"One-Pot" Method Preparation of Dendritic Mesoporous Silica-Loaded Matrine Nanopesticide for Noninvasive Administration Control of Monochamus alternatus: The Vector Insect of Bursapherenchus xylophophilus.

Monochamus alternatus is an important stem-boring pest in forestry. However, the complex living environment of Monochamus alternatus creates a natural barrier to chemical control, resulting in a very limited control effect by traditional insecticidal pesticides. In this study, a stable pesticide dendritic mesoporous silica-loaded matrine nanopesticide (MAT@DMSNs) was designed by encapsulating the plant-derived pesticide matrine (MAT) in dendritic mesoporous silica nanoparticles (DMSNs). The results showed that MAT@DMSNs, sustainable nanobiopesticides with high drug loading capacity (80%) were successfully constructed. The release efficiency of DMSNs at alkaline pH was slightly higher than that at acidic pH, and the cumulative release rate of MAT was about 60% within 25 days. In addition, the study on the toxicity mechanism of MAT@DMSNs showed MAT@DMSNs were more effective than MAT and MAT (0.3% aqueous solutions) in touch and stomach toxicity, which might be closely related to their good dispersibility and permeability. Furthermore, MAT@DMSNs are also involved in water transport in trees, which can further transport the plant-derived insecticides to the target site and improve its insecticidal effect. Meanwhile, in addition, the use of essential oil bark penetrants in combination with MAT@DMSNs effectively avoids the physical damage to pines caused by traditional trunk injections and the development of new pests and diseases induced by the traditional trunk injection method, which provides a new idea for the application of biopesticides in the control of stem-boring pests in forestry.

Expression of a thermostable glucose-stimulated ß-glucosidase from a hot-spring metagenome and its promising application to produce gardenia blue.

This study reports a thermostable glucose-stimulated ß-glucosidase, BglY442, from hot-spring metagenomic data that was cloned and expressed in Escherichia coli BL21 (DE3). The molecular mass of recombinant BglY442 was 69.9 kDa and was used in the production of gardenia blue. The recombinant BglY442 showed its maximum activity at pH 6.0 and 75 °C, maintained 50 % activity at 70 °C for 36 h, presented over 90 % activity in a broad pH range and a wide range of pH stability. Moreover, BglY442 exhibited excellent tolerance toward methanol and ethanol. The specific activity of BglY442 was 235 U/mg at pH 6.0 and 75 °C with 10 mM pNPG as substrate. BglY442 activity increased by over fourfold with 2 M glucose or xylose. Specifically, the enzyme kinetics of BglY442 seem to be non-Michaelis-Menten kinetics or atypical kinetics because the Michaelis-Menten saturation kinetics were not observed with pNPG, oNPG or geniposide as substrates. Under optimum conditions, geniposide was dehydrated by BglY442 and reacted with nine amino acids respectively by the one-pot method. Only the Arg or Met derived pigments showed bright blue, and these two pigments had similar ultraviolet absorption spectra. The OD590 nm of GB was detected to be 1.06 after 24 h with the addition of Arg and 1.61 after 36 h with the addition of Met. The intermediate was elucidated and identified as ginipin. Molecular docking analysis indicated that the enzyme had a similar catalytic mechanism to the reported GH1 Bgls. BglY442 exhibited potential for gardenia blue production by the one-pot method. With outstanding thermostability and glucose tolerance, BglY442 should be considered a potential ß-glucosidase in biotechnology applications.

Room-Temperature, Homogeneous, Single-Step, and Large-Scale Synthesis of Perovskite Nanoplatelets for Blue Light-Emitting Diodes.

Inorganic perovskite nanocrystals (IPNCs) have attracted considerable attention due to their excellent optoelectronic properties. However, problems arise from anion migration during the preparation of a blue light-emitting diode (LED), and only small-scale syntheses have been conducted on a laboratory scale. By using only Br as the anion here, CsPbBr3 was synthesized in the form of nanoplatelets to eliminate the effects of anion migration and to prepare an inorganic perovskite nanoplatelet (IPNPL) emitting blue light. In addition, the synthesis was performed under ambient conditions at room temperature, and the synthetic process was shortened to enable large-scale synthesis. We used a 1 L bottle for large-scale synthesis, and a photoluminescence quantum yield (PLQY) of 78% was observed at 460 nm. We fabricated LEDs by using IPNPLs, and we observed an electroluminescence peak at 461 nm. The developed synthetic method is expected to pave the way for commercialization of IPNCs and the next-generation display market.

