Latest ArticlesThe biosecurity hazards caused by pathogenic fungus have been widely concerned. Given the long-term coexistence of eukaryotic pathogens and quorum sensing bacteria in different habitats in environments, we hypothesized that they have social interactions via signal molecules. In this work, we firstly discovered the well-known bacterial signal molecules play an adverse role in the cell morphology and metabolism in a model pathogen Trichosporon asahii. N-Tetradecanoyl-L-homoserine lactone (C14-HSL) was discovered to increase pathogen hazards of T. asahii, which limited mycelium by 52%, but enhanced cell aggregation by 93%. Higher fluorescence intensity of tryptophan (59%) and aromatic protein (2-fold) contents after the treatment of C14-HSL, indicating that aromatic proteins helped aggregate Trichosporon and showed hydrophobicity. Transcriptome analysis revealed that C14-HSL upregulated the shikimate pathway (above 1-fold) located in downstream of tricarboxylic acid cycle, which contributed to the synthesis of more aromatic proteins and the formation of larger flocs. The limited mycelial growth of T. asahii attributed to the up-regulated expressions of cell cycle process. The fungal transboundary response to bacterial C14-HSL was controlled by signal transduction pathways. This study provides new insights into the co-evolution of bacterial and pathogenic fungi in microecosystems.
The exploration of advanced materials through rational structure/phase design is the key to develop high-performance lithium-ion capacitors (LICs). However, high complexity of material preparation and difficulty in quantity production largely hinder the further development. Herein, Cu5FeS4-x/C (CFS@C) heterojunction with rich sulfur vacancies has successfully achieved from natural bornite, presenting low cost-effective and bulk-production prospect. Density functional theory (DFT) calculations indicate that rich vacancies in bulk phase can decrease band gap of bornite and thus improve its intrinsic electron conductivity, as well as the heterojunction spontaneously evokes a built-in electric field between its interfacial region, largely reducing the migration barrier from 1.27 eV to 0.75 eV. Benefited from these merits, the CFS@C electrodes deliver outperformed lithium storage performance, e.g., high reversible capacity (822.4 mAh/g at 0.1 A/g), excellent cycling stability (up to 820 cycles at 2 A/g and 540 cycles at 5 A/g with respective capacity retention of over or nearly 100%). With CFS@C as anode and porous carbon nanosheets (PCS) as cathode, the assembled CFS@C//PCS LIC full cells exhibit high energy/power density characteristics of 139.2 Wh/kg at 2500 W/kg. This work is expected to offer significant insights into structure modifications/devising toward natural minerals for advanced energy-storage systems.
With the deep integration of electrochemical research with energy, environment, catalysis, and other fields, more and more new electrochemical catalytic reactions have entered our research field. Alloy catalysts have recently emerged as a new type of nanomaterial due to the rapid development of kinetic controlled synthesis technology. These materials offer several advantages over monometallic catalysts, including larger element combinations, complex geometries, bifunctional sites, and reduced use of precious metals. This paper provides a review of alloy electrocatalysts that are designed and prepared specifically for electrocatalytic applications. The use of alloy materials in electrocatalyst design is also discussed, highlighting their widespread application in this field. First, various synthesis methods and synthesis mechanisms are systematically summarized. Following that, by correlating the properties of materials with the structure, relevant strategies toward advanced alloy electrocatalysts including composition regulation, size, morphology, surface engineering, defect engineering, interface engineering and strain engineering are classified. In addition, the important electrocatalytic applications and mechanisms of alloy electrocatalysts are described and summarized. Finally, the current challenges and prospects regarding the development of alloy nanomaterials are proposed. This review serves as a springboard from a fundamental understanding of alloy structural dynamics to design and various applications of electrocatalysts, particularly in energy and environmental sustainability.
