Nuclear Magnetic Resonance Research Articles

Study on the Pilot-Scale Technology of Ginkgolide B Synthesis by Coprinus comatus

Ginkgo biloba extract (EGB) has been approved by the Food and Drug Administration in the United States for clinical studies on memory disorders. Ginkgolide B (GB) is the major terpene lactone component of EGB and is a specific and potent antagonist of platelet-activating factor (PAF). In a previous study, we reported the medium composition for the conversion of ginkgolides to GB by Coprinus comatus. In the present study, we applied the response surface methodology (RSM) to optimize the conversion conditions in a 20 L fermenter and applied HPLC-MS/MS, circular dichroism (CD) and infrared (IR) spectroscopy analyses, and nuclear magnetic resonance (NMR) to further confirm the sample structure. The optimal conversion conditions consisted of 12.7 L/min of ventilation, a 156 h conversion time, a 132 rpm rotating speed, a 0.04 MPa fermenter pressure, and a 27.8 °C conversion temperature. Under the optimal conditions, the GB conversion rate was 98.62%, and the GB content of the sample was higher than 98%. HPLC-MS/MS, CD, IR, and NMR analyses showed that the molecular formula of the sample was C20H24O10 and the chemical structure of the sample was in good agreement with the standard GB. Our current study lays the groundwork for the industrial production of GB.

Determining the Absolute Configuration of Small Molecules by Diffusion NMR Experiments

AbstractEnantiomers are ubiquitous in many areas of science, such as pharmaceuticals, agriculture, and food. Nuclear magnetic resonance (NMR) alone is not able to differentiate enantiomers as their spectra are identical. However, these can be distinguished using chiral auxiliaries (such as chiral complexing agents) that form diastereomeric complexes, but absolute identification is still troublesome, usually requiring a chemical reaction with a chiral derivatizing agent. Here, we propose a new method that uses a hybrid mixture of solvating agents in a simple comparison of diffusion NMR experiments, which can discriminate enantiomers in both frequency and diffusion domains, dubbed CHIMERA (CHIral Micelle Enantiomer Resolving Agent). The new method was assessed for twenty‐three small chiral molecules using a combination of BINOL and (−)‐DMEB, a chiral surfactant, and initial results indicate that absolute configuration can be obtained from a simple experiment.

Preparation of viscosity-reducing polycarboxylate superplasticizer (PCE) and its role in low water-to-cement ratio system

Owing to the low water-cement ratio (less than 0.25) of ultra-high-performance concrete (UHPC) materials, the system exhibits increased viscosity, diminished slurry flow, and challenges in pouring during the construction process, which compromise its workability. Consequently, the development of highly efficient viscosity-reducing polycarboxylate superplasticizer (PCE) is of paramount importance. In this study, we synthesized a series of viscosity-reducing polycarboxylate superplasticizers(JN-PCE) utilizing allyl polyethylene glycol ether (APEG), acrylic acid (AA), and sodium methallyl sulfonate (SMAS) as raw materials through the process of free radical polymerization. Fourier-transform infrared spectroscopy, nuclear magnetic resonance, gel permeation chromatography, and energy-dispersive X-ray spectroscopy were employed to characterize the materials. Subsequent evaluations of surface tension, fluidity, adsorption performance, and Marsh time demonstrated that these superplasticizers exhibited commendable dispersion and remarkable viscosity-reducing properties within a low water-cement ratio system. At a water-cement ratio of 0.18, the Marsh time of the JN-type PCE was reduced by 40% while maintaining the same fluidity, thereby underscoring the effective viscosity-reducing capabilities of the synthesized polycarboxylate superplasticizer.

Abstract 4140142: Neighborhood Perceptions Associate with Lipid Biomarkers in African-American Women with Cardiovascular-Kidney-Metabolic Syndrome: Data from the Step It Up Digital Health-Enabled, Community-Engaged Physical Activity Intervention