Controllable AgNPs encapsulation to construct biocompatible and antibacterial titanium implant.

Silver nanoparticles (AgNPs) are progressively becoming an in-demand material for both medical and life use due to their effective antimicrobial properties. The high surface area-to-volume ratio endows AgNPs with enhanced antibacterial capacity accompanied by inevitable cytotoxicity. Surface coating technique could precisely regulate the particle shape, aggregation, and Ag+ release pattern of AgNPs, by which the cytotoxicity could be significantly reduced. Various coating methods have been explored to shell AgNPs, but it remains a great challenge to precisely control the aggregation state of AgNPs and their shell thickness. Herein, we proposed a simple method to prepare a tunable polydopamine (pDA) coating shell on AgNPs just by tuning the reaction pH and temperature, yet we obtained high antibacterial property and excellent biocompatibility. SEM and TEM revealed that pDA coated AgNPs can form core-shell structures with different aggregation states and shell thickness. Both in vitro and in vivo antibacterial tests show that acid condition and heat-treatment lead to appropriate AgNPs cores and pDA shell structures, which endow Ti with sustained antibacterial properties and preferable cell compatibility. One month of implantation in an infected animal model demonstrated that the obtained surface could promote osteogenesis and inhibit inflammation due to its strong antibacterial properties. Therefore, this study provides a promising approach to fabricate biocompatible antibacterial surface.

One-Pot Preparation of HTPB/nNi and Its Catalyst for AP.

The liquid phase reduction method is a common method used for preparing nano-nickel powder (nNi). However, the nNi surface is easily oxidized to form nickel oxide film, which affects its performance. In this work, nNi was prepared using anhydrous ethanol as a solvent and hydrazine hydrate as a reducing agent. Furthermore, HTPB/nNi composites were prepared using hydroxyl-terminated polybutadiene (HTPB) as a coating agent. The structure and morphology of the samples are characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray powder diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS). The catalytic behavior of HTPB/nNi on the thermal decomposition of ammonium perchlorate (AP) is studied by differential scanning calorimetry (DSC) and thermogravimetric analyzer (TG). The results show that HTPB/nNi has little effect on the low temperature thermal decomposition of AP, but the peak of high temperature thermal decomposition advances from 456 °C to 332 °C.

A simple mesoporous silica Nanoparticle-based aptamers SERS sensor for the detection of acetamiprid.

In this study, we developed a novel, rapid, simple, and sensitive nano sensor based on the controlled release of 4-Aminothiophenol (4-ATP) signal molecules from aptamers (Apts) modified aminated mesoporous silica nanoparticles (MSNs-NH2) for the quantitative detection of acetamiprid (ACE). Firstly, we synthesized the positively charged MSNs-NH2 by one-pot method, then loaded 4-ATP signal molecules into the pore, and finally electrostatically adsorbed the Apts onto the MSNs-NH2, which acts as a gate to control the release of signal molecules. When ACE is added to the system, ACE preferentially and specifically binds to Apts, so the gate opens and 4-ATP signal molecules are released from the pore. Meanwhile, the silver-loaded mesoporous silica nanoparticles (Ag@SiO2) were prepared by one-pot method as surface-enhanced Raman spectroscopy (SERS) substrate to amplify the signal. The intensity of 4-ATP signal molecules at 1433 cm-1 position was observed to has a linear relationship with the concentration of ACE by SERS detection. Under the optimized detection conditions, a linear correlation was observed in the range of 5-60 ng/mL (R2 = 0.99749), and the limit of detection (LOD) was 2.66 ng/mL. The method has high sensitivity, good selectivity and reproducibility, and can be used for actual sample analysis with the recovery rate of 96.24-103.6 %. This study provides a reference for the rapid and convenient detection of ACE in agricultural products.

One-pot fabrication of Mo1-xWxS2 alloy nanosheets as SERS substrates with highly Raman enhancement effect and long-term stability.

