ABSTRACT
Continuous fermentation processes increasingly emphasized cell recycling, utilization, and renewal. In this study, to improve the sustainability of the immobilized Saccharomyces cerevisiae, the cells were recovered on the surface of the glucose-responsive supports through manipulating the competitive interactions of phenylboric acid groups between glycoproteins on the cells and glucose. Through a dopamine (DA)-assisted deposition approach, 3-acrylamidophenylboronic acid (APBA) was integrated to design the saccharide-sensitive cotton fibers (APBA@PDA-CF). The optimal co-deposition time (5â¯h) and ratio (1:1) resulted in an impressive immobilization efficiency of 69.64%. Meanwhile, 93.23% of Saccharomyces cerevisiae was captured and harvested on the surface of APBA@PDA-CF with the fermentation course through regulating the competitive interactions of phenylboric acid groups between glycoproteins on the cells and glucose regardless of pH. Notably, a strong interaction between the yeast cells and APBA@PDA-CF was observed at a low glucose concentration (0.1ï½2â¯g/L), with reduced sensitivity at high glucose concentrations (>5â¯g/L). Moreover, the ethanol production and yield could be increased to 25.37â¯g/L and 42.4% in the fifth-batch fermentation, respectively. Therefore, based on the feasible and versatile co-deposition method, this study not only broadened the application scope of APBA, but also explored the broad prospects of smart materials in cell immobilization, recovery and continuous fermentation.
ABSTRACT
Liquid-liquid separation, commonly referred to as oiling-out, frequently can occurs during crystallization, especially the anti-solvent crystallization process of phosphoryl compounds, and poses potential hurdle for high-quality product. Efficiently regulating oiling-out during crystallization remains a significant challenge. Among various techniques, ultrasound emerges as a green and effective approach to enhance the crystallization process. However, there is a dearth of in-depth research exploring the microscopic mechanisms of this process. Therefore, our research focused on the fructose-1,6-diphosphate (FDP), a typical phosphoryl compound, to gain a deeper understanding of how ultrasound influences the oiling-out process. The focused beam reflectance measurement (FBRM) technology was used to investigate the oiling-out phenomenon of FDPNa3 across various solvent ratios. In addition, the influence of ultrasound on the induction time was studied and the nucleation energy barrier was calculated. Finally, to further unravel the microscopic mechanisms, we utilized molecular simulation techniques to analyze the impact of ultrasound power on the dissolution-precipitation process. Our observations revealed a consistent oiling-out process that attainted a stable state regardless of the solvent employed. Notably, the results of the oiling-out induction time experiments indicated that ultrasound significantly reduced helped lower the nucleation energy barrier of FDP3- ions, thereby dismantling FDP3-clusters in solution. Thus, in turn, shortened the reduced induction time and promoted crystallization. Furthermore, ultrasound reduced the interactions between FDP3-ions and water molecules as well as FDP3- ions themselves. As simulated field intensity increased, these interaction forces gradually diminished, the thickness of the hydration layer surrounding the FDP3- clusters facilitating the disruption of clusters, ultimately enhancing the crystallization process.
ABSTRACT
When it comes to enzyme stability and their application in organic solvents, enzyme biocatalysis has emerged as a popular substitute for conventional chemical processes. However, the demand for enzymes exhibiting improved stability remains a persistent challenge. Organic solvents can significantly impacts enzyme properties, thereby limiting their practical application. This study focuses on Lipase Thermomyces lanuginose, through molecular dynamics simulations and experiments, we quantified the effect of different solvent-lipase interfaces on the interfacial activation of lipase. Revealed molecular views of the complex solvation processes through the minimum distance distribution function. Solvent-protein interactions were used to interpret the factors influencing changes in lipase conformation and enzyme activity. We found that water content is crucial for enzyme stability, and the optimum water content for lipase activity was 35 % in the presence of benzene-water interface, which is closely related to the increase of its interfacial activation angle from 78° to 102°. Methanol induces interfacial activation in addition to significant competitive inhibition and denaturation at low water content. Our findings shed light on the importance of understanding solvent effects on enzyme function and provide practical insights for enzyme engineering and optimization in various solvent-lipase interfaces.
Subject(s)
Enzyme Stability , Lipase , Molecular Dynamics Simulation , Solvents , Water , Water/chemistry , Solvents/chemistry , Lipase/chemistry , Lipase/metabolism , Protein Conformation , EurotialesABSTRACT
Vanadium dioxide (VO2) has received widespread attention for application in energy-efficient smart windows because of its distinct thermochromic property in the near-infrared region during the reversible metal-insulator phase transition. In this study, lepidocrocite VOOH ultrafine nanoparticles (NPs) with a diameter less than 30 nm were prepared by a mild and efficient hydrothermal method, and the Kirkendall effect played a vital role in the growth of the VOOH NPs. It was found that VOOH could be transformed into VO2via a subsequent annealing treatment during which the size and morphology of VOOH are well preserved even though the annealing temperature is up to 500 °C. The ultrafine VO2 NPs are crucial for achieving excellent nanothermochromic performance with a luminous transmittance (Tlum) up to 56.45% and solar modulation ability (ΔTsol) up to 14.95%. The environmental durability is well improved by coating VO2 NPs with an SiO2 shell as confirmed via progressive oxidation and acid corrosion experiments. Meanwhile, the Tlum of the VO2@SiO2 film is further increased from 56.45% to 62.29% while the ΔTsol remained unchanged. This integrated thermochromic performance presents great potential for the development of VO2-based smart windows.
