High Mass Research Articles

Drug-impregnated contact lenses via supercritical carbon dioxide: A viable solution for the treatment of bacterial and fungal keratitis

Keratitis is a corneal infection caused by various bacteria and fungi. Eye drop treatment of keratitis involves significant challenges due to difficulties in administration, inefficiencies in therapeutic dosage, and frequency of drug applications. All these are troublesome and result in unsuccessful treatment, high cost, time loss, development of drug resistance by microorganisms, and a massive burden on human health and the healthcare system. Most of the antibacterial and antifungal medications are non-water-soluble and/or include toxic drug formulations. Here, the aim was to develop drug-loaded contact lenses with therapeutic dosage formulations and extended drug release capability as an alternative to eye drops, by employing supercritical carbon dioxide (ScCO2) as a drug impregnation solvent to overcome inefficient ophthalmic drug use. ScCO2, known as a green solvent, has very low viscosity which provides high mass transfer power and could enhance drug penetration into contact lenses much better with respect to drug loading using other solvents. Here, moxifloxacin (MOX) antibiotic and amphotericin B (AMB) antifungal medicines were separately loaded into commercially available silicone hydrogel contact lenses through 1) drug adsorption from the aqueous solutions and 2) impregnation techniques via ScCO2 and their efficacies were compared. Drug impregnation parameters, i.e., 8–25 MPa pressure, 310–320 K temperature, 2–16-hour impregnation times, and the presence of ethanol as polar co-solvent were investigated for the optimization of the ScCO2 drug impregnation process. The highest drug loading and long-term release kinetic from the contact lenses were obtained at 25 MPa and 313 K with 2.5 h impregnation time by using 1 % ethanol (by volume). Furthermore, antibacterial/antifungal activities of the MOX- and AMB-impregnated contact lenses were effective against in vitro Pseudomonas aeruginosa (ATCC 10145) bacteria and Fusarium solani (ATCC 36031) fungus for up to one week. Consequently, the ScCO2 method can be effectively used to impregnate commercial contact lenses with drugs, and these can then be safely used for the treatment of keratitis. This offers a sustainable delivery system at effective dosage formulations with complete bacterial/fungal inhibition and termination, making it viable for real animal/human applications.

Development and application of UPLC-Q-Orbitrap HRMS methods for the determination of eight metabolites of p-chloronitrobenzene in human urine

Accurate, reliable, and sensitive methods for the determination of eight metabolites of p-chloronitrobenzene (p-CNB) were developed based on ultra-performance liquid chromatography − quadrupole − orbitrap high resolution mass spectrometry (UPLC-Q-Orbitrap HRMS). The free and conjugated forms of metabolites were determined before and after urine samples were hydrolyzed with acid. Subsequently, three solid phase extraction steps were used for concentration and purification. The calibration curves of the eight metabolites exhibited good linearity with an R2 of >0.999, and the precision was good as well, with the coefficient of variations of intra-day and inter-day being lower than 7.0 % and 8.5 %, respectively. Analytical accuracy for all metabolites varied within ranges of 76.0–102.9 %, and the limit of detection and limit of quantification of all the metabolites varied within ranges of 0.2–7.7 μg/L and 0.6–25.6 μg/L in human urine, respectively. In addition, the application potential of the proposed methods were evaluated by applying them to the determination of metabolites in the urine of workers exposed to p-CNB, and these results showed that these methods were accurate, reliable, and sensitive, which makes them an excellent choice for detecting the metabolites of p-CNB in the urine of exposed workers.

Subclinical hypothyroidism and metabolic syndrome in psychiatric patients: A systematic literature review and meta-analysis.

