| 1. |
- Akhtar, Ahmad Saleem, et al.
(författare)
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A portable and low-cost centrifugal microfluidic platform for multiplexed colorimetric detection of protein biomarkers
- 2023
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Ingår i: Analytica Chimica Acta. - : Elsevier BV. - 0003-2670 .- 1873-4324. ; 1245
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Tidskriftsartikel (refereegranskat)abstract
- Cytokines play a very important role in our immune system by acting as mediators to put up a coordinated defense against foreign elements in our body. Elevated levels of cytokines in the body can signal to an ongoing response of the immune system to some abnormality. Thus, the quantification of a panel of cytokines can provide valuable information regarding the diagnosis of specific diseases and state of overall health of an individual. Conventional Enzyme Linked Immunosorbent Assay (ELISA) is the gold-standard for quantification of cytokines, however the need for trained personnel and expensive equipment limits its application to centralized laboratories only. In this context, there is a lack of simple, low-cost and portable devices which can allow for quantification of panels of cytokines at point-of-care and/or resource limited settings.Here, we report the development of a versatile, low-cost and portable bead-based centrifugal microfluidic platform allowing for multiplexed detection of cytokines with minimal hands-on time and an integrated colorimetric signal readout without the need for any external equipment. As a model, multiplexed colorimetric quantification of three target cytokines i.e., Tumor necrosis factor alpha (TNF-α), Interferon gamma (IFN-γ) and Interleukin-2 (IL-2) was achieved in less than 30 min with limits of detection in ng/mL range. The developed platform was further evaluated using spiked-in plasma samples to test for matrix interference. The ease of use, low-cost and portability of the developed platform highlight its potential to serve as a sample-to-answer solution for detection of cytokine panels in resource limited settings.
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| 2. |
- Banan, Kamran, et al.
(författare)
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Nano-sized magnetic core-shell and bulk molecularly imprinted polymers for selective extraction of amiodarone from human plasma
- 2022
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Ingår i: Analytica Chimica Acta. - : Elsevier. - 0003-2670 .- 1873-4324. ; 1198
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Tidskriftsartikel (refereegranskat)abstract
- Bulk and magnetic core-shell Molecularly Imprinted Polymers (MMIPs) have been introduced and compared to extract and determine amiodarone from a complex matrix, i.e., plasma, due to the importance of Therapeutic Drug Monitoring (TDM). Polymer synthesis was confirmed by FTIR, AFM, TGA, DLS, VSM, TEM, and the adsorption studies such as capacity, isothermal models, selectivity, and regeneration were performed to evaluate and compare polymer efficiency in extraction and separation of amiodarone from sample solutions and human plasma. Both nano-sized and bulk polymers successfully extracted the target molecule at the low therapeutic ranges and the overdose concentrations (recoveries of 98.38%-102.70%). The maximum adsorption capacity of the MMIPs was 42.5 mu g/mg compared with 2.6 mu g/mg for bulk polymers. The imprinting factors of the polymers were 15.12 and 6.84 for MMIPs and bulk, respectively. MMIPs and bulk polymers presented 4.68 and 1.66 selectivity factors, respectively, towards amiodarone compared with lidocaine. LOD, LOQ and enrichment factor in human plasma were 0.09, 0.28 mu g mL(-1), and 10 respectively. Recoveries of therapeutic concentration from plasma were 91.38 and 97.33% for bulk and MMIPs, respectively. MMIPs as an adsorbent in amiodarone extraction from plasma offered reduced necessary sample amount, less adsorbent consumption, reduced pretreatment time, and reduced elution solvent waste while yielding higher extraction recovery and more specificity for the target compared with the bulk polymer. Bulk polymers have a more straightforward synthesis procedure due to fewer synthesis steps and fewer variables, and Molecularly Imprinted Polymer Solid-phase Extraction (MIP-SPE) has already been introduced commercially. MMIPs prevail on a small scale, and in the context of a simple extraction, separation, or concentration in large-scale bioanalysis, efforts towards optimization and development of MMIPs can unearth tremendous opportunities for green chemistry principles.
