Latest ArticlesImmune 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.
Native amino-directed palladium-catalyzed C(sp3)–H activation/functionalization has been developed for modification of α-amino acids and peptides. Herein a palladium(Ⅱ)-catalyzed C(sp2)–H arylation of α-amino-β-aryl esters has been disclosed, using the native amino as the directing group. A variety of chiral α-amino-β-aryl esters can be functionalized to give the corresponding ortho-substituted mono- and di-arylated products.
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.
Patients with epidermal growth factor receptor (EGFR) wild-type non-small cell lung cancer (NSCLC) often show primary resistance to gefitinib therapy. It is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of tumors. Herein, we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry (sDMH-scMS) by integrating living-cell electrolaunching ionization MS (ILCEI-MS) and high-performance liquid chromatography-MS (HPLC-MS) analysis, and the primary resistance of NSCLC cells to gefitinib was studied using this platform. The ILCEI-MS analysis showed that approximately 11.9% of NSCLC single cells contained the gefitinib metabolite M11; HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single cells. The intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells, and the intensity of gefitinib metabolites was significantly higher than in PC9 cells, suggesting that the primary resistance of NSCLC cells is related to gefitinib metabolism. Moreover, the combination of gefitinib and the drug-metabolizing enzyme inhibitor α-naphthoflavone was shown to overcome the primary resistance of the NSCLC cells. Overall, the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.
Rechargeable alkaline aqueous zinc batteries (RAZBs) have attracted increasing attention. However, most RAZBs are hindered by the limited availability of cathode materials. The practical electrochemical performance of most cathode materials is lower than the theoretical value due to their poor electrical conductivity and low utilization capacity. In this work, we develop a facile hydrothermal procedure to prepare highly uniform bimetallic sulfides as novel cathode materials for RAZBs. Copper-cobalt binary metallic oxides materials possess higher conductivity and larger capacity compared with their mono-metal oxides compounds due to bimetallic synergistic effects and multiple oxidation states. Furthermore, bimetallic sulfide compounds have smaller bond energy and longer bond length than their oxides, leading to less structural damage, faster kinetics of electrochemical reactions, and better stability. The as-prepared Co-Cu bimetallic sulfides show enhanced electrochemical performance due to various valences of Co and Cu as well as the existence of S. As a result, aqueous Zn/CuCo2S4 battery shows a high specific capacity of 117.4 mAh/g at 4 A/g and a good cycle life of over 8000 cycles. Based on PANa hydrogel electrolytes, a flexible Zn/CuCo2S4 battery demonstrates excellent cycling stability. This battery can also meet the requirements of electronic devices with different shapes and performs well in extreme environments, such as freezing, drilling, and hammering. This work opens new avenues to obtain high-rate and long-life cathode materials for RAZBs by utilizing the synergistic effects of bimetallic sulfides and provides a new platform for flexible energy storage devices.
Rapid analysis of metal ions and organic compounds in strong acidic solutions is of sustainable interest in multiple disciplines. However, complicated and time-consuming pretreatments are always required for MS analysis of the compounds in strong acidic solutions. Otherwise, it will result in a weak signal and cause serious damage to the mass spectrometer. Herein, a simple method inherited from nano-ESI MS was developed for rapid analysis of strong acidic solutions. Nanoliter (nL) strong acidic solution was first loaded in the nano-ESI emitter, followed by evaporation to remove the H+ and leave the analytes on the wall of the nano-ESI emitter. The evaporation process can be completed within 1 min because of the extremely tiny volume (≤1 nL) of the loaded solution. Then, the dried analytes on the wall of the nano-ESI emitter were redissolved by loading a new solvent, followed by nano-ESI MS analysis. By using this method, metal ions and organic compounds in the strong acidic solution can be detected with low sample consumption (1 nL), high speed (< 2 min/sample), high sensitivity (limit of detection = 0.2 µg/L), and high accuracy (> 90%). Proof-of-concept applications of the present method have been successfully achieved for the analysis of gastric juice (pH of the sample = 1), monitoring reaction catalyzed by strong acid (pH of the system = 0), and micro-area analysis of ores (pH of the extraction solvent = 0), showing great application potential in multiple fields.
Partial substitution of polyoxometalate (POM) is an efficient route to modulate the catalytic property of maternal POM. In this work, a new Keggin type POM involving {Ni6} cluster, {[Ni(H2O)2(Dach)2][Ni(Dach)2]2}{[Ni6Cl(μ-OH)3(H2O)(Dach)3(WO4)(PW9O34)][Ni6(μ-OH)3(H2O)2(Dach)3(WO4)(PW9O34)]}Cl·27H2O, (1, Dach = 1,2-diaminocyclohexane) was synthesized. Compounds 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene (AOB) in water. The apparently different results from that with the matrix {PW9O34} ({PW9}) suggest the successful regulation of the catalytic property of {PW9} by the introduction of the {Ni6} cluster into the skeleton. The experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites, which are respectively responsible for the oxidation and condensation steps in the production of AOB. The good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites, respectively.
We report a facile template-free fabrication of heterostructured Co3O4/CuO hollow nanospheres using pre-synthesized Co/Cu-glycerate as conformal precursor. The introduction of copper nitrate in the solvothermal reaction system of glycerol/isopropanol/cobalt nitrate readily induces the conversion from solid Co-glycerate to hollow Co/Cu-glycerate nanospheres, and the effect of the Co/Cu atomic ratio on the structure evolution of the metal glycerates as well as their corresponding oxides were investigated. When examined as anode materials for lithium-ion batteries, the well-defined Co3O4/CuO hollow nanospheres with Co/Cu molar ratio of 2.0 demonstrate excellent lithium storage performance, delivering a high reversible capacity of 930 mAh/g after 300 cycles at a current density of 0.5 A/g and a stable capacity of 650 mAh/g after 500 cycles even at a higher current density of 2.0 A/g, which are much better than their counterparts of bare CuO and Co3O4. The enhanced lithium storage performance can be attributed to the synergistic effect of the CuO and Co3O4 heterostructure with hollow spherical morphology, which greatly enhances the charge/electrolyte transfer and effectively buffers the volume changes upon lithiation/delithiation cycling.
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.
Due to its simplicity, high efficiency, and chemo-selectivity, bioorthogonal chemistry has shown a great application potential in pre-targeting. Currently, four bioorthogonal pairs as targeting tools, including (strept)avidin/biotin, antibody/antigen, oligonucleotide hybridization and IEDDA tools, have been developed and applied in targeted delivery. Nevertheless, all of these tools still suffer from some limitations, such as difficult modification, biochemical fragility and larger molecular weight for biological association tools, as well as chemical instability for IEDDA tools. Synthetic host-guest pairs with relatively small molecular sizes not only possess strong chemical stability, but also have the features of fast conjugation rate, tunable binding affinity, easy modification, and high chemo-selectivity. Consequently, they can be used as a novel non-covalent bioorthogonal tool for pre-targeting. In order to further promote the development of host-guest pairs as novel bioorthogonal tools for pre-targeted delivery, we firstly calculate their conversion rate to make researcher aware of their unique advantages; next, we summarize the recent research progress in this area. The future perspectives and limitations of these unique tools will be discussed. This review will provide a systemic overview of the development of synthetic host-guest pairs as novel bioorthogonal tools for pre-targeting, and may serve as a "go for" resort for researchers who are interested in searching for new synthetic tools to improve pre-targeting.
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