ABSTRACT
Almost all reported salts of nucleotides crystallized from solutions are in the form of hydrate. Layered hydrates often occur in crystals with more than five water molecules per host molecule. In the present report, five single-crystal structures of uridine-5'-monophosphate (UMP) series hydrates of acid or salts (UMPNa x ·yH2O, x = 0-2) were determined and analysed. It was found that all crystal hydrates were orthorhombic with a C2221 space group but with mere variation in the plane angle of adjacent bases and the distance between phosphate arms. The packing arrangements of UMPNa x ·yH2O hydrates present typical layered sandwich structures and show that the UMP molecular layers alternate with water molecular layers parallel to the ac plane, linked by hydrogen bonds or coupled with coordinate bonds besides ionic electrostatic interaction. Metal ions were located in water molecular layers as a form of hydration. In addition, we tried to deduce and give insights into the formation of UMPNa x ·yH2O hydrates. The effect of water molecules and metal ions on the crystal structure and stability was investigated. It was found that the coexistence of relatively rigid architectures constructed by host molecules and flexible interlayer regions was a key factor to the formation of these hydrates. Excessive loss of lattice water would give rise to the irreversible collapse of the host structure and loss of ability to recover to the initial state under humidity. Approximately seven crystal-water molecules were the balance point of sodium salt hydrates at room temperature under 43-76% RH conditions. The number of sodium ions in the crystal lattice is positively correlated with their thermal stability.
ABSTRACT
A new fluorescence probe L, which featured with a large Stokes shift (216â¯nm), was designed for sensitive detection of cysteine (Cys) and a potential sensing mechanism derived from excited state intramolecular proton transfer (ESIPT) was proposed. More importantly, probe L exhibits higher selective to Cys than other amino acid due to its specific cyclization between acrylate group and Cys. Meanwhile, the probe L shows a low detection limit of 8.82â¯×â¯10-8 M, which is enough for detecting Cys in organisms. Furthermore, this probe displays high biocompatibility and can image Cys in living cells.
Subject(s)
Cysteine , Fluorescent Dyes , Diagnostic Imaging , HeLa Cells , Humans , ProtonsABSTRACT
The photocatalytic efficiency of TiO2 is reduced by rapid electron-hole recombination. An effective approach to address this limitation is to have TiO2 doped with various metal ions or heteroatoms. Herein, we prepared a series of Li+-doped TiO2 nanoparticles showing high photocatalytic activities through the sol-gel method. The samples were characterized by X-ray diffraction (XRD) and surface area analyses. Effects of Li+ doping on the Brunauer-Emmett-Teller (BET) surface area, crystallite size, phase transformation temperature, and phase composition were studied. The results showed that Li+ doping can promote the generation of the rutile crystal phase in TiO2, lower the anatase-to-rutile transformation temperature, and generate the mixed-crystal effect. The photocatalytic degradation of methyl orange (MO) was used as a probe reaction to evaluate the photoactivity of the nanoparticles. Parameters affecting the photocatalytic efficiency, including the Li+ doping amount, calcination temperature, and catalyst amount, as well as the kinetics of the photocatalytic process toward the degradation of MO, were investigated. The mixed-crystal TiO2, which was doped with 1.0 mol % Li+ and calcined at 550 °C containing 27.1% rutile and 72.9% anatase phase, showed a 2.2-fold increase in the photoactivity on the basis of the rate constant of MO decomposition as compared with the undoped TiO2. The existence of a definite quantity of rutile phase could effectively inhibit the recombination of the electron-hole pairs, thus promoting photocatalytic activity.
ABSTRACT
The adsorption of quaternary mixtures of ethanol/glycerol/glucose/acetic acid onto a microporous hyper-cross-linked resin HD-01 was studied in fixed beds. A mass transport model based on film solid linear driving force and the competitive Langmuir isotherm equation for the equilibrium relationship was used to develop theoretical fixed bed breakthrough curves. It was observed that the outlet concentration of glucose and glycerol exceeded the inlet concentration (c/c0>1), which is an evidence of competitive adsorption. This phenomenon can be explained by the displacement of glucose and glycerol by ethanol molecules, owing to more intensive interactions with the resin surface. The model proposed was validated using experimental data and can be capable of foresee reasonably the breakthrough curve of specific component under different operating conditions. The results show that HD-01 is a promising adsorbent for recovery of ethanol from the fermentation broth due to its large capacity, high selectivity, and rapid adsorption rate.