Latest ArticlesVacancy 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.
Although it has been developed for many years, nucleic acid aptamer screening technology still fails to be widely used, a considerable part of it is due to the variability of tumor cell morphology, which leads to the use of immortalized cell lines in the laboratory to screen nucleic acid aptamers for recognition ability of tumor cells in the diseased body. To address this, primary cells that can be stably passaged were isolated and extracted from spontaneous tumors of genetically engineered pancreatic ductal adenocarcinoma model mice in this study. Next, an automated screening instrument for nucleic acid aptamers developed autonomously by our group was used to perform efficient aptamer screening using a limited number of cells, and the obtained nucleic acid aptamers were affinity verified at the cellular level. Finally, to answer the question of the cell growth environment difference on the recognition ability of nucleic acid aptamers, we verified its targeting ability to tumors in vivo on a nude mice xenograft tumor model, and further used a common antitumor drug doxorubicin combined with nucleic acid aptamers to verify the drug loading ability of this aptamer combined with the targeting therapeutic ability.
Two-dimensional (2D) MXenes have emerged as an archetypical layered material combining the properties of an organic-inorganic hybrid offering materials sustainability for a range of applications. Their surface functional groups and the associated chemical properties' tailorability through functionalizing MXenes with other materials as well as hydrophilicity and high conductivity enable them to be the best successor for various applications in textile industries, especially in the advancement of smart textiles and remediation of textile wastewater. MXene-based textile composite performs superb smartness in high-performance wearables as well as in the reduction of textile dyes from wastewater. This article critically reviews the significance of MXenes in two sectors of the textile industry. Firstly, we review the improvement of textile raw materials such as fiber, yarn, and fabric by using MXene as electrodes in supercapacitors, pressure sensors. Secondly, we review advancements in the removal of dyes from textile wastewater utilizing MXene as an absorbent by the adsorption process. MXene-based textiles demonstrated superior strength through the strong bonding between MXene and textile structures as well as the treatment of adsorbate by adsorbent (MXene in the adsorption process). We identify critical gaps for further research to enable their real-life applications.
Developing precise extracellular vesicles (EVs) labelling techniques with minimal disturbance is of great importance to the follow-up EVs detection and analysis. However, currently available methods such as using probes to conjugate phospholipids or membrane proteins have certain limitations due to EV steric hindrance, dye aggregation, etc. Here, we present a microfluidic platform to enhance EVs' labelling efficiency and improve their detection. This platform provides excellent sample throughput and high-efficiency EV labelling at lower label concentrations with an optimized flowing rate. Flow cytometry analysis (FCM) and cellular uptake results show that EV labelling by utilizing this platform possesses the merits of a higher labelling efficiency with 64.1% relative improvement than conventional co-incubation method and a lower background noise. Moreover, this technique maintains EVs' size, morphology and biological activities. After the recipient cells uptake the EVs treated by the microfluidic platform, the spatial and temporal distribution of EVs in the cells are clearly observed. These results demonstrate that our method holds great potential in efficient labelling of EVs, which is essential to subsequent EV quantification and analysis.
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.
Photodynamic therapy (PDT) is an effective treatment method for tumors. But the specifically accumulated of photosensitizer was very difficult in the tumor site, which greatly limited the efficacy of PDT. Here, mitochondria-targeted Janus mesoporous nanoplatform (JPMO-Pt-CTPP-ZnPc) for PDT was prepared, the nanoplatform has uniform size (275 nm) and good dispersion and biocompatibility. The confocal laser scanning microscopy (CLSM) revealed the signal of ZnPc of JPMO-Pt-CTPP-ZnPc were higher than JPMO-Pt-ZnPc in tumor cells, and flow cytometry results showed the cell uptake efficiency of JPMO-Pt-CTPP-ZnPc was 2.5-fold higher than that of JPMO-Pt-ZnPc. This revealed the modification of CTPP significantly improves the targeting ability of the nanoplatform. In vitro anti-tumor experiment showed the JPMO-Pt-CTPP-ZnPc significantly inhibited the growth of tumor cells upon the irradiation of low-power laser, and the survival rate of cells incubated with 60 µg/mL JPMO-Pt-CTPP-ZnPc was only 3%. Simultaneously, compared with JPMO-Pt-ZnPc (not modified with mitochondria targeting molecules CTPP), the PDT efficacy of JPMO-Pt-CTPP-ZnPc was significantly better, as it has targeted mitochondria in cells.
An atom economic β-C(sp3)−H chlorination of amide derivatives has been developed. This mild protocol employs CuCl2 instead of palladium catalysts with atom-economic HCl as chlorine sources and enables the late-stage functionalization of medicine derivatives. Mechanism studies suggest a plausible visible light triggered ligand-to-metal charge transfer (LMCT)/1,4-hydrogen atom transfer (HAT) cascade.
Two-dimensional (2D) carbon nitride sheets (CNs) with atomically thin structures are regarded as one of the most promising materials for solar energy conversion. However, due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups, the practical applicability of CNs in photocatalysis is limited. In this study, CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing. The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV, increasing their absorption of visible light. Interestingly, the CNs were distorted after annealing, which can differentiate the spatial positions of electrons and holes, enhancing the visible-light absorption efficiency. As a result, when exposed to visible light, the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times. This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.
After a century of standstill, bacteria-based tumor therapy has resurged recently benefiting from the revolution of tumor immunotherapy, which provides unique solutions to tackle the obstacles of traditional tumor treatments. Obligate and facultative anaerobes with active tropism can selectively colonize at tumor sites and suppress tumor growth via different mechanisms, serving as attractive tools for tumor treatment either as a monotherapy or combining with other therapies for synergistic anti-tumor effects. In this critical review, we introduce the recent advances of bacteria-based tumor therapy from the following aspects. First, the general properties of bacteria are reviewed emphasizing on their structural components related to tumor immunotherapy, and the main bacteria that have been used in tumor therapy are listed. Then, the benefits of bacteria for tumor therapy are illustrated, such as tumor targetability, deep penetration, and facile genetic engineering for attenuation, enhanced efficacy, as well as bioimaging. Next, anti-tumor mechanisms of bacteria are summarized, which refer to intrinsic tumoricidal activities, immune activation, bacteria metabolism, and their capability to regulate gut microbiota homeostasis. Moreover, bacteria could act as carriers to deliver various types of therapeutics to achieve combination therapy with improved efficacy. In addition, several challenges for anti-tumor applications of bacteria are discussed regarding the delivery, efficacy and safety issues, and potential solutions are also provided. Finally, the possible improvements and perspectives are discussed in the end, which provide a guideline for the design of advanced bacteria-based tumor therapeutics in the future.
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.
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