Background: Cardiovascular-kidney metabolic (CKM) syndrome is exacerbated among individuals experiencing chronic exposure to both environmental and psychosocial stressors. Both neighborhood and individual-level stressors increase chronic inflammation resulting in worsened CKM factors, such as hypertension, diabetes, and dys/hyperlipidemia. However, associations between neighborhood perceptions (NP) and lipid profiles remain understudied. Therefore, we examined associations between NP domains and lipid profiles among African-American (AA) women with ≥Stage 1 CKM syndrome (overweight/obesity) residing in resource-limited neighborhoods within the Washington, DC area. Methods: Participants were enrolled in Step It Up, a technology-enabled, community-engaged physical activity (PA) intervention. Fasting blood samples were drawn at baseline to measure lipoproteins using Nuclear Magnetic Resonance (NMR) spectroscopy. Factor analysis of overall NP identified four perception sub-scores: disorder, social cohesion, violence, and safety (higher score=favorable perception). Associations between NP domains and lipoprotein particles were analyzed using multivariable regression adjusting for BMI, ASCVD 10-year risk score, and lipid-lowering therapy. Results: Participants (n=169) had mean age=57.16 ± 12.00 and BMI 35.99 ± 6.57. Perceptions of safety were positively associated with LDL concentrations (LDLc) and large LDL particles (L-LDLp) (β=4.70 [SD=2.41], p=0.05, β= 43.75 [17.70], p= 0.01), respectively). Perceptions about neighborhood violence were positively associated with L-LDLp (marginally) and very-low-density lipoprotein size (VLDLz) (β= 7.10 [3.96], p=0.08, β= 0.31 [0.14], p= 0.02, respectively). No associations were found between disorder and social cohesion with lipid biomarkers. Conclusions: After adjusting for BMI, ASCVD risk, and lipid-lowering therapy, there were significant associations between neighborhood perceptions of safety and violence with lipid profiles among AA women with CKM syndrome. Greater perceived safety was associated with higher LDLc and L-LDLp while more favorable perception about neighborhood violence was associated with higher L-LDLp. Future work should examine whether improving neighborhood resources and perceptions may improve CKM health among urban AA women.

Structural characterization and physicochemical properties of different hydrophilic natural deep eutectic solvents.

To overcome the toxic nature of organic solvents, scientific interest in the use of green solvents, particularly natural deep eutectic solvents (NADES), has increased over the past decade, leading to new applications in the food, nutraceutical, pharmaceutical, and cosmetic industries. Understanding the physicochemical properties and molecular interactions of NADES is essential for uncovering new potential applications in these fields. In this study, several lactic and citric acid-based NADES, as well as chloride choline- and urea-based NADES, were evaluated for their physicochemical properties, including density, pH, viscosity, conductivity, and refractive index. Additionally, nuclear magnetic resonance (NMR), and in particular nuclear Overhauser enhancement spectroscopy (NOESY), was employed to investigate the intermolecular interactions between the NADES components to confirm the formation of the eutectic mixture. The extraction efficiency of the confirmed NADES was tested for extracting polyphenols as a proof of concept to highlight their relationship with the measured properties. Lactic and choline chloride-based NADES provided the highest extraction yields. These results were also compared with the predicted extraction capabilities of each NADES provided by the COSMO-RS software.

Bioinspired Passive Cooling Hydrogel for Visualizing Hygroscopicity and Desorption Process

AbstractSelf‐hygroscopic hydrogels, characterized by high evaporation enthalpy, cooling efficiency, and self‐regulating properties, have garnered significant attention. However, most current research focuses on enhancing the hygroscopic and desorption performance, often overlooking the importance of monitoring the self‐regulation process, which limits its further application. Advanced visualization technologies, such as in situ electrical impedance tomography, low‐field nuclear magnetic resonance, and hyperspectral imaging, offer potential insights into this behavior, yet they often require additional devices, incur high costs, and involve complex sample preparation processes. Therefore, drawing inspiration from nature, humidity‐color‐sensitive hydrogels (HCSHs) strategy is proposed for visualized cooling. Benefiting from the strong polar responsiveness of the aggregation‐induced emission (AIE) molecules, the hydrogel's fluorescence significantly changes with varying interior water content, thereby its self‐regulation process is monitored easily. Further, the obtained hydrogel could be applied in the electronic device cooling owing to the polymer skeletons’ high swelling ratio, strong adhesion, and excellent self‐hygroscopic properties. This strategy overcomes current limitations in the visual technology of self‐hygroscopic materials and provides new insights into intelligent thermal management for electronic devices.

