Latest ArticlesMetastatic breast cancer (MBC) is one of the most common and knotty diseases in female population which could place them in a life-threatening condition. For malignant proliferation and migration, cancer cells require a large amount of glucose and energy to meet the demand of rapid metabolism. Hence, efficiently diminishing the utilization of energy substances by cancer cells is emerging as validated therapeutic strategies for cancer therapy. Herein, a nanoplatform with dual-inhibition of glucose uptake and oxidative phosphorylation (OXPHOS) was designed, which consisted of albendazole (ABZ) and atovaquone (ATO) by simple carrier-free self-assembling. The introduction of ABZ could evidently decrease glucose uptake to reduce the main "energy fuel" of cancer cells. Meanwhile, as a blocker of OXPHOS, ATO would reduce adenosine triphosphate (ATP) production and ameliorate hypoxia microenvironment by suppressing mitochondrial respiratory chain. Under such dual inhibition of energy metabolism, AA NPs exerted synergistic energy exhaustion effect and outstanding hypoxia improvement function, efficiently inhibiting tumor growth and metastasis. This research not only illustrates the feasibility of energy metabolism therapy by co-inhibiting glucose uptake and OXPHOS, but also provides an ingenious tactic to diminish metastasis during MBC treatment
The conversion of propargylic alcohols and carbon dioxide (CO2) into fine chemicals suffers from issues of harsh reaction conditions and difficult catalyst recovery. To achieve efficient CO2 activation at low energy consumption, a silver-anchored porous aromatic framework catalyst Ag@PAF-DAB with high active phase density and CO2 adsorption capacity was proposed. Since Ag@PAF-DAB has the dual functions of CO2 capture and conversion, propargylic alcohols were completely converted into α-alkylidene cyclic carbonate or α‑hydroxy ketone as high value-added product under atmospheric pressure (CO2, 0.1 MPa) and low silver equivalent (0.5 mol%). Notably, Ag@PAF-DAB exhibited broad substrate diversity, high stability, and excellent reusability. By applying FTIR and GC, the key to green synthetic route of α‑hydroxy ketone was confirmed to lie in the further hydration of α-alkylidene cyclic carbonate.
Caproate, produced by microbial chain elongation process, is potential to replace the diversified fossil-based products, contributing to carbon neutrality. However, its production performance is far from industrial application, so the cost-effective enhancement measures are highly needed. This study confirmed powdered activated carbon (PAC) has a significant effect on enhancing caproate production performance. The production, yield, and selectivity of caproate were improved by more than 1-fold by the optimized PAC dosage of 15 g/L, comparing with control. Mechanism investigation from a new visual angle showed that PAC accelerated ethanol oxidation to generate acetyl-CoA, and simultaneously boosted the efficiency of reverse β oxidation (RBO) by promoting the timely reaction of butyrate and acetyl-CoA to synthesis caproate. The addition of PAC also shifted the microbial community by enriching more caproate-producing bacteria but eliminating irrelevant ones. Furthermore, metagenomic analysis revealed that PAC effectively up-regulated the functional genes encoding key enzymes responsible for ethanol oxidation and RBO pathway, which was the root cause for the improved caproate production. This study presented the intrinsic insights into the mechanism of PAC promoting caproate generation, laying a foundation to the scale production of caproate.
A label-free lactic acid sensor has been successfully developed by using a Dysprosium single crystal-based photoelectric potential technique via Dy-SCN/FTO electrode. Interestingly, the proposed sensor demonstrated excellent performance for L-lactic acid analysis with a wide linear range of 0.0196~16.31 mmol/L, the detection limit of as low as 3.20 µmol/L as well as an advisable stability. The feasibility of this strategy was also verified by practical application towards human sweat samples. The mechanism studies indicated that lactic acid molecules specifically bind to the surface of semiconductor materials, which alters the charge distribution of the electrode surface and subsequently results in band bending/photoelectric potential changes. The theoretical formula for this photoelectric chemistry (PEC) strategy was then derived according to charge balance theory. We believe that the proposed Dy-SCN/FTO sensor would open a new way for rapid, non-invasive L-lactic acid level evaluation during human physical condition monitoring.
In this paper, cucurbit[7]uril (CB[7])-mediated three-dimensional gold nanoassemblies were successfully prepared to increase the loaded amount of CB[7] and enhance the electrochemical detection of amino acids. Particle sizes of gold nanoparticles (AuNPs) significantly affect stability and detection sensitivity of nanoassemblies. The volume of gold nanoassemblies first increased and then decreased with the increase of CB[7] concentration. The 3D gold nanoassemblies composed of 16 nm AuNPs and 100 µmol/L CB[7] had excellent stability and maximum volume, exhibiting more sensitive detection for a variety of amino acids. And the detection limits of aromatic amino acids are lower in virtue of the higher binding constant between aromatic amino acids and CB[7]. This study will develop and deepen our understanding of molecular recognition in amino acids detection.
