28 research outputs found

    From CdTe Nanoparticles Precoated on Silicon Substrate to Long Nanowires and Nanoribbons: Oriented Attachment Controlled Growth

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    This manuscript describes a simple, environmentally friendly strategy for the rapid and large-scale growth of ultralong nanowires and nanoribbons of wurtzite CdTe. The nanowires and nanoribbons were prepared through the direct hydrothermal treatment of CdTe nanoparticles precoated on ⟨100⟩ Czochralski silicon, which did not involve complicated reactions. The well-crystalline nanowires and nanoribbons were grown along the [102] direction and were up to 100 μm long. The growth of the nanowires and nanoribbons was dominated by the mechanism of oriented attachment, which was clarified through the tracing of the temporal evolution of CdTe nanoparticles coated on the silicon substrate in the process of hydrothermal treatment. Furthermore, the proposed strategy was also effective in the preparation of anisotropic nanostructures of other II−IV group compounds (e.g., ZnO and CdSe)

    Total Synthesis of (+)-Aspidospermidine

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    A facile asymmetric total synthesis of (+)-aspidospermidine has been developed, which is accomplished in 11 steps in an overall yield of 9.6%. Key steps involve a palladium-catalyzed enantioselective decarboxylative allylation to install the quaternary carbon stereocenter and a highly efficient reductive amination–carbonyl reduction–dehydration–intramolecular conjugate addition cascade to build the cis D-ring

    Balancing Pyruvate Node Based on a Dual-Layered Dynamic Regulation System to Improve the Biosynthesis of Caffeic Acid in Candida glycerinogenes

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    Caffeic acid is a phenolic acid compound widely applied in the food and pharmaceutical fields. Currently, one of the reasons for the low yield of caffeic acid biosynthesis is that the carbon flow enters mainly into the TCA cycle via pyruvate, which leads to low concentrations of erythrose 4-phosphate (E4P) and phosphoenolpyruvate (PEP), the precursors of caffeic acid synthesis. Here, we developed a growth-coupled dual-layered dynamic regulation system. This system controls intracellular pyruvate supply in real time by responding to intracellular pyruvate and p-coumaric acid concentrations, autonomously coordinates pathway gene expression, and redirects carbon metabolism to balance cell growth and caffeic acid synthesis. Finally, our constructed engineered strain based on the dual-layered dynamic regulation system achieved a caffeic acid titer of 559.7 mg/L in a 5 L bioreactor. Thus, this study demonstrated the efficiency and potential of this system in boosting the yield of aromatic compounds

    Data_Sheet_1_Development of a co-culture system for green production of caffeic acid from sugarcane bagasse hydrolysate.PDF

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    Caffeic acid (CA) is a phenolic acid compound widely used in pharmaceutical and food applications. However, the efficient synthesis of CA is usually limited by the resources of individual microbial platforms. Here, a cross-kingdom microbial consortium was developed to synthesize CA from sugarcane bagasse hydrolysate using Escherichia coli and Candida glycerinogenes as chassis. In the upstream E. coli module, shikimate accumulation was improved by intensifying the shikimate synthesis pathway and blocking shikimate metabolism to provide precursors for the downstream CA synthesis module. In the downstream C. glycerinogenes module, conversion of p-coumaric acid to CA was improved by increasing the supply of the cytoplasmic cofactor FAD(H2). Further, overexpression of ABC transporter-related genes promoted efflux of CA and enhanced strain resistance to CA, significantly increasing CA titer from 103.8 mg/L to 346.5 mg/L. Subsequently, optimization of the inoculation ratio of strains SA-Ec4 and CA-Cg27 in this cross-kingdom microbial consortium resulted in an increase in CA titer to 871.9 mg/L, which was 151.6% higher compared to the monoculture strain CA-Cg27. Ultimately, 2311.6 and 1943.2 mg/L of CA were obtained by optimization of the co-culture system in a 5 L bioreactor using mixed sugar and sugarcane bagasse hydrolysate, respectively, with 17.2-fold and 14.6-fold enhancement compared to the starting strain. The cross-kingdom microbial consortium developed in this study provides a reference for the production of other aromatic compounds from inexpensive raw materials.</p