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| 3. |
- Celma Tirado, Alberto
(författare)
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Effects of structural characteristics of (un)conjugated steroid metabolites in their collision cross section value
- 2023
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Ingår i: Analytica Chimica Acta. - : Elsevier BV. - 0003-2670 .- 1873-4324. ; 1254
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Tidskriftsartikel (refereegranskat)abstract
- In this work, the collision cross section (CCS) value of 103 steroids (including unconjugated metabolites and phase II metabolites conjugated with sulfate and glucuronide groups) was determined by liquid chromatography coupled to traveling wave ion mobility spectrometry (LC-TWIMS). A time of flight (QTOF) mass analyzer was used to perform the analytes determination at high-resolution mass spectrometry. An electrospray ionization source (ESI) was used to generate [M+H]+, [M + NH4]+ and/or [M − H]- ions. High reproducibility was observed for the CCS determination in both urine and standard solutions, obtaining RSD lower than 0.3% and 0.5% in all cases respectively. CCS determination in matrix was in accordance with the CCS measured in standards solution showing deviations below 2%. In general, CCS values were directly correlated with the ion mass and allowed differentiating between glucuronides, sulfates and free steroids although differences among steroids of the same group were less significant. However, more specific information was obtained for phase II metabolites observing differences in the CCS value of isomeric pairs concerning the conjugation position or the α/β configuration, which could be useful in the structural elucidation of new steroid metabolites in the anti-doping field. Finally, the potential of IMS reducing interferences from the sample matrix was also tested for the analysis of a glucuronide metabolite of bolasterone (5β-androstan-7α,17α-dimethyl-3α,17β-diol-3-glucuronide) in urine samples.
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| 4. |
- Costalunga, Riccardo, et al.
(författare)
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Sodium adduct formation with graph-based machine learning can aid structural elucidation in non-targeted LC/ESI/HRMS
- 2022
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Ingår i: Analytica Chimica Acta. - : Elsevier BV. - 0003-2670 .- 1873-4324. ; 1204
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Tidskriftsartikel (refereegranskat)abstract
- Non-targeted screening with LC/ESI/HRMS aims to identify the structure of the detected compounds using their retention time, exact mass, and fragmentation pattern. Challenges remain in differentiating between isomeric compounds. One untapped possibility to facilitate identification of isomers relies on different ionic species formed in electrospray. In positive ESI mode, both protonated molecules and adducts can be formed; however, not all isomeric structures form the same ionic species. The complicated mechanism of adduct formation has hindered the use of this molecular characteristic in the structural elucidation in non-targeted screening. Here, we have studied the adduct formation for 94 small molecules with ion mobility spectra and compared collision cross-sections of the respective ions. Based on the results we developed a fast support vector machine classifier with polynomial kernels for accurately predicting the sodium adduct formation in ESI/HRMS. The model is trained on five independent data sets from different laboratories and uses the graph-based connectivity of functional groups and PubChem fingerprints to predict the sodium adduct formation in ESI/HRMS. The validation of the model showed an accuracy of 74.7% (balanced accuracy 70.0%) on a dataset from an independent laboratory, which was not used in the training of the model. Lastly, we applied the classification algorithm to the SusDat database by NORMAN network to evaluate the proportion of isomeric compounds that could be distinguished based on predicted sodium adduct formation. It was observed that sodium adduct formation probability can provide additional selectivity for about one quarter of the exact masses and, therefore, shows practical utility for structural assignment in non-targeted screening.
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| 5. |
- De Samber, Björn, et al.