Chromatographic analysis of ponatinib and its impurities: method development, validation, and identification of new degradation product

BackgroundPonatinib, a third-generation tyrosine kinase inhibitor, is employed in the management of adult chronic myeloid leukemia. Nevertheless, the presence of process impurities and degradation impurities linked to ponatinib may potentially influence its effectiveness and safety. Therefore, the objective of this research was to establish a robust liquid chromatography method and systematically validate it for the detection of substances related to ponatinib.MethodsThe separation of ponatinib and its impurities was conducted using an Agilent 5HC-C18 chromatographic column (4.6 mm × 250 mm, 5 μm). The mobile phase A comprised a mixture of water and acetonitrile in a 9:1 ratio, with an aqueous solution of pH 2.4 containing 2 mM potassium dihydrogen phosphate and 0.4% triethylamine. Mobile phase B, consisting of acetonitrile, was eluted in a gradient fashion. The flow rate was set at 1.0 mL/min, detection wavelength at 250 nm, column temperature at 40°C, and injection volume at 10 μL.ResultsThe method demonstrated high specificity, sensitivity, solution stability, linearity, precision, accuracy, and robustness. Additionally, this research unveiled a novel compound, imp-B, generated via the oxidative degradation of ponatinib. The molecular structure of the newly discovered product was elucidated through the utilization of nuclear magnetic resonance (NMR) and high-resolution mass spectrometry (HRMS).ConclusionIn conclusion, the chromatographic method developed in this study has the potential to be utilized for the detection of ponatinib and its impurities, thereby offering significant insights for quality assessment in ponatinib research.

Multi-omic molecular characterization and diagnostic biomarkers for occult hepatitis B infection and HBsAg-positive hepatitis B infection

BackgroundThe pathological and physiological characteristics between HBsAg-positive HBV infection and occult hepatitis B infection (OBI) are currently unclear. This study aimed to explore the immune microenvironment in the peripheral circulation of OBI patients through integration of proteomic and metabolomic sequencing, and to identify molecular biomarkers for clinical diagnosis of HBsAg-positive HBV and OBI.MethodsThis research involved collection of plasma from 20 patients with OBI (negative for HBsAg but positive for HBV DNA, with HBV DNA levels < 200 IU/mL), 20 patients with HBsAg-positive HBV infection, and 10 healthy individuals. Mass spectrometry-based detection was used to analyze the proteome, while nuclear magnetic resonance spectroscopy was employed to study the metabolomic phenotypes. Differential molecule analysis, pathway enrichment and functional annotation, as well as weighted correlation network analysis (WGCNA), were conducted to uncover the characteristics of HBV-related liver disease. Prognostic biomarkers were identified using machine learning algorithms, and their validity was confirmed in a larger cohort using enzyme linked immunosorbent assay (ELISA).ResultsHBsAg-positive HBV individuals showed higher ALT levels (p=0.010) when compared to OBI patients. The influence of HBV infection on metabolic functions and inflammation was evident through the analysis of distinct metabolic pathways in HBsAg-positive HBV and OBI groups. Tissue tracing demonstrated a connection between Kupffer cells and HBsAg-positive HBV infection, as well as between hepatocytes and OBI. Immune profiling revealed the correlation between CD4 Tem cells, memory B cells and OBI, enabling a rapid response to infection reactivation through cytokine secretion and antibody production. A machine learning-constructed and significantly expressed molecule-based diagnostic model effectively differentiated HBsAg-positive and OBI groups (AUC values > 0.8). ELISA assay confirmed the elevation of FGB and FGG in OBI samples, suggesting their potential as biomarkers for distinguishing OBI from HBsAg-positive infection.ConclusionsThe immune microenvironment and metabolic status of HBsAg-positive HBV patients and OBI patients vary significantly. The machine learning-based diagnostic model described herein displayed impressive classification accuracy, presenting a non-invasive means of differentiating between OBI and HBsAg-positive HBV infections.