A highly efficient asymmetric (3 + 2) cycloaddition of α-diazo pyrazoleamides with silyl enol ethers was realized by employing a chiral N, N'-dioxide-Ni(Ⅱ) complex catalyst. The process includes the formation of chiral nickel carbenoid intermediate and the following enantioselective cycloaddition reaction. The desired dihydrofuran O, O-acetal derivatives were obtained in good yields (up to 90%) with high enantioselectivity (up to 99% ee) under mild reaction conditions within short reaction time. On the basis of the determination of the catalyst structure, a possible transition state mode was proposed.
Lithium rich layered oxide (LRLO) has been considered as one of the promising cathodes for lithium-ion batteries (LIBs). The high voltage and large capacity of LRLO depend on Li2MnO3 phase. To ameliorate the electrochemical performance of Li2MnO3, also written as Li(Li1/3Mn2/3)O2, we propose a strategy to substitute Mn4+ and Li+ in Mn/Li transition metal layer with Ti4+, which can stabilize the structure of Li2MnO3 by inhibiting the excessive oxidation of O2− above 4.5 V. More significantly, the unequal-valent substitution brings about the emergence of interlayer Li vacancies, which can promote the Li-ion diffusion based on the enlarged interlayer and increase the capacity by activating the Mn3+/4+ redox. We designed Li0.7[Li1/3Mn2/3]0.7Ti0.3O2 with high interlayer Li vacancies, which presents a high capacity (290 mAh/g at 10 mA/g) and stable cycling performance (84% over 60 cycles at 50 mA/g). We predict that this strategy will be helpful to further improve the electrochemical performance of LRLOs.
Chiral glycosyl lactone is an important class of bioactive compound and pharmaceutical intermediate in nature, especially for chiral lactones with 4 carbon atoms, which are very useful building blocks for synthesis of biologically interesting compounds. Herein, a selective dehydrogenation and solvent matched catalytic system under oxygen-free conditions was developed to try to achieve the one-step direct conversion of cyclic hemiacetal sugars toward their chiral glycosyl lactones. During the process, the inherent structural characteristics of sugar was efficiently utilized, and the transfer of its chiral centers was realized. Under the optimum condition, the corresponding lactones were successfully prepared from C4-C6 sugars with cyclic hemiacetal structure in acetonitrile. The reaction mechanism in acetonitrile was explored by the first principle density functional theory calculations and tracking reaction process. It was found that the high lactone yield in acetonitrile was due to the high proportion of α-conformation form among multiple tautomers in it. This selective dehydrogenation process may further extend the possibility of the preparation of chiral synthons from carbohydrates directly.
Erythrocyte membrane (EM)-camouflaged chemotherapeutic delivery nanovehicles hold promise for solid tumor therapy because of their excellent biostability and biocompatibility. However, it is accompanied with insufficient targeting effect and deficient pharmacokinetic behavior due to the lack of a regulated biointerface to navigate and overcome biological transportation obstacles in solid tumor therapy. Herein, an anti-epidermal growth factor receptor (EGFR) aptamer (EApt) modified and EM-cloaked chemotherapeutic nanomissile delivery system was constructed. The anchored-EApt acting as a specific EGFR suppressor promotes to inhibit the overexpression of EGFR and initiate the cell apoptosis. Importantly, the resulting PLGA-DOX@EM-EApt orchestrated the bioactivity of each component and provided synergistic cell apoptosis and antitumor effects by precisely suppressing EGFR expression levels and delivering DOX. The in vitro and in vivo experimental results confirmed that the immune escape and active targeting behaviors of PLGA-DOX@EM-EApt could significantly promote its drug retention and tumor inhibition abilities. Our findings propose a novel strategy using the biointerface functionalization technique, demonstrating a promising therapeutic platform via a biomimetic drug delivery system for precise solid tumor recognition and synergistic therapy.
Staphylococcus aureus wall teichoic acids (WTAs) are attractive targets for antibacterial vaccine development. In this study, three core glycosylated WTA structure, including α-1,4-GlcNAc, β-1,4-GlcNAc and β-1,3-GlcNAc modified ribitol phosphates containing a linker are chemically synthesized and conjugated with tetanus toxin (TT) carrier protein as vaccine candidates. In vivo immunological studies demonstrate that the synthesized glycosylated WTAs display high immunogenicity and all conjugates provoke strong immune responses and elicit high levels of specific IgG antibodies against the GlcNAc-modified WTA. Furthermore, antibodies elicited by the vaccine candidates remain the capability to recognize S. aureus cells and display significant opsonophagocytic activity to clear S. aureus. This study demonstrates that the core structure of glycosylated WTAs are effective antigens for constructing anti-S. aureus vaccines to prevent and control S. aureus infections.
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