    Preparation and Characterization of Bifunctional ZnO/ZnS Nanoribbons Decorated by γ-Fe<sub>2</sub>O<sub>3</sub> Clusters

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    This manuscript presents the preparation and characterization of polycrystalline ZnO/ZnS nanoribbons decorated by γ-Fe2O3 clusters. The weight percentages of ZnO, ZnS, and γ-Fe2O3 in the product were 22.2, 69.3, and 8.5%, respectively. The nanoribbons were synthesized by a two-step, solution-based method. First, porous ZnO/ZnS microspheres were solvothermally prepared. Then, Fe2+and Fe3+ ions were transferred into the microspheres due to their porous property and good adsorption ability. Finally, a mineralizer such as ethylenediamine or aqueous ammonia or urea was introduced into the system to promote the mineralization of Fe2+and Fe3+ ions as well as the transformation of microspheres into nanoribbons. Through tracing the morphology evolution of porous microspheres to nanoribbons by transmission electron microscopy, the growth of the nanoribbons is clarified to be dominated by a dissolution−reconstruction mechanism. The measurements of the optical and magnetic properties revealed that these nanoribbons are bifunctional and have integrated the photoluminescent effect of ZnO and ZnS and the ferromagnetism of γ-Fe2O3

    Metabolic Engineering of Candida glycerinogenes for Sustainable Production of Geraniol

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    Geraniol is a class of natural products that are widely used in the aroma industry due to their unique aroma. Here, to achieve the synthesis of geraniol and alleviate the intense competition from the yeast ergosterol pathway, a transcription factor-mediated ergosterol feedback system was developed in this study to autonomously regulate ergosterol metabolism and redirect carbon flux to geraniol synthesis. In addition, the modification of ergosterol-responsive promoters, the optimization of transcription factor expression intensity, and stepwise metabolic engineering resulted in a geraniol titer of 531.7 mg L–1. For sustainable production of geraniol, we constructed a xylose assimilation pathway in Candida glycerinogenes (C. glycerinogenes). Then, the xylose metabolic capacity was ameliorated and the growth of the engineered strain was rescued by activating the pentose phosphate (PP) pathway. Finally, we obtained 1091.6, 862.4, and 921.8 mg L–1 of geraniol in a 5 L bioreactor by using pure glucose, simulated wheat straw hydrolysates, and simulated sugarcane bagasse hydrolysates, with yields of 47.5, 57.9, and 59.1 mg g–1 DCW, respectively. Our study demonstrated that C. glycerinogenes has the potential to produce geraniol from lignocellulosic biomass, providing a powerful tool for the sustainable synthesis of other valuable monoterpenes

    Experimental and Mathematical Methodology on the Optimization of Bacterial Consortium for the Simultaneous Degradation of Three Nitrogen Heterocyclic Compounds

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    This study aims to establish a systematic method to optimize the bacterial consortium for the simultaneous biodegradation of multixenobiotics in wastewater. Three nitrogen heterocyclic compounds (NHCs), pyridine, quinoline, and carbazole, were chosen as the target compounds with each about 200 mg/L. Different consortia originated from six bacteria for degrading pyridine (<i>Paracoccus</i> sp. BW001 and <i>Shinella zoogloeoides</i> BC026), quinoline (<i>Pseudomonas</i> sp. BW003 and BW004), and carbazole (<i>Pseudomonas</i> sp. BC039 and BC046) were tested for the capacity of NHCs simultaneous degradation. Mathematical methods including dummy-variable-laden kinetic modeling, cubic spline regression and interpolation, and dimensionality reduction were employed to evaluate the complex impacts of cocontaminants and coexisting bacteria on the simultaneous biodegradation, and the most efficient consortium was determined. The influences of cocontaminants on the bacterial degradation activity were far greater than the interactions among the mixed bacteria. Integrating the experimental results and mathematical analysis, consortium M19 (BC026, BW004, BC039, and BC046 with dose rate of 1:1:0.5:0.5) was the best one, which degraded over 95% of pyridine, quinoline, and carbazole simultaneously in 15.4 h. The research methodology in this study could be applied to the optimization of a bacterial consortium which might be used in the bioaugmentation and bioremediation of multixenobiotics removal

