Latest ArticlesThe lithium (Li) metal batteries (LMBs) are considered one of the most promising next-generation batteries due to its extremely high theoretical specific capacity. However, there are a couple of issues, e.g., the serious side reactions that occurred at the solid-liquid interface between the electrolyte and Li metal anode, hindering the broad commercialization of LMBs. Thus, a comprehensive understanding of the mechanisms underlying the decomposition of electrolytes is crucial to the design of LMBs. Herein, we utilize density functional theory simulations to explore the decomposition mechanism of electrolytes. The most commonly used ether electrolyte solvents, i.e., 1,2-dimethoxyethane (DME) and 1,3-dioxalane (DOL), based on suitable lithium salts, namely bis(trifluoromethanesulfonyl)imide (LiTFSI), are chosen to model the actual situations. We explicitly demonstrate that an electron-rich environment near the interface accelerates the decomposition of electrolytes. For ether electrolytes, we show that the LiTFSI degradation path is depending on the ratio of DOL to DME. In addition, the solvation structures of lithium-ion undergo a series of transformations upon electrolyte degradation, becoming thermodynamically more favorable and having a higher reduction potential in an electron-rich environment. Our finding provides new insights into the decomposition mechanisms of electrolytes and paves the way for the rational design of high-performance LMBs.
Traditional photosensitizers show limited singlet oxygen generation in hypoxic infection lesions, which greatly suppress their performance in antibacterial therapy. Meanwhile, there still is lack of feasible design strategy for developing hypoxia-overcoming photosensitizers agents. Herein, radical generation of π-conjugated small molecules is efficiently manipulated by an individual selenium (Se) substituent. With this strategy, the first proof-of-concept study of a Se-anchored oligo (thienyl ethynylene) (OT-Se) with high-performance superoxide radical (O2•−) and hydroxyl radical (•OH) generation capability is present, and achieves efficient antibacterial activities towards the clinically extracted multidrug-resistant bacteria methicillin-resistant S. aureus (MRSA) and carbapenem-resistant E. coli (CREC) at sub-micromolar concentration under a low white light irradiation (30 mW/cm2). The water-dispersible OT-Se shows a good bacteria-anchoring capability, biocompatibility, and complete elimination of multidrug-resistant bacteria wound infection in vivo. This work offers a strategy to boost type-Ⅰ photodynamic therapy (PDT) performance for efficient antibacterial treatments, advancing the development of antibacterial agents.
Second near-infrared (NIR-Ⅱ) light triggered in-situ tumor vaccination (ISTV) represents one of the most promising strategies in boosting the whole-body antitumor immunity. While most of previously developed nano-adjuvants for NIR-Ⅱ-triggered ISTV are “all-in-one” formulations, which may indiscriminately damage both the tumor cells and the immune cells, limiting the overall effect of immune response. To overcome this obstacle, we designed a “cocktail” nano-adjuvant by physically mixing hyaluronidases (HAase)-decorated gold nanostars (HA) for NIR-Ⅱ light triggered in situ production of tumor-associated antigens and CpG functionalized gold nanospheres (CA) for immune cells activation. Compared to “all-in-one” formulation, the “cocktail” nano-adjuvants displayed a significantly stronger immune response on NIR-Ⅱ light induced dendritic cells (DCs) mutation and T cells differentiation, greater effect on tumor-growth inhibition, and higher efficacy in inhibition of pulmonary metastases. What is more, increasing the molar ratio of HA to CA led to an enhanced anticancer immune responses. This study highlight the nano-adjuvant formulation effects on the treatment of tumors with multiple targets.
Early pathogenesis of ischemia-reperfusion (I/R)-induced acute kidney injury (AKI) is dominated by intracellular calcium overload, which induces oxidative stress, intracellular energy metabolism disorder, inflammatory activation, and a series of pathologic cascaded reactions that are closely intertwined with self-amplifying and interactive feedback loops, ultimately resulting in cell damage and kidney failure. Currently, most nanomedicines originate from the perspective of antioxidant stress, which can only quench existing reactive oxide species (ROS) but cannot prevent the continuous production of ROS, resulting in insufficient efficacy. As a safe and promising drug, BAPTA-AM is hydrolyzed into BAPTA by intracellular esterase upon entering cells, which can rapidly chelate with overloaded Ca2+, restoring intracellular calcium homeostasis, thus inhibiting ROS regeneration at the source. Here, we designed a KTP-targeting peptide-modified yolk-shell structure of liposome–poly(ethylene glycol)methyl ether-block-poly (l-lactide-co-glycolic) (mPLGA) hybrid nanoparticles (<100 nm), with the characteristics of high encapsulation rate, high colloid stability, facile modification, and prolonged blood circulation time. Once the BA/mPLGA@Lipo-KTP was targeted to the site of kidney injury, the cholesteryl hemisuccinate (CHEMS) in the phospholipid bilayer, as an acidic cholesterol ester, was protonated in the simulated inflammatory slightly acidic environment (pH 6.5), causing the liposomes to rupture and release the BA/mPLGA nanoparticles, which were then depolymerized by intracellular esterase. The BAPTA-AM was diffused and hydrolyzed to produce BAPTA, which can rapidly cut off the malignant loop of calcium overload/ROS generation at its source, blocking the endoplasmic reticulum (ER) apoptosis pathway (ATF4–CHOP–Bax/Bcl-2, Casp-12–Casp-3) and the inflammatory pathway (TNF-α–NF-κB–IL-6 axes), thus alleviating pathological changes in kidney tissue, thereby inhibiting the expression of renal tubular marker kidney injury molecule 1 (Kim-1) (reduced by 82.9%) and also exhibiting prominent anti-apoptotic capability (TUNEL-positive ratio decreased from 40.2% to 8.3%), significantly restoring renal function. Overall, this research holds huge potential in the treatment of I/R injury-related diseases.