As a type of new carbon-based nanomaterials, carbon dots (CDs) possess exceptional optical properties, making them highly desirable for use in fluorescent sensors. However, the CDs with deep-red (DR) or near-infrared (NIR) emission have rarely been reported. In this work, we prepared deep-red emissive fluorine-doped carbon quantum dots (F-CDs) by introducing a precursor simultaneously containing fluorine and amidogen. The synergistic effect of nitrogen doping and D-π-A pattern production contributed to the maximum emission of F-CDs at 636 nm with an absolute quantum yield of 36.00% ± 0.68%. Moreover, we designed an F-CDs-based fluorescence assay to determine the content of hypochlorite (ClO−), with a limit of detection (LOD) as low as 15.4 nmol/L, indicating the high sensitivity of F-CDs to ClO−. In real samples, the F-CDs-based fluorescent sensor exhibited excellent sensitivity and selectivity in the detection of ClO−, with an error below 2%, suggesting their great potential in daily life. In cancer cell imaging, the F-CDs not only demonstrated high sensitivity to ClO− but also exhibited excellent mitochondria targeting, as evidenced by the high Pearson's correlation coefficient (PCC) of 0.93 in colocalization analysis. The work presented here suggests the great potential of replacing commercial dyes with F-CDs for highly specific mitochondria labeling and cell imaging.
Exploring the therapeutic effect of single atom catalysts beyond reactive oxygen species (ROS) modulation would boost the prosperity of nanomedicine in cancer treatment. Autophagy as a vital therapy target offers new options for the control of renal cell carcinoma (RCC) progression. Herein, Fe single atom-decorated graphene oxide (Fe1-GO) nanosheet is developed to be a feasible autophagy inducer in RCC treatment. With the well-dispersed O−Fe1−O active sites, Fe1-GO kills ACHN cells effectively but maintains acceptable cytotoxicity to the normal podocyte and HK2 ones. In-depth analyses ascribe the inhibition of ACHN cells to the upregulated autophagy instead of the commonly known catalytic ROS generation. The in vivo therapeutic effect of Fe1-GO nanomedicine is also validated by the RCC-bearing BALB/c mice model, realizing an 89% reduction of tumor weight and good biosafety. This work provides new insights into the design of autophagy regulators as well as potential therapeutic strategies for RCC treatment.
C-Oligosaccharides are rare in nature and possess diverse bioactivities. However, their chemical synthesis faces many challenges. In this work, enzymatic introduction of C-linked sugar chains to target aglycones was successfully achieved by multi-enzymatic cascade reactions. A C-glycosyltransferase from Aloe barbadensis was employed to introduce the first C-linked glucose and then a cyclomaltodextrin glucanotransferase from Bacillus licheniformis was used to extend the sugar chain. A total of twenty C-oligosaccharides with 2–6 sugars were synthesized from scale-up reactions and exhibited good water solubility and sodium-dependent glucose transporter 2 (SGLT2) inhibitory activity. Furthermore, a glucoamylase was used to control the length of the sugar chain and the C-maltosides were efficiently synthesized. These findings not only expanded the structural diversity of C-oligosaccharides, but also provided a strategy for the modification of C-glycoside drugs to improve the druggability.
Lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility, large atomic number, and long carrier lifetime, but the toxicity of lead is regarded as the major factor hindering their development. Here, we introduce organic molecule (R)-(-)-2-methylpiperazine (R-MPz) into the bismuth-based structure to synthesize lead-free (R)-(H2MPz)BiI5 (R-MBI). The high-quality centimeter-sized single crystals have been obtained, which show a low dark current and superior environmental stability. Particularly, the single-crystal device of R-MBI exhibits a high μτ product up to 1.88 × 10−4 cm2/V and a low trap density of 1.21 × 1010 cm−3. Further, the detector displays excellent detection sensitivity of 263.58 µC Gyair−1 cm−2 and a favorable low detection limit of 4.35 µGyair/s, both of which meet the requirement for medical diagnostics. These findings shed light on the exploration of innovative bismuth-based hybrid perovskites for high-performance X-ray detection.
