Search Results (76)

The growing use of experimental radiopharmaceuticals for targeted radionuclide therapy (TRT) highlights the need for robust “in house” radiolabeling protocols. Among these, PSMA-ALB-56 is a PSMA ligand incorporating an albumin-binding moiety to enhance pharmacokinetics, which showed promise for prostate cancer treatment. This study investigated manual radiolabeling conditions of this vector molecule with lutetium-177 and developed a corresponding automated synthesis protocol. Manual experiments on low activities explored buffer systems and antioxidants, identifying sodium acetate buffer and L-methionine as optimal, achieving radiochemical purities above 97% with excellent stability over 48 h. However, when these conditions were transposed directly to an automated process on a GAIA^® module with activities > 2 GBq, radiochemical purity dropped below 70% due to significant radiolysis. This result emphasized that conditions optimized at low activities are not directly transferable to high-activity automated production, and highlighted the crucial role of antioxidant concentration. An optimized automated method was subsequently developed, integrating a solid-phase extraction purification step, higher antioxidant levels during radiolabeling and formulation, and a larger final product volume. These changes led to radiochemical purities above 98.9% and excellent product stability over 120 h for 3 test batches. The presence of high concentrations of methionine and ascorbic acid was essential to protect against radiolysis. This work underscores the importance of adjusting radiolabeling strategies during process scale-up and confirmed that antioxidant concentration is essential for successful ¹⁷⁷Lu radiolabeling. The optimized automated method developed here for [¹⁷⁷Lu]Lu-PSMA-ALB-56 may also be adapted to other radiopharmaceuticals in development for TRT. Full article

Wastewater analysis plays a central role in monitoring patterns of drug use within specific populations. It provides objective and real-time estimates of consumption, with minimal ethical concerns. In the current European context, drugs of abuse continue to be detected in wastewater, with varying incidences across countries. Their monitoring enables the prioritisation of public health and legal interventions by healthcare professionals and drug monitoring agencies. Therefore, the development and implementation of efficient methodologies for monitoring drugs of abuse in wastewater samples is of critical importance. This systematic review aims to explore the use of miniaturised sample extraction techniques based on solid-phase microextraction for the determination of drugs of abuse in wastewater. In fact, the extraction procedure must be fast, effective, and selective in order to retain the analytes of interest. Miniaturised techniques have thus emerged as promising alternatives to conventional methods. Magnetic solid-phase extraction (MSPE) and molecularly imprinted polymers (MIPs) represent the most widely applied solid-phase microextraction techniques in recent years for the analysis of drugs of abuse in wastewater. Looking ahead, future perspectives include the development of eco-friendly workflows, automated and time-efficient techniques, increasingly selective sorbents, and robust analytical methods. Full article

Conventional methods for testing steroids and hormones (SHs) in environmental samples are exhaustive, complex, and score poorly in sustainability matrices. Therefore, this study evaluates the automated sample preparation approach using the modular Biomek i7 Workstation for the analysis of 27 SHs in wastewater. Method development involved optimizing Ultra Performance Liquid Chromatography–Tandem Mass Spectrometry (UPLC-MS/MS) parameters, preparing wastewater matrix blank, and assessing extraction efficiency using three solid phase extraction (SPE) cartridges. Extraction efficiency trials showed suitability in the order of Hydrophilic–Lipophilic Balance (HLB) > Mixed-Mode Cation Exchange (MCX) > Mixed-Mode Anion Exchange (MAX). The method demonstrated specificity for all targeted SHs, with Cholesterol showing a maximum interfering peak of 17.71% of the quantification limit (LOQ). The method met matrix effect tolerance of ±20% for 26 SHs, while Epi Coprostanol (34.92%) showed signal enhancement >20%. The 8-point calibration curve plotted using automated extraction demonstrated acceptable linearity across the tested range. Spiked studies at low (LQC), middle (MQC), and higher (HQC) quality control (QC) levels (n = 6, repeated on three separate occasions) demonstrated % RSD values within 20% and recoveries ranging from 71.54% to 115.00%. The method met validation criteria, showing reliability in Intra-Laboratory Comparison (ILC) and Blind Testing (BT). The method outperformed the conventional approach in greenness assessment (Complex Modified Green Analytical Procedure Index) and practicality evaluation (Blue Applicability Grade Index), offering an effective and sustainable protocol for environmental testing laboratories. Full article

