Such high catalytic performance of Ni16L6(SiW9)4 POC catalyst could be attributed to its unique cage structure, thereby offering more efficient catalytic component accessibility. In addition, spectroscopic analyses illustrated the photocatalytic mechanism and the structural stability of the TBA-Ni16L6(SiW9)4 catalyst during the photocatalytic process.
The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry. By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)2I and β-diketiminato FeⅡ chloride, the ferrogermylene complexes 3a, 3b and 4a were synthesized and structurally characterized. The structural and IR characterizations show the presence of the Ge←Fe π backbonding in molecules 3a, 3b and 4a. The computational works on frontier molecular orbitals and their comparison of energy states confirmed that σ donation and π backbonding are both weak in these molecules, despite three complexes have longer Ge-Fe bonds, whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a, 3b to 4a.
Promethazine (PHZ) is used as a sedative in veterinary medicine, and its residue can threaten the health of human. The electrochemical detection of PHZ is suitable method for application in the field. However, the traditional electroanalysis is difficult to perform directly in meat samples due to matrix interference. This work integrates magnetic solid-phase extraction and differential pulse voltammetry for highly sensitive and selective determination of PHZ in beef and beef liver for the first time. CoFe2O4/graphene coated with C18-functionalized mesoporous silica (MG@mSiO2-C18) is synthesized as dispersed magnetic adsorbent to extract PHZ. Magnetic glassy carbon electrode modified with nitrogen-doped hollow carbon microspheres (HCM) attracts the MG@mSiO2-C18 with PHZ, and directly detects the PHZ without elution procedure. MG@mSiO2-C18 can separate PHZ to avoid the interference of impurities on following detection, and also concentrate PHZ on magnetic electrode. Additionally, the electrode modification with HCM can amplify the electrochemical signal of PHZ. Finally, the integrated PHZ determination method exhibits a wide linear range from 0.08 µmol/L to 300 µmol/L with a low limit of detection of 9.8 nmol/L. The beef sample analysis presents excellent recovery, demonstrating that this protocol is promising for the rapid and onsite detection of PHZ in real meat samples
Introducing covalently crosslinked network to polymer matrix can merge the advantages in reprocessing and durability of polymers. In this contribution, a series of high-performance vitrimeric elastomers were achieved via polycondensation. The topological structures of polymers were tuned by varying the feeding ratios of bisacetoacetate, hex–substituted bisacetoacetate, bisamine and tris(2-aminoethyl)amine. With these structural manipulations, the vitrimeric elastomers presented great elastic recovery properties (strain recovery value up to 80%) benefiting from the introduction of long chain branch. Furthermore, the elastomers exhibited excellent reprocessing property, water vapor/oxygen barrier and adhesive properties. Specially, the elastomers could be degraded into monomer under acid conditions which enabled the elastomer synthesis again in closed loop recycling system. The ease of the polycondensation in this work to prepare highly elastic and recyclable vitrimeric elastomers demonstrated exciting opportunities for the synthesis of sustainable polymers.
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