A New Class of Oxyhalide Solid Electrolytes NaNbCl6‐2xOx for Solid‐state Sodium Batteries

AbstractSodium‐based batteries are gaining momentum due to the abundance and lower cost of sodium compared to lithium. Solid‐state sodium batteries can also provide further safety advantages. However, sodium‐based solid‐state electrolytes (SSEs) that meet all the rigorous requirements, such as high ionic conductivity, oxidative stability with the cathode, and ease of processability, are lacking. We present here a new class of sodium‐based oxyhalide electrolytes NaNbCl6‐2xOx with a facile mechanochemical synthesis. The oxyhalide NaNbCl4O exhibits close to two orders of magnitude higher ambient‐temperature sodium‐ion conductivity (1.03×10−4 S cm−1) compared to the halide counterpart NaNbCl6 (3×10−6 S cm−1). Structural motifs unique to the oxygen content in NaNbCl6‐2xOx are identified with 23Na and 93Nb magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy and x‐ray diffraction (XRD). Solid‐state sodium batteries assembled with NaNbCl4O electrolyte and the cobalt‐ and nickel‐free layered Na0.70Fe0.3Mn0.65Al0.05O2 cathode exhibit a maximum discharge capacity of 155 mAh g−1 with good cycle life at ambient temperature.

Abstract 4133257: Circulating Ketone Bodies, Lipoprotein(a) and Incident Cardiovascular Outcomes and Mortality: Insights from The UK Biobank

Background: Lipoprotein(a) [Lp(a)] is an independent risk factor for atherosclerotic cardiovascular disease (ASCVD). Recent epidemiological studies have revealed an association between ketone bodies (KB) and adverse cardiovascular outcomes, offering a unique insight into metabolic health and its impact on mortality risk. Elevated levels of both Lp(a) and KB may synergistically amplify pathological processes, including endothelial dysfunction, inflammation, and oxidative stress, through their involvement in shared pathophysiological pathways, thereby exacerbating disease progression beyond the impact of each biomarker individually. Methods: Utilizing data from the UK Biobank, KB were measured by nuclear magnetic resonance spectroscopy and serum Lp(a) concentrations were measured using an immunoturbidimetric assay. Four groups were created as follows: Group 1: Lp(a)<125 nmol/L and Total KB<75 th percentile (<94 μmol/L); Group 2: Lp(a)≥125 nmol/L and Total KB<75 th percentile; Group 3: Lp(a)<125 nmol/L and Total KB≥75 th percentile; and Group 4: Lp(a)≥125 nmol/L and Total KB≥75th percentile. Multivariable-adjusted Cox proportional hazard models were used to examine the association of Lp(a) and total KB with incident cardiovascular outcomes and mortality. Results: A total of 72,704 UK Biobank participants (mean age 56 y, SD=8, 55% women) without prevalent CVD or HF with a median follow up of 13.4 years were included. In the fully adjusted model, compared with those in the reference group (Group 1), participants in Group 2, Group 3, and Group 4 demonstrated a 14%, 17%, and 38%, increased risk of incident ASCVD events, respectively (p<0.01 for all). However, those with Lp(a) ≥ 125 nmol/L and total KB < 75th percentile demonstrated no increased risk of HF, all-cause mortality, stroke, or CVD mortality. Participants with elevated levels of both Lp(a) and KB had significantly increased risk of all outcomes (Table). There was no evidence for a statistically significant interaction between Lp(a) and KB on any outcome. Conclusion: Consistent with prior literature, Lp(a) was associated with atherosclerotic outcomes. However, elevated KB was associated with all outcomes, irrespective of Lp(a) levels.

Tracking the Facet Transformation of CeO2 by 17O Solid-State Nuclear Magnetic Resonance.

CeO2 nanomaterials expose various crystal facets with distinct surface geometry, resulting in different surface reactivities and material behaviors that ultimately determine their performances and suitability for a wide range of applications. Here, we apply 17O solid-state nuclear magnetic resonance (NMR) to follow the facet transformation of CeO2 at increased temperatures, observing a transition from (100) to (110) and finally to the more stable (111), based on the characteristic NMR shifts associated with the unique surface structure of each facet. In addition, we explore the effects of Pt ions on the conversion of different facets, which are found to promote the formation of the thermally stable (111) facet. Furthermore, 17O solid-state NMR provides a semiquantitative method for measuring the fractions of exposed facets. This work offers new insights and a more comprehensive understanding of crystal facet structures, and the new approach can be readily extended to study the facets of other oxide-based materials.

An Efficient and Stable Polarizing Agent for In-Cell Magic-Angle Spinning Dynamic Nuclear Polarization NMR Spectroscopy.