Conventional methods for detecting pharmaceutical and personal care products (PPCPs) in environmental samples are complex, resource-intensive, and not sustainable. Therefore, this study aimed to evaluate an automated sample preparation approach using the Biomek i7 Workstation to analyze 69 PPCPs in wastewater, with the objective to improve monitoring of public health and environmental protection. The method underwent extensive development, including optimization of UPLC-MS/MS parameters, preparation of wastewater matrix blank sample and assessment of extraction efficiency using three types of SPE cartridges. Extraction efficiency trials revealed that the order of suitability for SPE cartridges is Mixed-Mode Anion Exchange (MAX) > Mixed-Mode Cation Exchange (MCX) > Hydrophilic–Lipophilic Balance (HLB). The method demonstrated specificity for all targeted PPCPs, with the max interfering peak for 1, 7 Dimethylxanthine reaching 14.79% of the response at the target limit of quantification (LOQ). The method met ±20% matrix effect tolerance for 63 PPCPs, while 6 PPCPs showed signal enhancement. The 8-point procedural calibration curve prepared using automated robotic extraction has demonstrated linearity across the tested range. A spiking study at low (LQC), medium (MQC), and high (HQC) quality control levels (n = 6), repeated on three separate occasions, showed % RSD values within 20% and % recovery between 80 and 120%. The method met validation requirements, showed reliability in Intra-Laboratory Comparison, Blind Testing (BT) and received high ratings for greenness (Green Analytical Procedure Index, Analytical GREEnness) and practicality (Blue Applicability Grade Index). Full article

Fumonisins, primarily produced by Fusarium spp. and Aspergillus section nigri, are common contaminants in maize, cereal grains, and other processed and derived products, representing a significant risk to food safety and public health. This study presents the development and optimisation of a high-performance liquid chromatography method with fluorescence detection (HPLC-FLD) for the quantification of fumonisin B1 (FB1) and B2 (FB2) in various food matrices. In contrast with conventional protocols employing potassium phosphate buffers as the mobile phase, the proposed method utilises formic acid, offering enhanced compatibility with liquid chromatography systems. An automated online precolumn derivatisation with o-phthaldialdehyde (OPA) was optimised through experimental design and response surface methodology, enabling baseline separation of FB1 and FB2 derivatives in less than 20 min. The method demonstrated high sensitivity, with limits of detection of 0.006 µg mL⁻¹ for FB1 and 0.012 µg mL⁻¹ for FB2, and excellent repeatability (intraday RSD values of 0.85% and 0.83%, respectively). Several solid-phase extraction (SPE) strategies were evaluated to enhance sample clean-up using a variety of food samples, including dried figs, raisins, dates, corn, cornmeal, wheat flour, and rice. FumoniStar Inmunoaffinity columns were the only clean-up method that provided optimal recoveries (70–120%) across all tested food matrices. However, the MultiSep™ 211 column yielded good recoveries for both fumonisins in dried figs and raisins. Additionally, the C18 cartridge achieved acceptable recoveries for both fumonisins in dried figs and wheat flour. Full article

Plant roots influence various soil physical properties by altering the soil structure and pore configuration; however, a detailed understanding of these effects remains limited. In this study, we applied a relatively simple approach for segmenting plant roots and soil constituents using X-ray computed tomography (CT) images to evaluate root-induced changes in soil structure. The method combines manual initialization with a layer-wise automated region-growing approach, enabling the extraction of the root systems of soybean, Italian ryegrass, and Guinea grass. The method utilizes freely available software with a simple interface and does not require advanced image analysis skills, making it accessible to a wide range of researchers. The soil particles, pore water, and pore air were segmented using a Kriging-based thresholding technique. The segmented four-phase images allowed for the quantification of the volume fractions of soil constituents, pore size distributions, and coordination numbers. Furthermore, by separating the rhizosphere and bulk soil, we found that the root presence significantly reduced solid fractions and increased water content, particularly in the upper soil layers. Macropores and fine pores were observed near the roots, highlighting the complex structural impacts of root growth. While further validation is needed to assess the method’s applicability across different soil types and imaging conditions, it provides a practical basis for visualizing and quantifying root–soil interactions, and could contribute to advancing our understanding of how plant roots influence key soil hydraulic and thermal properties. Full article