Corrosion of reinforcement induced by chloride invasion is extensively considered as the dominating deterioration mechanism of reinforced concrete (RC) structures, leading to serious safety hazards and tremendous economic losses. However, it still lacks well dispersive and cost-efficient nanomaterials to improve the anti-chloride-corrosion ability of RC structures. Herein, specific carbon dots (CDs) with high dispersity and low cost are deliberately designed, successfully prepared by hydrothermal processing, and then firstly applied to immensely enhance chloride binding performance of cement, thereby contributing to suppressing the corrosion of reinforcement. Specifically, the tailored CDs are composed of the carbon core with highly crystalline sp2 C structures and oxygen-containing groups connecting on the carbon core; The typical equilibrium test confirms that with respect to that of the blank cement paste, the chloride binding capacity of cement paste involving 0.2 wt% (by weight of cement) CDs is increased by 109% after 14-day exposure to 3 mol/L NaCl solution; according to comprehensive analyses of phase compositions, the chloride binding mechanism of CDs-modified cement is rationally attributed to the fact that the incorporation of CDs advances the formation of calcium silicate hydrate (C–S–H) gels and Friedel's salt (Fs), thus enormously enhancing the physically adsorbed and chemically bound chloride ions of cement pastes. This work not only firstly provides a novel high-dispersity and low-cost nanomaterial toward the durability enhancement of RC structures, but also broadens the application of CDs in the field of engineering, conducing to stimulating their industrialization development.
Heterogeneous reaction of mineral aerosols and atmospheric polluting gases play an important role in atmospheric chemistry. In this study, the reactions of NO2 with or without SO2 mixture gas on the surface of α-Fe2O3 particles under dry conditions were studied. The effects of sodium dodecyl sulfate (SDS) and the heterogeneous reaction under both dark and UV irradiation conditions were investigated. The infrared spectrum analyzed by the two-dimensional correlation spectroscopy (2D-COS) was used to obtain the products formation sequences. The results showed that UV irradiation can promote the production of nitrate. The 2D-COS analysis indicated SDS changed the sequence order of nitrate and nitrite species during reactions. In oxidation conditions, the final product of heterogeneous reaction of NO2 and α-Fe2O3 was monodentate nitrate. Only the heterogenous reaction of NO2 and α-Fe2O3 containing SDS (FOS) without UV light, the final product was bidentate nitrate. SDS was the catalysis agent supply and photoresist to the system. With surface active compounds, the environmental lifetime of heterogeneous reactions between trace gases and aerosols extends. Surfactants, ultraviolet light, and the types of gases involved in the reaction all have complex effects on the aerosol aging process. This study provided a reference for subsequent heterogeneous reaction studies and the formation of aerosols.
The combination of horseradish peroxidase (HRP) and a fluorescence substrate has been attracting great interests in developing sensitive biochemical analysis and immunoassays. 10-Acetyl-3,7-dihydroxyphenoxazine (ADHP or Amplex red) is the most sensitive fluorogenic substrate known for HRP in current market, however, it suffers from some drawbacks, such as non-specific reactivity to carboxylesterase and limited fluorescence stability. In the present study, a novel HRP substrate 10-cyclopropylcarbonyl-dichloro-dihydroxyphenoxazine (AR-2), has been prepared, which exhibited improved sensitivity than ADHP in sensing HRP. Moreover, the fluorescence of AR-2/HRP demonstrated improved tolerance to physiological relevant pH fluctuation as compared to ADHP/HRP. Successful detection of uric acid/urate oxidase reaction indicated excellent application prospect of AR-2/HRP for monitoring H2O2-generating biochemical reactions. More interestingly, an enzyme-linked immunosorbent assay (ELISA) using AR-2 as the fluorescence reporter has been successfully used in detecting IgG against severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) from human serum samples. Overall, AR-2 exhibits improved performances over the commercial ADHP, which will be an ideal alternative to ADHP in HRP-based fluorescence biochemical analysis and immunoassays.