(författare)
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Effect of sample preparation techniques upon single cell chemical imaging : A practical comparison between synchrotron radiation based X-ray fluorescence (SR-XRF) and Nanoscopic Secondary Ion Mass Spectrometry (nano-SIMS)
- 2020
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Ingår i: Analytica Chimica Acta. - : Elsevier. - 0003-2670 .- 1873-4324. ; 1106, s. 22-32
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Tidskriftsartikel (refereegranskat)abstract
- Analytical capabilities of Nanoscopic Secondary Ion Mass Spectrometry (nano-SIMS) and Synchrotron Radiation based X-ray Fluorescence (SR nano-XRF) techniques were compared for nanochemical imaging of polymorphonuclear human neutrophils (PMNs). PMNs were high pressure frozen (HPF), cryosubstituted, embedded in Spurr's resin and cut in thin sections (500 nm and 2 mu m for both techniques resp.) Nano-SIMS enabled nanoscale mapping of isotopes of C, N, O, P and S, while SR based nano-XRF enabled trace level imaging of metals like Ca, Mn, Fe, Ni, Cu and Zn at a resolution of approx. 50 nm. The obtained elemental distributions were compared with those of whole, cryofrozen PMNs measured at the newly developed ID16A nano-imaging beamline at the European Synchrotron Radiation Facility (ESRF) in Grenoble, France. Similarities were observed for elements more tightly bound to the cell structure such as phosphorus and sulphur, while differences for mobile ions such as chlorine and potassium were more pronounced. Due to the observed elemental redistribution of mobile ions such as potassium and chlorine, elemental analysis of high pressure frozen (HPF), cryo-substituted and imbedded cells should be interpreted critically. Although decreasing analytical sensitivity occurs due to the presence of ice, analysis of cryofrozen cells - close to their native state - remains the golden standard. In general, we found nanoscale secondary ion mass spectrometry (nano-SIMS) and synchrotron radiation based nanoscopic X-ray fluorescence (SR nano-XRF) to be two supplementary alternatives for nanochemical imaging of single cells at the nanoscale.
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| 6. |
- Gonzalez de Vega, Raquel, et al.
(författare)
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A multi-platform approach for the comprehensive analysis of per- and polyfluoroalkyl substances (PFAS) and fluorine mass balance in commercial ski wax products
- 2024
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Ingår i: Analytica Chimica Acta. - : Elsevier B.V.. - 0003-2670 .- 1873-4324. ; 1314
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Tidskriftsartikel (refereegranskat)abstract
- The unique properties of per- and polyfluoroalkyl substances (PFAS) have led to their extensive use in consumer products, including ski wax. Based on the risks associated with PFAS, and to align with PFAS regulations, the international ski federation (FIS) implemented a ban on products containing “C8 fluorocarbons/perfluorooctanoate (PFOA)” at all FIS events from the 2021/2022 season, leading manufactures to shift their formulations towards short-chain PFAS chemistries. To date, most studies characterising PFAS in ski waxes have measured a suite of individual substances using targeted analytical approaches. However, the fraction of total fluorine (TF) in the wax accounted for by these substances remains unclear. In this study, we sought to address this question by applying a multi-platform, fluorine mass balance approach to a total of 10 commercially available ski wax products. Analysis of TF by combustion ion chromatography (CIC) revealed concentrations of 1040–51700 μg F g−1 for the different fluorinated waxes. In comparison, extractable organic fluorine (EOF) determined in methanol extracts by CIC (and later confirmed by inductively-coupled plasma-mass spectrometry and 19F- nuclear magnetic resonance spectroscopy) ranged from 92 to 3160 μg g−1, accounting for only 3–8.8 % of total fluorine (TF). Further characterisation of extracts by cyclic ion mobility-mass spectrometry (IMS) revealed 15 individual PFAS with perfluoroalkyl carboxylic acid concentrations up to 33 μg F g−1, and 3 products exceeding the regulatory limit for PFOA (0.025 μg g−1) by a factor of up to 100. The sum of all PFAS accounted for only 0.01–1.0 % of EOF, implying a high percentage of unidentified PFAS, thus, pyrolysis gas chromatography-mass spectrometry was used to provide evidence of the nature of the non-extractable fluorine present in the ski wax products.
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| 7. |
- Huang, Ruihua, et al.
