Latest ArticlesDNA nanomaterials hold great promise in biomedical fields due to its excellent sequence programmability, molecular recognition ability and biocompatibility. Hybridization chain reaction (HCR) is a simple and efficient isothermal enzyme-free amplification strategy of DNA, generating nicked double helices with repeated units. Through the design of HCR hairpins, multiple nanomaterials with desired functions are assembled by DNA, exhibiting great potential in biomedical applications. Herein, the recent progress of HCR-based DNA nanomaterials for biosensing, bioimaging and therapeutics are summarized. Representative works are exemplified to demonstrate how HCR-based DNA nanomaterials are designed and constructed. The challenges and prospects of the development of HCR-based DNA nanomaterials are discussed. We envision that rationally designing HCR-based DNA nanomaterials will facilitate the development of biomedical applications.
Protein S-sulfenylation (protein sulfenic acid), as one of the most significant oxidative post-translational modifications (OxiPTMs), plays a vital role in regulating protein function. A variety of activity-based probes have been developed to profile sulfenic acid in living cells. However, due to the transient presence and low content of sulfenic acid in living cell, high doses of probes are needed to achieve efficient labeling. More importantly, current probes have no temporal control over sulfenic acid labeling. To overcome these limitations, two caged cysteine sulfenic acid probes DYn-2-ONB and DYn-2-Cou with either an o-nitrobenzyl or coumarin protecting group were developed in this study. Both probes can be efficiently uncaged via irradiation to produce the active C-nucleophile probe DYn-2. Labeling assay in living cells demonstrated DYn-2-ONB exhibited better labeling capacity compared with DYn-2, providing it as a powerful tool for improved monitoring of protein S-sulfenylation in living cells.
Artificial photocatalytic energy conversion is considered as the most potential strategy for solving the increasingly serious energy crisis and environmental pollution problems by directly capturing solar energy. Therefore, high efficiency photocatalyst has drawn significant research attention in recent years. Due to the excellent electronic, optical, structural, and physicochemical performances, silver-based g-C3N4 have become promising photocatalysts. This review emphasizes the recent progresses and challenges on g-C3N4 decorated with silver for photocatalytic energy conversion. The extensive use of g-C3N4 decorated with silver in diverse photocatalytic reactions, including hydrogen evolution, pollutant degradation and carbon dioxide reduction, is also fully introduced. In addition, we propose the perspectives of g-C3N4 decorated with silver on photocatalytic applications. We hope that this review will shed some light on the photocatalytic energy conversion of g-C3N4 decorated with silver.
The construction of hydrogels with good mechanical properties and phosphorescent properties is full of challenges. Herein, we report a supramolecular phosphorescent hydrogel with long lifetime, high tensile strength and self-healing property, which can be easily constructed through in-situ thermal-initiated polymerization of isocyanatoethyl acrylate-modified β-cyclodextrin (β-CD-DA) and acrylate-modified adamantane (Ad-DA), acrylic acid (AA), followed by the non-covalent association with carbon dots (CNDs). The lifetime of phosphorescent hydrogel can reach 1261 ms at room temperature, and the quantum yield is 11%. Importantly, through the efficient triplet to singlet Förster resonance energy transfer (TS-FRET), the phosphorescent hydrogel shows the good phosphorescence energy transfer property for organic dyes Rhodamine B and Eosin Y with the delayed fluorescence lifetime up to 730 ms and 585 ms as well as the energy transfer efficiency (ΦET) up to 99.9% and 99.3%, respectively. Moreover, owing to the host-guest interactions between β-CD-DA and Ad-DA, the three-dimensional cross-linked network phosphorescent hydrogel can be easily stretched to 18 times of its original length, and can achieve self-healing of the cut surfaces within 30 min. These results will expand the scope of phosphorescent materials and provide new ideas and opportunities for materials science.
Exosomes are membrane-bound nanoscale extracellular vesicles, which produced by almost all organisms. Due to the excellent biocompatibility, long circulation time as well as low immunogenicity, exosomes as naturally-derived drug delivery carriers have experienced explosive growth over the past decades. However, issues such as insufficient loading efficiency, heterogeneous delivery efficiency, uncontrollable targeting ability, and low production limit their wide application. Recently, the emerging exosome–liposome fusion strategy has become a potential approach to solve such issues. Thus, this review mainly focuses on the currently developed exosome–liposome fusion strategy and their application in drug delivery as well as disease treatment. This review aims to shed light on the advantages of fusion strategy in drug delivery and provides a better understanding for more rational design. The current challenge and future perspective regarding their clinical translation and application will also be discussed.
Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer, regulate adsorption energy of reaction intermediates, and provide additional active sites, which are regarded as valid means for improving catalytic activity. However, the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear. Herein, the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel (NF) has been synthesized through continuous phosphating and reduction processes. The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities, and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm2 in 1 mol/L KOH, respectively. Moreover, as both the cathode and anode of overall water splitting, the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm2, which are far exceeding the benchmark commercial electrodes. DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor, tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates. Furthermore, the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site, avoid catalyst shedding, thus improving the activity and structural stability of NiCo/NiCoP. This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.