The systematic review evaluated the association of subclinical hypothyroidism (SCH) with metabolic syndrome (MetS) and specific MetS components in people with major psychiatric disorders. A systematic review and meta-analysis was conducted to evaluate the association of SCH with MetS and its components in people with major psychiatric conditions. Five studies incorporating 24,158 participants met the inclusion criteria. All five studies comprised patients with depression and/or anxiety. Three studies incorporating 3365 participants were suitable for the meta-analysis. The pooled Odds Ratio (OR) of MetS was 3.46 (95% Confidence Interval/CI = 1.39-8.62) in major depressive disorder (MDD) and anxiety disorders patients with concurrent SCH compared to those without SCH. Meta-analysis showed a significant positive association between SCH and high body mass index (OR = 2.58, 95%CI = 1.33-5.01), high fasting plasma glucose (OR = 3.05, 95%CI = 1.79-5.18) and low high-density lipoprotein cholesterol (OR = 2.30, 95%CI = 1.82-2.92). These findings suggest a significant positive association between MetS and SCH in people with MDD and anxiety disorders. This review informed the clinical implications of MetS in MDD with comorbid SCH and the importance of early diagnosis and treatment for SCH and MetS in psychiatric patients.

Low-dimensional signal representations for massive black hole binary signals analysis from LISA data

The space-based gravitational wave observatory LISA will provide a wealth of information to analyze massive black hole binaries with high chirp masses, beyond $10^5$ solar masses. The large number of expected MBHBs (one event a day on average) increases the risk of overlapping between events. As well, the data will be contaminated with non-stationary artifacts, such as glitches and data gaps, which are expected to strongly impact the MBHB analysis, which mandates the development of dedicated detection and retrieval methods on long time intervals. Building upon a methodological approach we introduced for galactic binaries, in this article we investigate an original non-parametric recovery of MBHB signals from measurements with instrumental noise typical of LISA in order to tackle detection and signal reconstruction tasks on long time intervals. We investigated different approaches based on sparse signal modeling and machine learning. In this framework, we focused on recovering MBHB waveforms on long time intervals, which is a building block to further tackling more general signal recovery problems, from gap mitigation to unmixing overlapped signals. To that end, we introduced a hybrid method called SCARF (sparse chirp adaptive representation in Fourier), which combines a deep learning modeling of the merger of the MBHB with a specific adaptive time-frequency representation of the inspiral. Numerical experiments have been carried out on simulations of single MBHB events that account for the LISA response and with realistic realizations of noise. We checked the performances of the proposed hybrid method for the fast detection and recovery of the MBHB.

Vacuum Loss Detection of PTC in CSP Plants via Temperature-Sensors

The efficient operation of a solar field is an essential factor for the commercial operation of a concentrating solar power (CSP) plant. In addition to predictive control for the highest possible constant outlet temperature at high mass flow, efficient operation also includes early detection of defective components and heat losses. This work presents a method for non-invasive heat loss detection as a strong indication for vacuum losses, based on measured operational data of Andasol III, an operating 50 MW parabolic trough collector (PTC) plant located in southern Spain. To detect vacuum losses via this method, mass flow rate and temperature reduction are determined separately for each individual loop via the analysis of a short-term temperature rise of the heat transfer fluid (HTF) during preheating. While the temperature reduction was measured directly, the mass flow was determined via the thermal time-of-flight (ToF) method using the same installed temperature sensors. By measuring thermal step responses during the preheating of the solar field at nighttime operation, the influence of fluctuating direct normal irradiance (DNI), misalignment of the absorber tubes and an offset in collector focus was circumvented. In the scope of the presented work, single loops were detected, which show a higher heat loss at lower mass flow rate and therefore have an increased probability of a higher vacuum loss. Better localization and early detection of these vacuum losses would allow the corresponding absorber tubes to be renewed at the economically and environmentally best time, improving the efficiency of the solar field and thus the entire CSP plant.