(författare)
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Star-shaped porous nitrogen-doped metal-organic framework carbon as an electrochemical platform for sensitive determination of Cd(II) in environmental and tobacco samples
- 2022
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Ingår i: Analytica Chimica Acta. - : Elsevier. - 0003-2670 .- 1873-4324. ; 1228
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Tidskriftsartikel (refereegranskat)abstract
- In this study, cetyltrimethylammonium bromide and zeolitic imidazolate framework-8 (ZIF-8) were first assembled via the chemical co-precipitation, and high-quality carbon-based metal-free nanomaterials were synthesized using a heat-treatment process. The internal and morphological characteristics of hexagonal Star ZIF-8 were investigated using scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The electrochemical sensor with a good response to Cd(II) was prepared via square-wave anodic stripping voltammetry (SWASV) with Star ZIF-8 nanomaterial-modified glassy carbon electrodes. The main parameters were adjusted to obtain the optimal stripping response and a wide linear range. Concurrently, under the calculation of SWASV, the sensitivity of Star ZIF-8-Nafion/GCE to Cd(II) was increased by five orders of magnitude (0.5–230 μg/L), and the determination level was even low to 0.48 μg/L. Based on the high anti-interference ability and stability of the sensor, the application potential of Star ZIF-8 carbon-based metal-free nanomaterials for the detection of trace Cd(II) in was confirmed.
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| 8. |
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| 9. |
- Krikstolaityte, Vida, et al.
(författare)
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Characterization of nano-layered solid-contact ion selective electrodes by simultaneous potentiometry and quartz crystal microbalance with dissipation.
- 2020
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Ingår i: Analytica Chimica Acta. - : Elsevier. - 0003-2670 .- 1873-4324. ; 1128, s. 19-30
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Tidskriftsartikel (refereegranskat)abstract
- Nano-layered solid-contact potassium-selective electrodes (K+-ISEs) were explored as model ion-selective electrodes for their practical use in clinical analysis. The ultra-thin ISEs ought to be manufactured in a highly reproducible manner, potentially making them suitable for mass production. Thus, their development is pivotal towards miniaturised sensors with simplified conditioning/calibration protocols for point-of-care diagnostics. To study nano-layered ISEs, the ultra-thin nature of ISEs for the first time enabled to combine potentiometry-quartz crystal microbalance with dissipation (QCM-D) to obtain value-added information on the ISE potentiometric response regarding their physical state such as mass/thickness/viscoelastic properties/structural homogeneity. Specifically, the studies were focused on real-time observations of the ISE potentiometric response in relation to changes of their physicochemical properties during the ISE preparation (conditioning) and operation (including biofouling conditions) to identify the occurring processes that may accordingly be critical for potential instability of the ISEs, impeding their practical application. The K+-ISEs were prepared on a QCM-D gold sensor by electrodepositing poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate) layer serving as an ion-to-electron transducer subsequently covered by a spin-coated poly(vinyl chloride) based K+-ion selective membrane (K+-ISM). The studies demonstrated that the performance of the nano-layered design of K+-ISEs is detrimentally affected by such processes as water layer formation accordingly causing the instability of the electrode potential. The changes in the ISE physical state such mass/viscoelastic properties associated with water layer formation and origin of the potential instability was already observed at the ISE conditioning stage. The potential instability of nano-layered ISEs limits their practical applicability, indicating the need of new solutions in designing ISEs, for instance, exploiting new water-resistant materials and modifying preparation protocols.
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| 10. |
- Li, Rongbin, et al.
(författare)
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Nonlinearity in mass spectrometry for quantitative multi-component gas analysis in reaction processes
- 2022
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Ingår i: Analytica Chimica Acta. - : Elsevier BV. - 0003-2670 .- 1873-4324. ; 1194, s. 339412-
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Tidskriftsartikel (refereegranskat)abstract
- Quantitative mass spectrometry analysis for multi-component gas phase reaction processes is a typical multi-input and multi-output (MIMO) nonlinear problem. Conventional calibration and analytical methods that are based on the common hypothesis of linearity of the detected signal and gas parameters, could result in misjudgment of the reaction mechanism and inaccuracy in the determination of the reaction kinetics. In the present work, theoretical derivations based on equivalent characteristic spectrum analysis (ECSA (R)), discrete mode experiments and continuous mode experiments were performed, and the nonlinearity of mass spectrometry was confirmed. It is only possible to determine the physical parameters such as flow rate and/or concentrations of gases by properly handling the nonlinearity of mass spectrometry. In such case comprehensive reaction mechanisms and even the kinetics of the process can be accurately characterized. Well-handled nonlinear mass spectrometry analysis ensures a reliable and highly accurate identification for the multi-component gas phase reaction processes, and ensures high signal-to-noise ratio for detecting the small-flow gases at a wide range of carrier gas flow.
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