Heterocyclic aromatic amines (HAAs), known for their mutagenic and carcinogenic potential, are formed during the heating of protein-rich food items. Detecting HAAs swiftly and accurately poses challenges due to complex food matrices and low HAA concentrations. In this study, a simple and efficient magnetic solid-phase extraction (MSPE) strategy was developed for the simultaneous isolation and enrichment of three HAAs such as 2-amino-3,4,8-trimethylimidazo [4,5-f]quinoxaline (4,8-DiMeIQx), 2-amino-3,8-dimethylimidazo [4,5-f]quinoxaline (MeIQx), and 2-amino-3-methylimidazo [4,5-f]quinoline (IQ) in processed meats, employing the magnetic covalent organic framework Fe₃O₄@MOF-545-AMSA as an adsorbent. It was synthesized via a solvothermal method, with Fe₃O₄ as the magnetic core. Its building blocks are as follows: zirconium (Zr) as the coordination metal ion, tetrakis(4-carboxyphenyl)porphyrin and benzoic acid as organic ligands, and aminomethanesulfonic acid (AMSA). This composite captures targeted HAAs efficiently by exploiting the unique porous MOF-545-AMSA structure, specific metal–ligand coordination, and AMSA’s amino and sulfonic acid groups. The quantification of HAAs was achieved through the combination of Ultra-Performance Liquid Chromatography–Tandem Mass Spectrometry (UPLC-MS/MS) and MSPE, demonstrating satisfactory linearity (R² ≥ 0.9917), high recovery rates (83.7–111.0%), and low detection limits (0.1–1.0 μg/kg). Moreover, an automated high-throughput detection system was developed using MSPE to assess the presence of HAAs in meat products. Full article

Background: Actinium-225 (²²⁵Ac) has gained interest in nuclear medicine for use in targeted alpha therapy (TAT) for the treatment of cancer. However, the number of suitable chelators for the stable complexation of ²²⁵Ac³⁺ is limited. The promising physical properties of ²²⁵Ac result in an increased demand for the radioisotope that is not matched by its current supply. To expand the possibilities for the development of ²²⁵Ac-based TAT therapeutics, a new hydroxamate-based chelator, DFO*¹², is described. We report the DFT-guided design of dodecadentate DFO*¹² and an efficient and convenient automated solid-phase synthesis for its preparation. To address the limited availability of ²²⁵Ac, a small-scale ²²⁹Th/²²⁵Ac generator was constructed in-house to provide [²²⁵Ac]AcCl₃ for research. Methods: DFT calculations were performed in ORCA 5.0.1 using the BP86 functional with empirical dispersion correction D3 and Becke–Johnson damping (D3BJ). The monomer synthesis over three steps enabled the solid-phase synthesis of DFO*¹². The small-scale ²²⁹Th/²²⁵Ac generator was realized by extracting ²²⁹Th from aged ²³³U material. Radiolabeling of DFO*¹² with ²²⁵Ac was performed in 1 M TRIS pH 8.5 or 1.5 M NaOAc pH 4.5 for 30 min at 37 °C. Results: DFT calculations directed the design of a dodecadentate chelator. The automated synthesis of the chelator DFO*¹² and the development of a small-scale ²²⁹Th/²²⁵Ac generator allowed for the radiolabeling of DFO*¹² with ²²⁵Ac quantitatively at 37 °C within 30 min. The complex [²²⁵Ac]Ac-DFO*¹² indicated good stability in different media for 20 h. Conclusions: The novel hydroxamate-based dodecadentate chelator DFO*¹², together with the developed ²²⁹Th/²²⁵Ac generator, provide new opportunities for ²²⁵Ac research for future radiopharmaceutical development and applications in TAT. Full article

Miniaturized solid-based approaches have added an eco-friendly dimension to analytical procedures, establishing themselves as promising strategies for a wide range of applications. Among these, microextraction by packed sorbent (MEPS) stands out due to its ability to facilitate efficient sample interaction with a densely packed sorb ent phase within the microextraction system. MEPS offers several advantages, including preconcentration capabilities and the use of minimal sample and solvent volumes, making it an appealing choice for modern analytical workflows. Since the extraction efficiency is largely dictated by the sorbent phase, recent advancements in sorbent design have garnered considerable attention in the field of sample preparation. Innovations in sorbent phases have not only enhanced the MEPS efficiency but also enabled the development of semi- and fully automated systems, paving the way for high-throughput methodologies. These advancements have elevated MEPS beyond traditional offline miniaturized sample preparation methods, offering new opportunities for streamlined and scalable analyses. Therefore, this study provides a comprehensive overview of novel sorbent phases used in MEPS, with a particular focus on both bio-based and synthetic materials. Furthermore, it explores the semi- and fully automated aspects of MEPS, highlighting current trends, technological advancements, and future directions in this rapidly evolving field. Full article