Nuclear Magnetic Resonance (NMR) spectroscopy would be a method of choice to follow biochemical events in cells because it can analyze molecules in complex environments. However, the intrinsically low sensitivity of NMR makes in-cell measurements challenging. Dynamic Nuclear Polarization (DNP) has emerged as a method to circumvent this limitation, but most polarizing agents developed for DNP are unstable in reducing cellular environments. Here, we introduce the use of Gd(III)-based DNP polarizing agents for in-cell NMR spectroscopy. Specifically, we show their persistent stability in cellular formulations, and we investigate the DNP performance of the Gd(III)-based complex [Gd(tpatcn)] in human embryonic kidney cell lysates and intact cells. For cell lysates, DNP enhancements up to -27 are obtained on the cellular signals, reproducible even after storage at room temperature for days. Mixing the [Gd(tpatcn)] solution with intact cells enables the observation of cellular signals with DNP, and DNP enhancement factors of about -40 are achieved.

Enhancing CO2 uptake by aqueous K2CO3 solutions using H2O2‐derived reactive oxygen species: Novel rate promotion for CCU processes

AbstractThis study introduces a novel approach to promote CO2 absorption by aqueous K2CO3 solutions through the in‐situ generation of reactive oxygen species (ROS) via the alkali activation of H2O2. The superoxide radical anion (O2•‐) is recognized as a major contributor in this process, with its presence confirmed by UV‐Vis (Ultraviolet–visible) spectroscopy through the characteristic diformazan peak formed from the reaction between nitro blue tetrazolium (NBT) and superoxide. CO2 absorption experiments and 13C NMR (Carbon‐13 nuclear magnetic resonance) characterization demonstrate the enhanced efficiency of the promoted solution in both CO2 absorption and the conversion of K2CO3 to KHCO3. Comparative analysis with traditional promoters reveals the superior kinetic performance of the H2O2‐promoted system at room temperature. Notably, our system yields pure KHCO3 without by‐products, making it highly suitable for carbon capture and utilization (CCU) by enabling versatile subsequent transformation processes. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.

Unveiling Biodiesel Production: Exploring Reaction Protocols, Catalysts, and Influential Factors

AbstractAn environmentally responsible and sustainable replacement for finite fossil fuels is biodiesel. Because of its amazing qualities, biodiesel is becoming more and more popular as a renewable fuel around the globe. The many approaches, feedstocks, catalysts, comparison standards, reaction kinetics, final product analysis, and final product characterization of biodiesel are covered in this review article. Researchers have used a variety of techniques to produce biodiesel throughout history, with transesterification emerging as the most effective approach in more recent times. Numerous studies on biodiesel feedstock and catalysts to produce high biodiesel yields have been published; nevertheless, it should be highlighted that the type of feedstock must be considered while choosing a catalyst. The review paper highlights the significance of several parameters that are crucial to the manufacture of biodiesel, without which achieving a high yield would be challenging. The literature has also discussed the limitations and advantages of different catalysts, and scientists are currently working to identify the ideal catalyst within certain optimal parameters for the manufacture of biodiesel. Homogeneous reaction‐based biodiesel synthesis has a number of drawbacks, though, such as water content, a laborious purification procedure, and a low tolerance for free fatty acids. To address these issues, scientists have started investigating heterogeneous reactions involving solid catalysts. A large pore network, a moderate‐to‐high density of strong acid sites, a hydrophobic surface, and the ability to control surface hydrophobicity to avoid deactivation are all desirable characteristics of an ideal solid catalyst. Ion exchange resins, sulfated oxides, heterogeneous base catalysts, boron group‐based heterogeneous catalysts, alkaline earth metal oxides, mixed metal oxides, alkali metal oxides, heterogeneous catalysts derived from waste materials, and different approaches to biodiesel synthesis that employ enzymes, carbon‐based heterogeneous catalysts, and ionic liquids as catalysts are among the categories of catalysts that can be used in the production of biodiesel. The finest benchmarks to compare the quality of biodiesel with European and American Society for Testing Material standards. For detailed characterization of the finished product, gas chromatography and nuclear magnetic resonance are the most effective methods.

Antimicrobial and acaricide sanitizer tablets produced by wet granulation of spray-dried soap and clove oil-loaded microemulsion.