Common origin for black holes in both high mass X-ray binaries and gravitational-wave sources

Black-hole (BH) high-mass X-ray binary (HMXB) systems are likely to be the progenitors of BH-BH mergers detected in gravitational waves by LIGO/Virgo/KAGRA (LVK). Yet merging BHs reach higher masses ($ than BHs in HMXBs ($ and typically exhibit lower spins BH 0.25$ with a larger values tail) than what is often claimed for BHs in HMXBs BH 0.9$). This could suggest that these two classes of systems belong to different populations, but here we show that this may not necessarily be the case. The difference in masses is easily explained as the known HMXB-BHs are in galaxies with relatively high metallicity, so their progenitor stars are subject to strong mass loss from winds, leading to relatively low-mass BH at core collapse. Conversely, LVK is also able to detect BHs from low-metallicity galaxies that are known to naturally produce more massive stellar-origin BHs. However, the difference in spin is more difficult to explain. Models with efficient angular momentum transport in stellar interiors produce slowly spinning progenitors for both LVK and HMXB BHs. Known HMXBs have orbital periods that are too long for efficient tidal spin-up and are also unlikely to have undergone significant accretion spin-up. Instead, we show that the derived value of the BH spin depends strongly on how the HMXB accretion disc emission is modelled. We argue that since Cyg X-1 is never observed to be in a soft spectral state, the appropriate spectral models must take into account the Comptonisation of the disc photosphere. We show that such models are consistent with low spin values, namely: $a_ BH This was recently confirmed by other teams for both Cyg X-1 and LMC X-1 and here we show this is also the case for M33 X-7. We conclude that all known HMXB BHs can exhibit a low spin in accordance with the results of stellar evolution models. Hence, the observations presented in this work are consistent with the scenario where LVK BHs and HMXB BHs belong to the same population.

Insight into the mechanism of adsorption and release of 11-nor-9-carboxy-Δ9-tetrahydrocannabinol in sewage by modeling regional suspended particles for evaluation of the influence on monitoring of cannabis illicit abuse

The adsorption of 11-nor-9-carboxy-∆9-tetrahydrocannabinol (THC-COOH) by the suspended particles in sewage makes it fail to accurately monitor cannabis abuse. In this work, the model sewage sample was prepared through equivalent mixing the sewage from 10 different sewage treatment plants in Guangdong province of China and used as a comprehensive representative for investigating the adsorption and release behavior of THC-COOH on the suspended particles under different temperature and pH. The solid-liquid distribution of THC-COOH in sewage depended strongly on the adsorption and release properties which were susceptible to the temperature and pH, specially adjusting pH to 11.0 could release more than 90% of THC-COOH from the suspended particles. By means of the kinetics models, pseudo-second-order kinetic and Weber-Morris models revealed the mechanism of adsorption and release of THC-COOH in sewage that was a relatively reversible and controllable process with multiple interactions, and then it was further confirmed by the validation experiment in a variety of actual sewage samples. According to the suggested pH, the modification of the existing detection protocol prior to high performance liquid chromatography-tandem triple quadrupole mass spectrometry (HPLC-TQ-MS/MS), was successfully applied to determination of THC-COOH in the stimulated positive samples, and the recoveries and RSDs were respectively 95.48-99.79% and 4.0-5.6%. The finding could greatly help improving the accuracy of not only the detection of THC-COOH in sewage but also the estimation data of the consumption level of cannabis in the related regions.

Global years lived with disability for musculoskeletal disorders in adults 70 Years and older from 1990 to 2019, and projections to 2040