A new Mo1-xWxS2 two-dimensional nanosheets were prepared by the one-pot method. After certain Mo atoms in MoS2 were replaced by W ones in a hydrothermal reduction procedure, Mo1-xWxS2 was formed on the Mo foil. Well enhanced Mo1-xWxS2 nanosheets were prepared when the sodium tungstate concentration got under control. Various characterizations were carried out, which indicate that Mo1-xWxS2 nanosheets with good crystallinity. Compared with MoS2, the Raman intensity of Rhodamine 6G (10-6 M) was amplified by 1.7 times with Mo1-xWxS2 nanosheets as the substrate. The characteristic Raman peaks could still be clearly distinguished until the concentration of Rhodamine 6G (R6G), Methylene blue (MB) and Crystal violet (CV) down to 10-8, 10-8 and 10-7 M, respectively. With abundant edge active sites that facilitate charge transfer, Mo1-xWxS2 nanosheets could better enhance SERS signals of target detection molecules and get a good linear relationship exists within the concentration and Raman peak strength. In addition, R6G SERS detection also shows excellent reproducibility and long-term stability of this TMDs SERS substrate.

One-Pot Synthesis of UPy-Functionalized Nanocellulose under Mechanochemical Synergy for High-Performance Epoxy Nanocomposites.

The high strength, high specific surface area, excellent biocompatibility, and degradability of nanocellulose (NCC) make it a potential reinforcing phase for composite materials. However, the polyhydroxyl property of NCC renders it prone to self-aggregation and it has weak interfacial compatibility with non-polar substrates, limiting its enhancement performance for composite materials. Therefore, based on the high reactivity of NCC, the chemical modification of NCC to introduce functional groups is the basis for effectively reducing its self-aggregation, improving its interfacial compatibility with the polymer matrix, and creating nanocellulose-based functional materials. The existing functional modifications of NCC have limitations; they require cumbersome steps, generate low yields, and are environmentally unfriendly. Herein, ureido-pyrimidinone (UPy) was introduced to NCC through a sustainable and high-efficiency avenue formed by the mechanochemical synergy of microwaves and ultrasonication. The obtained UPy-modified nanocellulose (NCC-UPy) exhibited a rod-like shape, with a length of 200−300 nm and a width of 20−30 nm, which presented oriented and stable dispersion in an aqueous medium, and the zeta potential reached −40 mV. Moreover, NCC-UPy had good thermostability (>350 °C) and high crystallinity (82.5%) within the crystal type of cellulose I. Using the as-prepared NCC-UPy as a molecular bridge, it was organically combined with epoxy resin through multiple hydrogen bonds to construct a nanocomposite membrane with superior mechanical strength and thermal stability. The results revealed that NCC-UPy dispersed uniformly in the epoxy matrix without aggregating and that the interfacial compatibility was good, leading to an 87% increase in the tensile strength of the formed nanocomposite membrane when 0.5 wt.% NCC-UPy was loaded. It was proved that NCC-UPy had remarkable reinforcing potential and effective stress transfer capacity for composites. Consequently, this study may open the door to the development of a one-pot green approach for undertaking the functional modification of NCC, and it is of great significance for the development of NCC-based nanocomposites.

Facile pathway to construct mesoporous silica nanoparticles loaded with pyraclostrobin: Physicochemical properties, antifungal activity, and biosafety.

BACKGROUND: A controlled-release formulation based on mesoporous silica nanoparticles (MSNs) provides an effective way for reducing pesticide use and protecting the ecological environment. In this study, MSNs loaded with pyraclostrobin (PYR@MSNs) were prepared using a one-pot method. RESULTS: The characteristics of PYR@MSNs were systematically investigated, including morphology, loading content, ultraviolet (UV) resistance, release behavior, control effects against pathogens, and safety to nontarget organisms. The results show that the prepared PYR@MSNs presented characteristics of regular spherical shapes, uniform particle size (200 nm), high drug loading (38.9%), and enhanced UV resistance. Compared with traditional formulation, PYR@MSNs exhibited improved control effects against Fusarium graminearum, an extended control period, and lower toxicity to zebrafish, earthworms and BEAS-2B cells. CONCLUSIONS: This research will facilitate the development of efficient and safe pesticide delivery systems. The PYR@MSNs has showed its potential as a new controlled-release formulation with increased efficacy and is expected to benefit the sustainable development of agriculture. © 2022 Society of Chemical Industry.