A novel sanitizer tablet containing clove essential oil (CO) microemulsion was developed. A preformulation study using nuclear magnetic resonance and thermal analyses showed component compatibility. The main components of the samples remained intact despite a color change, probably due to a strong acid-base interaction between eugenol and diethanolamine. The CO microemulsion showed acaricidal and larvicidal activities superior to the commercial product, with product efficacy of 99.9% and larvae mortality of 94%. Optimal spray-drying conditions were achieved with inlet and outlet temperatures of 50°C and 40°C, respectively, an aspiration rate of 1 m3 min⁻1, and a 0.25 L h⁻1 injection flow. The feed suspension comprised 50% (v/v) liquid soap, 37.5% (v/v) water, 12.5% (v/v) ethanol, and 5.0% (w/v) silica. This formulation and processing parameters allowed for successful free-flow powder formation, providing a suitable matrix for incorporating the CO microemulsion via wet granulation without heating. Finally, sanitizer tablets produced from such granules resulted in a uniform product with low weight variation (coefficient of variation of 0.15%), eugenol content of 95.5% ± 3.3, and friability of 0.58%. Furthermore, the tablets showed rapid aqueous dispersion, forming a colloidal system with particle sizes of 221 nm and a zeta potential of -17.2 mV. Antimicrobial activity tests demonstrated the effectiveness of the sanitizer tablet against bacteria and fungi, exhibiting comparable antimicrobial potency to isolated CO. Hence, the sanitizer tablet developed represents a promising candidate as a practical and efficient solution for pest control, offering strong antimicrobial and acaricidal activity.

The Mesoscopic Damage Mechanism of Jointed Sandstone Subjected to the Action of Dry–Wet Alternating Cycles

The effect of the dry–wet cycle, characterized by periodic water level changes in the Three Gorges Reservoir, will severely degrade the bearing performance of rock formations. In order to explore the effect of the dry–wet cycle on the mesoscopic damage mechanism of jointed sandstone, a list of meso-experiments was carried out on sandstone subjected to dry–wet cycles. The pore structure, throat features and mesoscopic damage evolution of jointed sandstone with the action of the dry–wet cycle were analyzed using a-low-field nuclear magnetic resonance (NMR) technique. Subsequently, the impact on the mineral content of dry–wet cycles was studied by small angle X-ray scattering (SAXS). Based on this, the mesoscopic damage mechanism of sandstone subjected to dry–wet cycles was revealed. The results show that the effects of the drying–wetting cycle can promote the development of porous channels within sandstone, resulting in cumulative damage. Besides, with an increase in dry–wet cycles, the proportion of small pores and pore throats decreased, while the proportion of medium and large pores and pore throats increased. The combined effects of extrusion crush, tensile fracture, chemical reaction and dissolution of minerals inside the jointed sandstone contributed to the development of mesoscopic pores, resulting in the increase of porosity and permeability of rock samples under the dry–wet cycles. The results provide an important reference value for the stability evaluation of rock mass engineering under long-term dry–wet alternation.

Dual-Responsive Nanoparticles for Smart Drug Delivery: A NIR Light-Sensitive and Redox-Reactive PEG-PCL-Based System.

Stimuli-responsive polymeric nanoparticles (NPs) can serve as smart drug delivery systems (DDSs) by triggering drug release upon external or internal stimuli. A dual-responsive DDS made of a triblock poly(ε-caprolactone)-poly(ethylene glycol)-poly(ε-caprolactone) (PCL-SS-PEG-SS-PCL) copolymer, bearing disulfide bonds between PCL and PEG, was synthesized. The copolymer was functionalized with coumarin and sensitive to near-infrared (NIR) light irradiation, while the S-S bonds could be cleaved by GSH (10 mM). Characterization was achieved by nuclear magnetic resonance, size exclusion chromatography, and Fourier transform infrared analyses. Nile Red (NR)-loaded NPs were prepared through self-assembly of the copolymer in water and analyzed by dynamic light scattering and field-emission scanning electron microscopy. The NR release upon ultraviolet (UV)/NIR light irradiation as well as by GSH concentrations was monitored by using fluorescence spectroscopy, while simultaneous exposure to UV/NIR light and intracellular GSH concentration led to faster NR release. AlamarBlue assay showed satisfactory cell viability of the NR-loaded NPs, while their cellular uptake in human dermal fibroblast cells was investigated by fluorescence microscopy and fluorescence emission measurements.