Due to the structural diversity of flavonoids in functional plant foods and the inherent limitations of existing techniques, it is important to develop a simple and green (environmentally friendly) method of extracting flavonoids from plant foods. In this study, a method involving solvent extraction followed by automated solid-phase extraction was developed for extracting flavonoids from Lonicerae japonicae flos (JYH) and Lonicerae flos (SYH), both of which are widely used functional plant-based foods in Asian countries. For the optimisation of the solvent extraction method, solvent concentration (0.0, 20.0, 40.0, 60.0, 80.0 and 100.0% (v/v) of ethanol–water solution), extraction temperature (40, 60 and 80 °C) and extraction time (15.0, 30.0, 60.0, 90.0 and 120.0 min) were evaluated via design of experiment after screening. For solid-phase extraction, five cartridges (Strata-X, InertSep RP-2, InertSep RP-C18, Bond Elut-ENV, Oasis Prime HLB) were evaluated and different elution steps were optimised to obtain high recoveries (79.69–140.67%) for eight target flavonoids, including rutin, isoquercetin and luteolin. Antioxidant capacity assays revealed that JYH samples demonstrated superior antioxidant potential compared to SYH. The optimised extraction method provides a valuable tool for industrial-scale flavonoid production. Full article

Adenine nucleotides (ANs)—adenosine 5′-triphosphate (ATP), adenosine 5′-diphosphate (ADP), and adenosine 5′-monophosphate (AMP)—are essential for energy transfer and the supply of countless processes within cellular metabolism. Their concentrations can be expressed as adenylate energy charge (AEC), a measure of cellular metabolic energy that directly correlates with the homeostasis of the organism. AEC index has broad diagnostic potential, as reduced ATP levels are associated to various conditions, such as inflammatory diseases, metabolic disorders, and cancer. We introduce a novel methodology for rapid isolation, purification, and quantification of ANs from a single drop of capillary blood. Of all the stationary phases tested, activated carbon proved to be the most efficient for the purification of adenine nucleotides, using an automated micro-solid phase extraction (µ-SPE) platform. An optimized µ-SPE method, coupled with RP-HPLC and a run time of 30 min, provides a reliable analytical framework for adenine nucleotide analysis of diverse biological samples. AN concentrations measured in capillary blood samples were 1393.1 µM, 254.8 µM, and 76.9 µM for ATP, ADP, and AMP molecules aligning with values reported in the literature. Overall, this study presents a streamlined and precise approach for analyzing ANs from microliters of blood, offering promising applications in clinical diagnostics. Full article

With ever-developing analytical capabilities, the protection of the dairy chain from contamination by residues of veterinary drugs is improving. Legislative requirements are an inherent part of this process. Of antibiotics in dairy farming, representatives of the beta-lactams, tetracyclines, sulfonamides, (fluoro)quinolones, aminoglycosides, or polypeptide antibiotics are the most widely used. Due to the typically low levels of antibiotic residues in milk, mass spectrometry is the most commonly used detection technique. However, the interference of the sample matrix is one of its main limiting factors, and therefore, it needs to be eliminated. In the first step, the lipid fraction is removed and proteins are precipitated, followed by solid-phase or liquid–liquid extraction. The current trends include the reduction in the consumption of organic solvents (to reduce occupational hazards and burden to the environment) and automation, eliminating the influence of human error and optimizing the workflow. These trends lead to the development of new microextraction and automated techniques as well as the use of new sorbents and/or (green) solvents of natural origin. To capture the latest developments in the field and the relatively recent aforementioned trends, this review focuses on papers investigating antimicrobial residues in milk that were published between 2015 and 2024, providing an overview of emerging techniques applicable to antibiotic residue detection in milk samples. Full article