In this article, we provided a comprehensive overview and in-depth analysis of global patterns and temporal trends in years lived with disability (YLDs) for musculoskeletal (MSK) disorders in individuals aged ≥70. Data on YLDs for MSK disorders in individuals aged ≥70 were obtained from the Global Burden of Disease 2019. The average annual percentage change (AAPC) was calculated to assess the temporal trends in the YLDs rate of MSK disorders. A Bayesian Age-Period-Cohort model was used to predict the YLDs rate up to the year 2040. In 2019, the global rate of YLDs for MSK disorders in individuals aged ≥70 were 4819.81 (95 % UI: 3402.91 - 6550.77) per 100,000 persons. The YLDs rate of MSK disorders in female was 1.36 times higher than that in male, and was highest in high SDI regions. From 1990 to 2019, the global YLDs rate showed a slightly downward trend (AAPC = −0.04 %, 95 % CI: −0.06 % to −0.03 %), while it significantly increased in high, low-middle, low SDI regions. Tobacco and high body mass index were the primary risk factors worldwide, while in low SDI regions, occupational risks emerged as the predominant factors. Up to 2040, the global YLDs rate of MSK disorders are expected to increase by 1.78 %, with 36.39 %, 20.66 %, 18.96 % and 5.32 % growth in other MSK disorders, rheumatoid arthritis, neck pain and osteoarthritis. MSK disorders are a significant and continuously growing public health concern among older adults. Tailored interventions should be developed for older adults, taking into account the variations across distributions, trends, and risk factors in terms of sex and SDI levels.

Understanding proteome quantification in an interactive learning module on Google Cloud Platform.

This manuscript describes the development of a resource module that is part of a learning platform named 'NIGMS Sandbox for Cloud-based Learning' https://github.com/NIGMS/NIGMS-Sandbox. The overall genesis of the Sandbox is described in the editorial NIGMS Sandbox at the beginning of this Supplement. This module delivers learning materials on protein quantification in an interactive format that uses appropriate cloud resources for data access and analyses. Quantitative proteomics is a rapidly growing discipline due to the cutting-edge technologies of high resolution mass spectrometry. There are many data types to consider for proteome quantification including data dependent acquisition, data independent acquisition, multiplexing with Tandem Mass Tag reporter ions, spectral counts, and more. As part of the NIH NIGMS Sandbox effort, we developed a learning module to introduce students to mass spectrometry terminology, normalization methods, statistical designs, and basics of R programming. By utilizing the Google Cloud environment, the learning module is easily accessible without the need for complex installation procedures. The proteome quantification module demonstrates the analysis using a provided TMT10plex data set using MS3 reporter ion intensity quantitative values in a Jupyter notebook with an R kernel. The learning module begins with the raw intensities, performs normalization, and differential abundance analysis using limma models, and is designed for researchers with a basic understanding of mass spectrometry and R programming language. Learners walk away with a better understanding of how to navigate Google Cloud Platform for proteomic research, and with the basics of mass spectrometry data analysis at the command line. This manuscript describes the development of a resource module that is part of a learning platform named ``NIGMS Sandbox for Cloud-based Learning'' https://github.com/NIGMS/NIGMS-Sandbox. The overall genesis of the Sandbox is described in the editorial NIGMS Sandbox [1] at the beginning of this Supplement. This module delivers learning materials on the analysis of bulk and single-cell ATAC-seq data in an interactive format that uses appropriate cloud resources for data access and analyses.

Temperature and pressure prediction of offshore high CO2-content associated gas lift and analysis of influencing factors

With the continuous injection of CO2 into the reservoir, a portion of the sequestered CO2 is co-produced with crude oil, resulting in a significant concentration of CO2 in the associated gas. Utilizing high CO2-content associated gas for offshore gas lift operations improves the reutilization of such gas and reduces costs related to sourcing and transporting it. To ensure smooth activation of the gas lift valve, conducting a thorough study on temperature and pressure within the wellbore during the gas lift process is essential. This study developed a dynamic model for calculating the transient temperature and pressure within offshore gas lift wellbores and fitted equations to calculate the physical properties of high CO2-content associated gas for specific compositions. This refinement minimized computational discrepancies arising from fluctuations in physical property parameters. When applying this model to oilfield scenarios, the maximum error observed was 3.83%, which aligned well with the accuracy standards required for oilfield computations. By integrating oilfield production data, this research explored the influence of injection parameters on temperature and pressure dynamics within the gas lift wellbore. The results revealed that variations in injection temperature and pressure had minimal impact on the temperature at the gas lift valve. Yet, they induced significant changes in the pressure at that point. An increase in CO2 concentration within the gas source composition was associated with considerable shifts in temperature and pressure gradients throughout the wellbore. At high mass flow rates, the temperature gradient of the wellbore was notably reduced, while the pressure gradient was significantly enhanced. These research findings provided a theoretical basis for optimizing gas lift operations using high CO2-content associated gas in offshore settings.