Stimuli-responsive smart materials exhibit reverse chemical/physical changes in response to external stimuli and research on stimuli-responsive smart materials with self-powered properties is still uncultivated ground. Here, we report perovskite crystalline self-powered multiple stimuli-responsive materials triggered by chemical and thermal stimuli. [HMEP]PbI3·(H2O) (1; HMEP is a hydroxytris(1-methylethyl)phosphorus cation) crystallizes in a chiral space group P21 at 293 K and has the piezoelectric reaction (d33 = 10 pC/N and output voltage = 1 V) of self-powered modes, this value is larger than the value of 3 pC/N for the classical piezoelectric material ZnO. Piezoelectric materials can generate energy due to mechanical deformation, and using thermal heating to lose water, [HMEP]PbI3 (2) can be obtained. 2 crystallizes in the non-centrosymmetric space group, undergoes two reversible phase transitions at 243/255 K and 315/348 K, and shows second harmonic generation switching. Interestingly, 2 can return to the hydrated form 1 after absorbing water. This work will lay the foundation for self-powered stimuli-responsive compounds and contribute to the construction of novel organic-inorganic hybrid materials with second harmonic generation switching.
Immune checkpoint inhibitors (ICIs) therapy targeting programmed cell death ligand 1 (PD-L1) and programmed death protein 1 (PD-1) had exhibited significant clinical benefits for cancer treatment such as triple negative breast cancer (TNBC). However, the relatively low anti-tumor immune response rate and ICIs drug resistance highlight the necessity of developing ICIs combination therapy strategies to improve the anti-tumor effect of immunotherapy. Herein, the immunomodulator epigallocatechin gallate palmitate (PEGCG) and the immunoadjuvant metformin (MET) self-assembled into tumor-targeted micelles via hydrogen bond and electrostatic interaction, which encapsulated the therapeutic agents doxorubicin (DOX)-loaded PEGCG-MET micelles (PMD) and combined with ICIs (anti-PD-1 antibody) as therapeutic strategy to reduce the endogenous expression of PD-L1 and improve the tumor immunosuppressive microenvironment. The results presented that PMD integrated chemotherapy and immunotherapy to enhance antitumor efficacy in vitro and in vivo, compared with DOX or anti-PD-1 antibody for the therapy of TNBC. PMD micelles might be a potential candidate, which could remedy the shortcomings of antibody-based ICIs and provide synergistic effect to enhance the antitumor effects of ICIs in tumor therapy.
Accurate and sensitive strategies for Concanavalin A (Con A) sensing are conducive to the better cognition of various important biological and physiological processes. Here, by designing dextran-functionalized fluorescent microspheres (DxFMs) and boric acid-modified carbon dots (BCDs) as recognition unit and built-in signal reference respectively, a ratiometric fluorescent detection platform was proposed for Con A detection with high reliability. In this protocol, the BCDs/DxFMs precipitation was formed due to the covalent interactions between cis-diol of DxFMs and boronic acid groups of BCDs, thus only fluorescence of BCDs could be detected in the supernatant. When Con A was presented, it could bind to DxFMs through its carbohydrate recognition ability and suppress the subsequent assembly between DxFMs and BCDs, leading to the simultaneous capture of DxFMs and BCDs fluorescence in the supernatant. Since the BCDs content was superfluous, their fluorescence intensities were basically constant in all cases. Based on the unchanged BCDs fluorescence signal and target-dependent DxFMs fluorescence signal in supernatant, the ratiometric detection of Con A was realized. Under optimized conditions, this ratiometric fluorescent platform displayed a linear detection range from 0.125 µg/mL to 12.5 µg/mL with a detection limit of 0.089 µg/mL. Moreover, satisfied analytical outcomes for Con A detection in serum samples were obtained, manifesting huge application potential of this ratiometric fluorescent platform in clinical diagnosis.
Lithium-rich layered cathode material (LLM) can meet the requirement of power lithium-ion energy storage devices due to the great energy density. However, the de/intercalation of Li+ will cause the irreversible loss of lattice oxygen and trigger transition metal (TM) ions migrate to Li+ vacancies, resulting in capacity decay. Here we brought Ti4+ in substitution of TM ions in Li1.2Mn0.54Ni0.13Co0.13O2, which could stabilize structure and expand the layer spacing of LLM. Moreover, optimized Ti-substitution can regulate the anions and cations of LLM, enhance the interaction with lattice oxygen, increase Ni3+ and Co3+, and improve Mn4+ coordination, improving reversibility of oxygen redox activation, maintaining the stable framework and facilitating the Li+ diffusion. Furthermore, we found 5% Ti-substitution sample delivered a high discharge capacity of 244.2 mAh/g at 50 mA/g, an improved cycling stability to 87.3% after 100 cycles and enhanced rate performance. Thereby Ti-substitution gives a new pathway to achieve high reversible cycle retention for LLMs.
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