    Spatiotemporal Regulation and Transport Engineering for Sustainable Production of Geraniol in Candida glycerinogenes

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    Geraniol is an attractive natural monoterpene with significant industrial and commercial value in the fields of pharmaceuticals, condiments, cosmetics, and bioenergy. The biosynthesis of monoterpenes suffers from the availability of key intermediates and enzyme-to-substrate accessibility. Here, we addressed these challenges in Candida glycerinogenes by a plasma membrane-anchoring strategy and achieved sustainable biosynthesis of geraniol using bagasse hydrolysate as substrate. On this basis, a remarkable 2.4-fold improvement in geraniol titer was achieved by combining spatial and temporal modulation strategies. In addition, enhanced geraniol transport and modulation of membrane lipid-associated metabolism effectively promoted the exocytosis of toxic monoterpenes, significantly improved the resistance of the engineered strain to monoterpenes and improved the growth of the strains, resulting in geraniol yield up to 1207.4 mg L–1 at shake flask level. Finally, 1835.2 mg L–1 geraniol was obtained in a 5 L bioreactor using undetoxified bagasse hydrolysate. Overall, our study has provided valuable insights into the plasma membrane engineering of C. glycerinogenes for the sustainable and green production of valuable compounds

    Solution-Based Doping of Manganese into Colloidal ZnO Nanorods

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    This manuscript describes the low-temperature, solution-based doping of Mn2+ ions into colloidal ZnO nanorods, and the yield of the products is in a gram scale. The structures and chemical compositions of the products were characterized by XRD, XPS, EDS, and FT-IR spectroscopy. The results demonstrate that Mn2+ ions were successfully incorporated into the lattice position of Zn2+ ions in ZnO. The concentration of Mn2+ ions (in molar %) in the products can be controlled in the range of 1.25∼5%. The surfaces of Mn-doped ZnO nanocrystals have very rich hydroxyl groups, which enhance their solubility in many polar and nonpolar solvents. TEM and FESEM were used to characterize the morphology of ZnO and Mn-doped ZnO nanocrystals, and they revealed that both the undoped and doped ZnO nanocrystals are composed of uniform nanorods with a diameter of 8 nm and a length of 95 nm. The doping of Mn2+ ions has significant influences on the optical properties of ZnO nanorods. UV−vis absorption spectroscopy measurements reveal that the doping of Mn2+ lead to a red shift of the absorption edge of ZnO nanorods. Undoped ZnO nanorods exhibit a pure excitonic emission centered at 384 nm, whereas Mn-doped ZnO nanorods only show a red emission that is assigned to the Mn2+ 4T(G) ligand-field excited state

    Production of Caffeic Acid with Co-fermentation of Xylose and Glucose by Multi-modular Engineering in Candida glycerinogenes

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    Caffeic acid (CA), a natural phenolic compound, has important medicinal value and market potential. In this study, we report a metabolic engineering strategy for the biosynthesis of CA in Candida glycerinogenes using xylose and glucose. The availability of precursors was increased by optimization of the shikimate (SA) pathway and the aromatic amino acid pathway. Subsequently, the carbon flux into the SA pathway was maximized by introducing a xylose metabolic pathway and optimizing the xylose assimilation pathway. Eventually, a high yielding strain CG19 was obtained, which reached a yield of 4.61 mg/g CA from mixed sugar, which was 1.2-fold higher than that of glucose. The CA titer in the 5 L bioreactor reached 431.45 mg/L with a yield of 8.63 mg/g of mixed sugar. These promising results demonstrate the great advantages of mixed sugar over glucose for high-yield production of CA. This is the first report to produce CA in C. glycerinogenes with xylose and glucose as carbon sources, which developed a promising strategy for the efficient production of high-value aromatic compounds
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