Hollow Fiber Contactors with Improved Hydrophobicity for Acid Gas Removal: Progress and Recent Advances

The gas–liquid membrane contactor technology, which integrates the absorption process with membranes, is a developing membrane technology that is especially pertinent to acid gas absorption. When it comes to removing acid gases from natural gas or after combustion, membrane technology has demonstrated potential as a substitute for conventional absorption columns. The membrane contactor offers exceptional operating flexibility and a high mass transfer area. In addition to summarizing the key elements of membrane materials, absorbents, and membrane contactor design, this paper presents the working principle and wetting mechanism of hollow membrane contactors and focuses the most recent advancements in membrane contactor research in gas separation from gas mixtures. The state-of-the-art overview of highly hydrophobic microporous membranes is presented after a discussion of the main challenges to the preparation of superhydrophobic membranes.

Vertical VOPO4·2H2O Nanosheets with Richly Exposed (200) Plane Enable Fast-Kinetics High-Mass-Loading Cathodes for Zn-Ion Batteries.

Extending the layer spacing of the (001) planes to regulate the mobility of Zn2+ is widely adopted to optimize the performance of VOPO4·2H2O cathode for zinc-ion batteries. However, the unique function originating from other planes is often neglected. Herein, an effective in situ conversion methodology is proposed for the synthesis of the (200) oriented growth of vertical VOPO4·2H2O nanosheets with oxygen vacancies (VOd-VOPO4). Theoretical simulation and ex situ characterizations collaboratively demonstrate that the richly exposed (200) plane with tetragonal channels can offer quick pathways for in-layer and cross-layer migration of Zn2+, exhibiting enhanced transfer kinetics with improved reversible capacity. Meanwhile, efficient electron migration in VOd-VOPO4 is guaranteed by the introduction of oxygen vacancies. Thus, the as-prepared VOd-VOPO4 harvests exceptional discharge capacity, impressive rate capability, and remarkable long-cycle stability at high mass loading. Notably, the VOd-VOPO4 electrode (15mg cm-2) provides a capacity of 213.5mAhg-1 with an ultrahigh areal capacity of 3.02 mAh cm-2 at 0.1 A g-1, showing great potential for applications. This study highlights the orientated growth strategy for facilitating ion storage and migration, offering novel perspectives on the development of high-performance electrodes and beyond.

10-year outcome after Roux-en-Y gastric bypass vs. duodenal switch with high body mass index: a randomized clinical study

10-year outcome after Roux-en-Y gastric bypass vs. duodenal switch with high body mass index: a randomized clinical study

The tubular baffled reactor and its potential for the biological methanation of carbon dioxide

The biological Power to Methane process (PtM) is gaining ground as an answer to the long-term renewable energy storage problem. Methane is an efficient hydrogen carrier, has an established worldwide transport infrastructure and can serve as a link between renewable power generation and a circular carbon economy. One of the defining factors regarding the scalability of the PtM process is the design of the reactor as it can determine the production rate/energy expenditure ratio. The tubular baffled reactor, a popular reactor design within the chemical industry has been assessed in the present study as a biomethanation reactor for the first time. The experiments were conducted with mixed cultures and the results point to high gas-liquid mass transfer capabilities as indicated by the methanation rates achieved (>90 % CH4 at 270 L/L/d mixed gas input rate). The gas/liquid flow ratio appears to have a stronger effect on methanation than the gas residence time. The working length of the reactor determines the pressure drop experienced by the culture, with higher pressure drops showing a negative correlation to methanogenesis.

Adopting adalimumab combined surgery in the management of moderate to severe hidradenitis suppurativa: Experience from a single medical center in southern Taiwan.