One-pot synthesis and multifunctional surface modification of lithium-rich manganese-based cathode for enhanced structural stability and low-temperature performance.

High-energy-density lithium-rich Li1.2Ni0.13Co0.13Mn0.54O2 is regarded as one of the most promising cathode materials for lithium-ion batteries. However, its practical application is restricted by critical kinetics drawbacks and poor low-temperature electrochemical performances. In this research, Li1.2Ni0.13Co0.13Mn0.54O2 submicron particles coated by a Li7La3Zr2O12 (LLZO) layer and co-doped by La/Zr cations has been fabricated via a facile one-pot sol-gel technique and subsequent heat treatment. The coating LLZO layer with a few nanometers is able to build a rapid lithium-ion transport channel for adjacent particles and suppress severe side reactions between active material and the electrolyte. Moreover, large-radius La/Zr cations co-doping can broaden the diffusion paths of lithium ions, hinder the detrimental structural transformation, and improve the electrochemical structure stability of the cathode during repeated cycles. Owing to numerous merits from this multifunctional surface modification strategy, the modified Li1.2Ni0.13Co0.13Mn0.54O2 composite exhibits the significantly decreased interface impedance, enhanced Li+ diffusion kinetics and mitigated phase transformation, as well as excellent low-temperature electrochemical performance. It can contribute ultrahigh capacities of 173.8 mAh g-1 at -10 ℃ and 134.1 mAh g-1 at -20 ℃, respectively, displaying great application prospects of Li-rich cathode materials.

One-Pot Synthesis of Multifunctional Carbon-Based Nanoparticle-Supported Dispersed Cu2+ Disrupts Redox Homeostasis to Enhance CDT.

In chemodynamic therapy (CDT), the levels of reactive oxygen species (ROS) production plays an important role for evaluating the therapeutic efficacy. However, the high levels of glutathione (GSH) in tumor cells consume the ROS, directly reducing the therapeutic efficiency. Herein, we synthesized carbon-based nanoparticle (Cu-cys CBNPs) using one-pot strategy, which consume GSH via redox reactions to produce Cu+ that catalyze H2 O2 to produce . OH, thus the ROS level was observably increased through this synergistic effect. In vivo experiments further revealed that Cu-cys CBNPs could effectively inhibit tumor growth. Additionally, Cu-cys CBNPs can affect the activity of some protein sulfhydryl groups in cells, which was assessed by rdTOP-ABPP assay. In general, this study not only provides a potential CDT drug, but also provides a strategy for one-pot synthesis of multifunctional nanomaterials.

Preparation and characterization of templated porous carbons from sucrose by one-pot method and application as a CO2 adsorbent.

The templated porous carbons were prepared from sucrose by one-pot method. In this method in which the pre-synthesis of the hard template is eliminated, the porous carbons were produced by organic-inorganic self-assembly of sucrose, tetraethyl ortosilicate (TEOS), Pluronic P123 and n-butanol in an acidic medium, and subsequent carbonization. The synthesis parameters such as sucrose amount, TEOS molar ratio and carbonization temperature were evaluated for describing their effects on the pore structures of the synthesized carbons. The prepared porous carbons were characterized by N2 adsorption, thermogravimetric analysis (TGA), Raman spectroscopy, X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), and transmission electron microscopy (TEM) techniques. The carbon dioxide adsorption uptakes of the obtained porous carbons were determined at 1 bar and 273 K. The templated carbon obtained with the lowest TEOS molar ratio exhibited the highest BET surface area of 1289 m2/g and micropore volume of 0.467 cm3/g, and showed the highest CO2 uptake of 2.28 mmol/g.

One-Pot Synthesis of Al-P-O Catalysts and Their Catalytic Properties for O-Methylation of Catechol and Methanol.