The coupling of Solid-Phase Microextraction (SPME) technology with gas chromatography (GC) has a well-established and successful history. Traditionally, SPME fibers have been the most popular form thanks to their versatility and the ease with which they can be fully automated. However, alternative geometries for SPME have been developed over the years, beginning with Stir Bar Sorptive Extraction (SBSE) and later evolving into Thin-Film SPME (TF-SPME) devices. Each of these formats offers distinct advantages and disadvantages, which are explored in this study. The primary objective of this study was to comprehensively compare available forms of SPME devices, with a special focus on the advantages of TF-SPME, a novel microextraction method particularly suited for the analysis of odorants in food. The study involved analyzing a standard mixture of 11 key food odorants, representing a range of polarities, to evaluate the efficiency of TF-SPME devices in terms of the number of analytes extracted. Furthermore, four types of TF-SPME devices were compared against each other in both standard mixtures and actual food samples. The final stage of the study employed GCxGC-ToFMS analysis to showcase the potential of the most efficient HLB-TF-SPME device in the non-targeted analysis of complex samples, exemplified by unfiltered wheat beer. This analysis demonstrated the significant capability of HLB-TF-SPME in capturing and identifying a wide range of volatile compounds in complex matrices. Full article

Quinolone antibiotics (QNs) contamination in the aquatic environment is a global public health issue considering their resistance and mobility. In this study, a simple, efficient, and sensitive method was developed for the accurate quantification of fifteen QNs in water using automated disk-based solid-phase extraction (SPE) coupled with ultra-performance liquid chromatography–tandem mass spectrometry (UPLC–MS/MS). By utilizing a 3M SDB-XC disk to enrich QNs from a 1000 mL water sample, the detection limits were improved to 0.008–0.055 ng/L due to the satisfactory enrichment factors of 897−1136, but only requiring about 60 min per six samples. The linearity of the method ranged from 0.05 to 100 μg/L for the 15 QNs, with correlation coefficients of 0.9992–0.9999, and the recoveries were in the range of 81–114%, with relative standard deviations of 0.2–13.3% (n = 6). The developed method was applicable for the quantification of trace QNs at low ng/L levels in drinking and environmental waters. The results showed that no QNs were detected in tap water, while three and four QNs were detected in the river water of Zhoushan and the seawater of Daiquyang and Yueqing Bay, East China, respectively, with a total concentration of 1.600–8.511 ng/L and 1.651–16.421 ng/L, respectively. Among the detected QNs, ofloxacin (OFL) was the predominant compound in river water, while enrofloxacin (ENR) was predominant in seawater. The risk quotient (RQ) results revealed that QNs posed a low risk to crustaceans and fish, but a low-to-medium risk to algae, and OFL presented the main ecological risk factor in river water, while ENR and CIP in seawater. Overall, the proposed automated disk-based SPE–UPLC–MS/MS method is highly efficient and sensitive, making it suitable for routine analysis of QNs in drinking and environmental waters. Full article

Despite advancements in the sensitivity and performance of analytical instruments, sample preparation remains a bottleneck in the analytical process. Currently, solid-phase extraction is more widely used than traditional organic solvent extraction due to its ease of use and lower solvent requirements. Moreover, various microextraction techniques such as micro solid-phase extraction, dispersive micro solid-phase extraction, solid-phase microextraction, stir bar sorptive extraction, liquid-phase microextraction, and magnetic bead extraction have been developed to minimize sample size, reduce solvent usage, and enable automation. Among these, in-tube solid-phase microextraction (IT-SPME) using capillaries as extraction devices has gained attention as an advanced “green extraction technique” that combines miniaturization, on-line automation, and reduced solvent consumption. Capillary tubes in IT-SPME are categorized into configurations: inner-wall-coated, particle-packed, fiber-packed, and rod monolith, operating either in a draw/eject system or a flow-through system. Additionally, the developments of novel adsorbents such as monoliths, ionic liquids, restricted-access materials, molecularly imprinted polymers (MIPs), graphene, carbon nanotubes, inorganic nanoparticles, and organometallic frameworks have improved extraction efficiency and selectivity. MIPs, in particular, are stable, custom-made polymers with molecular recognition capabilities formed during synthesis, making them exceptional “smart adsorbents” for selective sample preparation. The MIP fabrication process involves three main stages: pre-arrangement for recognition capability, polymerization, and template removal. After forming the template-monomer complex, polymerization creates a polymer network where the template molecules are anchored, and the final step involves removing the template to produce an MIP with cavities complementary to the template molecules. This review is the first paper to focus on advanced MIP-based IT-SPME, which integrates the selectivity of MIPs into efficient IT-SPME, and summarizes its recent developments and applications. Full article