Hidradenitis suppurativa (HS) is a chronic inflammatory disorder primarily affecting the intertriginous and anogenital regions. Guidelines recommend various treatments for HS, including biologic agents like adalimumab for moderate to severe cases. Adalimumab is a type of human monoclonal IgG1 antibody designed to target tumor necrosis factor α. Recent studies have shown the effectiveness of adalimumab, either alone or combined with surgery, in managing HS. We retrospectively analyzed the medical chart of HS patients in a southern Taiwan medical center from 2019 to 2022 and investigated clinical features and treatment response. The institutional review board at Chang Gung Medical Foundation granted approval for the study. We primarily focused on moderate to severely affected patients. One hundred and two clinically diagnosed HS patients participated, with a male-to-female ratio of 2:1 and an average age of 31.8 at diagnosis. Among them, 41.2% were in Hurley stage III and 32.4% in stage II. Nineteen patients received excision with pre-surgical adalimumab; their average age at diagnosis was 31.1, with a gender ratio of 5.3:1. Surgery was most common on the buttocks (68%), axillae (21%), and groin (10%). Excision patients were primarily in advanced stages (Hurley III 94.7%, II 5.3%) with high body mass index. Adalimumab and surgery combined yielded a 68.4% improvement rate, while 15.8% remained stable and 15.8% did not respond as expected. In addition, smoking and obesity were prevalent among patients. Adalimumab showed promising results in moderate to severe HS, with significant improvement observed in our cases. The combination of adalimumab and surgery appeared effective in advanced HS patients with larger involved areas and more tunnels. No severe adverse events were reported. However, our study was limited by its retrospective nature and the lack of a control group. Despite these limitations, our study revealed the benefits of integrating adalimumab with suitable surgical procedures in managing patients experiencing moderate to severe HS in real-world scenarios.

Highly active and robust Ir-Ru electrocatalyst for alkaline HER/HOR: Combined electronic and oxophilic effect

Developing efficient and robust electrocatalysts for alkaline hydrogen oxidation/evolution reaction (HOR/HER) is crucial to alkaline fuel cells and water electrolysis. Herein, we report iridium-ruthenium nanoclusters on carbon support (Ir-Ru@C) electrocatalyst with ultra-high alkaline HOR/HER catalytic activity and anti-CO poisoning capability. The HOR mass activity and specific activity of Ir-Ru@C electrocatalyst are 2.3 and 5.7 times that of commercial Pt@C. For alkaline HER, Ir-Ru@C shows an ultra-low overpotential of 13 mV at 10 mA cm−2 and high mass activity of 4.0 A mg−1(Ir+Ru) at 60 mV (vs. RHE), superior to commercial Pt@C and most of the advanced electrocatalysts reported in literature. Mechanism studies based on spectroscopic, electrochemical and DFT results reveal that the combined electronic and oxophilic regulation of Ir-Ru bimetallic nanoclusters simultaneously optimizes Had and OHad adsorption, leading to its high activity and anti-CO poisoning capabilities.

Polyprenylated acylphloroglucinols from Hypericum sampsonii with cytotoxicity against pancreatic carcinomas

Chemical investigation on the 80% EtOH extract of the air dried aerial parts of Hypericum sampsonii resulted in the isolation of two new polycyclic polyprenylated derivatives, hypersampines A and B (1 and 2). The structures of the new compounds were elucidated by spectroscopic data (NMR, IR, and UV) and high resolution mass analysis. The two isolated polyprenylated acylphloroglucinols were tested in vitro for cytotoxic activities against 6 pancreatic cell lines. As a result, compounds 1 and 2 possessed modest cytotoxic activities against all the tested tumor cell lines with IC50 values less than 40 μM.