A series of Al-P-O catalysts (Al-xP-O) were prepared using a P123-assisted one-pot method at different P/Al molar ratios and used for O-methylation of catechol and methanol. The influences of the P/Al molar ratio and P123 addition on catalyst structure and surface acid-base characteristics were investigated in detail. Increasing the P/Al molar ratio more favored crystalline aluminophosphate. The P123-assisted Al3+ and PO43- are known to be stabilized through weak steric force so that the formation of crystalline aluminophosphate could be inhibited at higher P/Al molar ratios. The results showed that the prepared Al-P-O catalysts possessed appropriate weak acid and weak base sites, which was beneficial to the reaction of catechol and methanol. The Al-1.1P-O catalyst synthesized with the assistance of P123 exhibited superior catalytic performances, with 52.5% catechol conversion and higher guaiacol selectivity of 97.6%.

Facile Synthesis of Thermoplastic Polyamide Elastomers Based on Amorphous Polyetheramine with Damping Performance.

Novel thermoplastic polyamide elastomers (TPAEs) consisting of long-chain semicrystalline polyamide 1212 (PA1212) and amorphous polyetheramine were synthesized via one-pot melt polycondensation. The method provides accessible routes to prepare TPAEs with a high tolerance of compatibility between polyamide and polyether oligomers compared with the traditional two-step method. These TPAEs with 10 wt % to 76 wt % of soft content were obtained by reaction of dodecanedioic acid, 1,12-dodecanediamine, and poly(propylene glycol) (PPG) diamine. The structure-property relationships of TPAEs were systematically studied. The chemical structure and the morphologic analyses have revealed that microphase separation occurs in the amorphous region. The TPAEs that have long-chain PPG segments consist of a crystalline polyamide domain, amorphous polyamide-rich domain, and amorphous polyetheramine-rich domain, while the ones containing short-chain PPG segments comprise of a crystalline polyamide domain and miscible amorphous polyamide phase and amorphous polyetheramine phase due to the compatibility between short-chain polyetheramine and amorphous polyamide. These novel TPAEs show good damping performance at low temperature, especially the TPAEs that incorporated 76 wt % and 62 wt % of PPG diamine. The TPAEs exhibit high elastic properties and low residual strain at room temperature. They are lightweight with density between 1.01 and 1.03 g/cm3. The long-chain TPAEs have well-balanced properties of low density, high elastic return, and high shock-absorbing ability. This work provides a route to expand TPAEs to damping materials with special application for sports equipment used in extremely cold conditions such as ski boots.

A Facile and In-situ Methanol-mediated Fabrication of Low Pd Loading, High-efficiency and Size-selectivity Pd@ZIF-8 Hydrogenation Catalyst.

In-situ encapsulation of tiny and well-dispersed Pd nanoparticles (Pd NPs) in zeolitic imidazolate frameworks (ZIFs) was firstly achieved using a one-pot and facile methanol-mediated growth approach, in which methanol served as both solvent and a mild reductant. The microstructure, morphology, crystallinity, porosity as well as evolution process of the catalysts were determined by TEM, XRD, N2 adsorption and UV-vis spectra. Due to the complete encapsulation of such Pd NPs combined with ultrahigh surface area and uniform microporous structure of ZIF-8, the resulting Pd@ZIF-8-60 min nanocomposite exhibited more superior catalytic activity for olefins hydrogenation with TOF of 7436 h-1 and excellent size selectivity than previously reported catalysts. Furthermore, the catalyst displays excellent recyclability for 1-octene hydrogenation and without any loss of the Pd active species.

Insight into the surface composition of bimetallic nanocatalysts obtained from microemulsions.

The enhancement of catalysts efficiency of bimetallic nanoparticles depends on the ability to exert control over surface composition. However, results relating surface composition and feeding solution of bimetallic nanoparticles synthesized in microemulsions are controversial and apparently contradictory. In order to comprehend how the resulting surface can be modified under different synthesis conditions and for different pairs of metals, a computer simulation study was carried out. The resulting surface compositions are explained based on the relative rates of deposition of the two metals, which depend on the particular metal pair, the concentration of reactants and the microemulsion composition. This study provides a satisfactory understanding of experimental results and allows us to identify the main factors affecting the nanoparticle's surface composition. Consequently, concrete and practical guidelines can be established to facilitate the experimental synthesis of bimetallic nanoparticles with tailored surfaces.

One-pot synthesis of rugged PdRu nanosheets as the efficient catalysts for polyalcohol electrooxidation.