Efficient Search Algorithms for Identifying Synergistic Associations in High-Dimensional Datasets

In recent years, there has been a notably increased interest in the study of multivariate interactions and emergent higher-order dependencies. This is particularly evident in the context of identifying synergistic sets, which are defined as combinations of elements whose joint interactions result in the emergence of information that is not present in any individual subset of those elements. The scalability of frameworks such as partial information decomposition (PID) and those based on multivariate extensions of mutual information, such as O-information, is limited by combinational explosion in the number of sets that must be assessed. In order to address these challenges, we propose a novel approach that utilises stochastic search strategies in order to identify synergistic triplets within datasets. Furthermore, the methodology is extensible to larger sets and various synergy measures. By employing stochastic search, our approach circumvents the constraints of exhaustive enumeration, offering a scalable and efficient means to uncover intricate dependencies. The flexibility of our method is illustrated through its application to two epidemiological datasets: The Young Finns Study and the UK Biobank Nuclear Magnetic Resonance (NMR) data. Additionally, we present a heuristic for reducing the number of synergistic sets to analyse in large datasets by excluding sets with overlapping information. We also illustrate the risks of performing a feature selection before assessing synergistic information in the system.

Synthesis of Amorphous Cellulose Derivatives via Michael Addition to Hydroxyalkyl Acrylates for Thermoplastic Film Applications

The aim of this study is to prepare new cellulose derivatives that show good feasibility and processability. Accordingly, in this study, we demonstrate Michael addition to hydroxyalkyl acrylates, that is, 2-hydroxyethyl and 4-hydroxybutyl acrylates (HEA and HBA, respectively), to synthesize amorphous cellulose derivatives under alkaline conditions. The reactions were carried out in the presence of LiOH in ionic liquid (1-butyl-2,3-dimethylimidazolium chloride)/N,N-dimethylformamide (DMF) solvents at room temperature or 50 °C for 1 h. The Fourier transform infrared and 1H nuclear magnetic resonance (NMR) measurements of the products supported the progress of Michael addition; however, the degrees of substitution (DS) were not high (0.3–0.6 for HEA and 0.6 for HBA). The powder X-ray diffraction analysis of the products indicated their amorphous nature. The cellulosic Michael adduct from HEA with DS = 0.6 was swollen with high polar organic liquids, such as DMF. In addition to swelling with these liquids, the cellulosic Michael adduct from HBA was soluble in dimethyl sulfoxide (DMSO), leading to its 1H NMR analysis in DMSO-d6. This adduct was found to form a cast film with flexible properties from its DMSO solutions. Furthermore, films containing an ionic liquid, 1-butyl-3-methylimidazolium chloride, showed thermoplasticity. The Michael addition approach to hydroxyalkyl acrylates is quite effective to totally reduce crystallinity, leading to good feasibility and processability in cellulosic materials, even with low DS. In addition, the present thermoplastic films will be applied in practical, bio-based, and eco-friendly fields.

Research on mechanical properties and pore structure evolution process of steam cured high strength concrete under freeze thaw cycles.

With the widespread use of high-strength concrete structures (HC), the impact of pore structure on their performance has become a current research focus. The mechanism by which different curing conditions and freeze-thaw cycles influence the evolution of pore structure remains unclear. Therefore, this study systematically investigated the frost resistance of high-strength concrete under different curing conditions, measured the mass loss rate, compressive strength, and relative dynamic elastic modulus of concrete under freeze-thaw cycles. Utilizing low-field nuclear magnetic resonance (NMR) technology, this study analyzed the evolution of pore structure in HC under freeze-thaw cycles. Additionally, the fractal dimension was used to evaluate the change of concrete internal pore structure, so as to reflect the influence of pore structure on the mechanical properties of concrete subjected to freeze-thaw cycles, and then evaluated the freeze-thaw damage of HC. The experimental results indicated that the steam curing regimes led to an increase in the porosity of HC, thereby influencing its frost resistance. Steam-cured high-strength concrete (SMHC) exhibited a higher degradation rate under freeze-thaw cycles, resulting in a greater level of deterioration compared to standard curing high-strength concrete (SDHC), even under the same number of freeze-thaw cycles.