Wood derived carbon embedded with shell-core CoP@CoFe for efficient oxygen evolution

Development of hybrid materials with specific architecture, interface, and multicomponent interactions demonstrates effective paradigm for pursuing high-performance energy conversion materials. Herein, using renewable and inexpensive wood-derived carbon as host, the shell-core CoP@CoFe particles are embedded on walls of carbonized wood channels (termed as CoP@CoFe/CW) to fabricate composite catalyst for electrocatalysis oxygen evolution reaction (OER). With benefits of the well distribution of CoP@CoFe particles, high conductivity of CW with channels, and good integration between them, highly exposed catalysis surface as well as rapid charge/mass transfer are achieved. The interface effect of shell-core hybrid activates the intrinsic OER efficiency of CoP@CoFe. Thus, the designed CoP@CoFe/CW yields excellent OER performance with ultralow overpotential of 120 mV (10 mA cm−2). This strategy of catalyst design based on eco-friendliness and renewable CW host may offer promising reference to explore composite materials with high conductivity and fast mass transfer for water electrolysis and other energy storage/conversion systems.

A Triple Crosslinked Binder with Hierarchical Stress Dissipation and High Ionic Conductivity for Advanced Silicon Anodes in Lithium-ion Batteries.

Silicon (Si) is a promising anode material for high-energy-density lithium-ion batteries, but the significant volume change of Si particles during alloying/dealloying with lithium (Li) undermines the mechanical integrity of Si anode, causing electrode fracture, delamination and rapid capacity decay. Herein, a robust triple crosslinked network (TCN) binder with high ionic conductivity and hierarchical stress dissipation is reported for Si anodes, which is prepared by in situ chemical crosslinking polyacrylic acid (PAA) and melamine (MA). The triple interactions of hydrogen bonds, electrostatic interactions, and covalent amide bonds enhance the adhesion of binder to Si and synergistically promote stress dissipation within Si anodes, thus strengthening the dynamic structural stability of Si anodes during cycling. Moreover, the rapid coupling/decoupling of Li+ with the TCN binder enables an impressive Li+ transference number of 0.63 and high ionic conductivity of 1.2 × 10-4 Scm-1. Consequently, the Si-TCN anode delivers specific capacity of 2268 mAhg-1 with a high mass loading of 2mgcm-2, high-rate performance of 1673 mAhg-1 at 5 Ag-1, and stable cycling for 250 cycles at 1 Ag-1, thus showing great prospects for high-energy-density Si-based batteries.

Empowering the rapid authentication of the botanical origin of monofloral honey by coated blade spray mass spectrometry (CBS-MS)

In the quest for a rapid and cost-effective tool for determining the botanical origin of monofloral honey, the analytical capabilities of coated blade spray mass spectrometry (CBS-MS) were investigated. To this aim, the chemical profiles of 64 honey samples from seven different botanical origins (acacia, dandelion, chestnut, rhododendron, citrus, sunflower, and linden) were captured by the absorbent of the coated blades and then analyzed by mass spectrometry. An exploratory analysis was performed by principal component analysis (PCA) to generate a graphical representation of the CBS-MS data that allows the discovery of patterns, outliers, or relations between types of honey in an unsupervised manner. Additionally, the performances of four different classification algorithms (least absolute shrinkage and selection operator (LASSO), random forest (RF), and neural network (NNET) partial least squares discriminant analysis (PLS-DA)) were built up and compared. The performances of the four classifiers were verified by a 50 times-repeated, 5-fold-cross-validation and permutation test. Although all classifiers performed well, the RF showed significantly higher performances in cross-validation (with area under the curve (AUC) of 0.99, overall accuracy 0.94, Kappa 0.93, sensitivity 0.94, and specificity 0.99). Moreover, the permutation tests showed the models were not overfitted. Finally, to determine the molecular identities of the ions that most contribute to the classification, extracts from the same honey samples were prepared, analyzed by liquid chromatography coupled to high resolution tandem mass spectrometry (LC-HRMS/MS), and the most significant features were annotated. This proof-of-principle work warrants a future large-scale study to validate and challenge this CBS-MS-based method with a greater number of honeys from different years and geographical origins.