Recently, intensive attention has been attracted to the two-dimensional metal nanosheets, owing to their excellent electrocatalytic performance for direct alcohol fuel cells (DAFCs). Herein, PdRu nanosheets have been synthesized successfully by a facile one-pot method. The rugged nanosheet structure provided plentiful surface active sites to enhance the electrocatalytic activity. Moreover, benefiting from the synergistic effect and improved electronic structure, PdRu NSs exhibited splendid electrocatalytic performance in ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR). Specifically, the mass activity of PdRu NSs was 1.72 and 3.69 times over those of Pd NSs and Pd/C catalysts in EGOR. Moreover, PdRu NSs displayed the largest mass activity in GOR, 1.48 and 2.47 times as large as Pd NSs and Pd/C catalysts. The results of stability tests demonstrated that the durability of PdRu NSs was the highest among the obtained catalysts. This work plays a directive role on the in-depth engineering on Pd-based catalysts with nanosheet architectures.

A Facile and Catalyst-Free Microwave-Promoted Multicomponent Reaction for the Synthesis of Functionalised 1,4-Dihydropyridines With Superb Selectivity and Yields.

We report a highly efficient green protocol for developing a novel library of 1,2,4-triazole-tagged 1,4-dihydropyridine analogs through the one-pot process from the four-component fusion of the 1H-1,2,4-triazol-3-amine with different chosen aldehydes, diethyl acetylenedicarboxylate, and active methylene compounds in a water medium under microwave irradiation and catalyst-free conditions. Excellent yields (94-97%) of the target products were achieved with high selectivity with a short reaction time (<12 min) at room temperature. The structures of the synthesized pyrimidine analogs were established by NMR and HRMS spectroscopic analysis. Simple workup, impressive yields, no column chromatography, green solvent, rapid reaction, and excellent functional group tolerance are the benefits of this protocol.

Silver-hydroxyapatite nanocomposites prepared by three sequential reaction steps in one pot and their bioactivities in vitro.

Hydroxyapatite (HA) combined with antimicrobial agents for biomedical application can effectively avoid the bacteria infection, while HA have the good performance. In this study, we prepared silver-hydroxyapatite (Ag-HA) nanocomposites using a one-pot method consisting of three sequential steps of wet chemical precipitation, ion exchange, and a silver mirror reaction. The HA nanoparticles used as the precursor for Ag ion doping were first synthesised by wet chemical precipitation. Next, Ag+ absorbed on HA surface through ion exchange reaction. Glucose was then added to initiate the silver mirror reaction, which made the Ag+ ions reduce to Ag0 and Ag nanoparticles in situ formed on HA nanoparticles. Subsequently, Ag-HA nanocomposites with different Ag content were prepared. X-ray diffraction, SEM, EDX mapping and TEM imaging confirmed that spherical Ag nanoparticles ~20-40 nm in diameter were adhered to the surface of HA nano-rods (0.4-0.8 µm in length and 15-40 nm in diameter). The Ag content (1.9-15.2 wt%) in the Ag-HA nanocomposites was adjusted by varying the feeding Ag/Ca molar ratio (2.0-20%). The cell viability evaluation in vitro proved that Ag-HA nanocomposites had low cytotoxicity to L929 normal cells. Meanwhile, the antibacterial examinations in vitro demonstrated that Ag-HA nanocomposites had obvious antibacterial effects on Gram-positive bacteria, Gram-negative bacteria, and fungus. The antibacterial results were dose-dependent on the accumulation of silver content. The Ag-HA nanocomposites loaded PMMA resins also demonstrated a potential antibacterial activity against S. mutans. This paper presents a convenient and bio-friendly approach for preparing Ag-HA nanocomposites with adjustable Ag content, which are a promising material for biomedical applications.

Stereoselective syntheses of 3-dehydroxynaltrexamines and N-methyl-3-dehydroxynaltrexamines.

Methodology is presented for the synthesis of 6α/ß-3-dehydroxynaltrexamines and 6α/ß- N-methyl-3-dehydroxynaltrexamines. A stereoselective route is provided for each target compound while a novel one-pot method for the synthesis of 6 α/ß-3-N-methyl-3-dehydroxynaltrexamines is also explored. These results enable the versatile and efficient preparation of key epoxymorphinan intermediates to facilitate future selective opioid ligand discovery and development.