Highly efficient catalysts for electrolysis of water are crucial to the development of hydrogen energy which is helpful to carbon neutralization. Recently, high temperature shock (HTS), with advantage of rapid speed, universality and scalable production, has been a promising method in synthesis of nanomaterials. In this paper, HST was used to treat low Pt loading Mo6S8 for enhanced water splitting performance. Impressively, the optimized MoS2/MoO2/Mo6S8 nano-composite with low Pt mass loading (~4%) displays well hydrogen evolution reaction (HER) electrochemical performance. The overpotential is 124 mV to reach 10 mA/cm2 and the corresponding Tafel slope is 88 mV/dec in acidic electrolyte. Its mass activity is 6.2 mA/µgPt at -124 mV vs. RHE, which is almost 2 times relative to 20% Pt/C. Moreover, it presents distinguished stability even after 2000 cycles. This work will broaden the way of catalysts preparation and the application of hydrogen evolution.
Fungal symbionts co-evolve with hosts and microbial co-inhabitants to acquire an unpredictable potential for producing novel bioactive metabolites, but the knowledge about the topic remains patchy and superficial. Here we present the chemical characterization of acatulides A−G (1−7) as architecturally unprecedented macrolides from the solid-state culture of Acaulium album H-JQSF, an arthropod-associated fungus. The acatulide structures were elucidated by spectroscopic analysis, modified Mosher's method and single-crystal X-ray diffraction. The plausible biosynthetic pathways for compounds 1−4 are proposed. Interestingly, acatulides B−D (2−4) and G (7) were demonstrated to be neuroprotective against the 1-methyl-4-phenylpyridinium (MPP+)-induced damage to SH-SY5Y cells and nematode Caenorhabditis elegans (C. elegans).
In order to solve the contradiction between the rapidly growing energy demand and the excessive exploitation of fossil fuels, it is urgent to research and develops more environmentally friendly and efficient energy storage technologies. Therefore, the development of high-performance cathode materials to enhance the energy density of SIB is currently one of the most important topics of scientific research. Advanced high-voltage and low-cost cathode material for SIBs, a composite of carbon-coated Na4MnCr(PO4)3 (NASICON-type), polyvinylpyrrolidone (PVP), and modified carbon nanotubes (CNTs) is prepared by sol-gel and freeze-drying method. Due to the high conductivity of CNTs, the conductivity of the composite is significantly improved, and its initial capacity is increased to 114 mAh/g at 0.5 C and 96 mAh/g at 5 C (Mn2+/Mn4+ conversion for voltage windows 1.4-4.3 V). Moreover, the multi-electrons transfer of Cr3+/Cr4+ and Mn2+/Mn4+ can provide a high capacity of 165 mAh/g at 0.1 C and 102 mAh/g at 5 C in the high voltage window of 1.4-4.6 V. Furthermore, PVP can effectively inhibit the Jahn-Teller effect caused by Mn ion, making the composite have more excellent high-rate performance and stability. In addition, GITT, EIS and CV curves were drawn to better reveal the excellent kinetic properties of Na4MnCr(PO4)3@C@PVP@CNT cathode, and the mechanism of its performance improvement is deeply studied and discussed. Accordingly, the co-doping of CNTs and PVP is a simple way to high conductivity and fast charging of cathode materials for SIBs.
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.
Electrochemical nitrate reduction reaction (NITRR) is regarded as a “two birds-one stone” method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia, which is retarded by the lack of highly reactive and selective electrocatalysts. Herein, for the first time, nickel foam supported Co4N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced strategy. At the optimal potential, the Co4N/NF catalyst achieves ultra-high Faraday efficiency and NH3 selectivity of 95.4% and 99.4%, respectively. Ex situ X-ray absorption spectroscopy (XAS), together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to ammonia. Theoretical calculations confirm that Co4N with abundant nitrogen vacancies can optimize the adsorption energies of NO3- and intermediates, lower the free energy (ΔG) of the potential-determining step (*NH3 to NH3) and inhibit the formation of N-containing byproducts. In addition, we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen, making H2 quite difficult to produce, and lowering ΔG from *NO to *NOH, which facilitates the selective reduction of nitrate. This study reveals significant insights about the in-situ nonmetal leaching to enhance the NITRR activity.
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.
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