Ion Mobility Research Articles

Rapid separation of bile acid isomers via ion mobility mass spectrometry by complexing with spiramycin.

Bile acid (BA) is one of the main active components of bile and has multiple isomers, the structure or content of its isomers often changes due to diseases and other health problems; thus, the accurate detection of BA isomers is very important. In this study, two groups of BA isomers of glycine-conjugated BAs and taurine-conjugated BAs were simultaneously separated and quantitatively analyzed by ion mobility mass spectrometry (IM-MS). Especially, baseline mobility separation between the isomers was achieved by the formation of binary complexes via simple interaction with spiramycin (SPM), for which a separation resolution (Rp-p) of 1.96was reached. Moreover, BA isomers were quantitatively analyzed, and the limit of detection (LOD) of absolute quantification for TCDCA/TUDCA and GUDCA/GCDCA/GHDCA was 0.514 and 0.611ng∙mL-1, respectively; the LODs for molar ratio ranges of relative quantification for TCDCA/TUDCA, GUDCA/GHDCA, and GCDCA/GHDCA were 1:18-30:1, 1:18-21:1, and 1:19-21:1, respectively. Additionally, BA isomers analyzed in pig bile powder and bear bile powder were measured, which were in good consistency with those labeled, revealing the differences in BA composition and content between the two powders. Finally, BA detection and recovery analyses were performed on serum samples, with a recovery rate of ≥73.69%, RSD of ≤6.8%, and SR (standard deviation of recoveries, the degree of difference between measured values and average recovery) of ≤1.27. Due to the simple, rapid, and lack of need for complex sample preparation and chromatographic separation, the proposed method can be an effective method for BA detection in practical samples.

Mechanical and Ionic Characterization for Organic Semiconductor-Incorporated Perovskites for Stable 2D/3D Heterostructure Perovskite Solar Cells.

Hybrid metal halide perovskite (MHP) materials, while being promising for photovoltaic technology, also encounter challenges related to material stability. Combining 2D MHPs with 3D MHPs offers a viable solution, yet there is a gap in the understanding of the stability among various 2D materials. The mechanical, ionic, and environmental stability of various 2D MHP ligands are reported, and an improvement with the use of a quater-thiophene-based organic cation (4TmI) that forms an organic-semiconductor incorporated MHP structure is demonstrated. It is shown that the best balance of mechanical robustness, environmental stability, ion activation energy, and reduced mobile ion concentration under accelerated aging is achieved with the usage of 4TmI. It is believed that by addressing mechanical and ion-based degradation modes using this built-in barrier concept with a material system that also shows improvements in charge extraction and device performance, MHP solar devices can be designed for both reliability and efficiency.

High-volume recycled glass cementitious and geopolymer composites incorporating graphene oxide

This study presents the development of high-volume recycled glass construction materials using recycled glass aggregate (RGA) as a 100 % sand replacement, recycled glass powder (RGP) as 40 wt% of the binder, and 0.1 wt% graphene oxide (GO) as nano-reinforcement. The research investigates the individual and their combined effects on the engineering performance, reaction kinetics (using calorimetry, X-ray diffraction-XRD, Fourier Transform Infrared-FTIR and Thermogravimetric analysis-TGA), and microstructure (Scanning Electron Microscopy/ Energy Dispersive X-ray Spectroscopy-SEM/EDS) for both cementitious and geopolymer systems. The results indicate that while RGA reduces strength and exacerbates alkali-silica reaction (ASR), the presence of 40 wt% RGP significantly mitigates ASR despite a lower strength gain in both systems. Geopolymers exhibit significantly lower ASR expansion compared to cementitious matrices owing to their superior alkali-binding capacity and denser microstructure, which restricts water and alkali ion mobility. 0.1 wt% GO was found to accelerate geopolymerisation, enhancing the strength of geopolymer mixes, but it decreased compressive strength in cement-based mixes due to self-desiccation-induced micro-cracking under ambient curing condition. The study also highlights that cement and metasilicate, as well as slag, are the main contributors to cost and CO2 emissions in cementitious and geopolymer systems, respectively. Overall, geopolymers exhibit a significantly lower global warming potential (< 180 kg CO2-eq/m3) compared to cement-based mixes (> 365 kg CO2-eq/m3) with a comparable cost (190–230 AUD/m3). The results indicate the potential for sustainable construction applications using high volumes of recycled glass, incorporating over 70 % of the mixture by weight.

Blue energy conversion utilizing smart ionic nanotransistors

The use of concentration gradients across nanofluidic membranes for energy generation presents a novel and sustainable approach to power production. This study investigates the impact of ion nanotransistor configurations on ion transport and energy generation. Two types of cylindrical symmetrical nanotransistors, PNP and NPN, were tested. Using the finite element method, the Poisson-Nernst-Planck and Navier-Stokes equations were solved to evaluate how the configuration of soft layers, concentration ratios, and charge density influence energy output. Results show that the NPN configuration consistently outperforms the PNP setup in energy production, with energy generation ranging from 40pW to 56pW, compared to 35pW to 43pW for the PNP structure, when soft layer charge density increase from 25mol/m3 to 100mol/m3. The superior performance of the NPN arrangement is attributed to its higher electrostatic potential and enhanced ion mobility. These findings underscore the potential of NPN nanotransistor configurations for optimizing energy generation as well as water desalination in nanofluidic systems.

Phonon-Lithium Ion Interactions: A Case Study of LiM(SeO3)2 (M = Al, Ga, In, Sc, Y, and La).

Li ion diffusion is fundamentally a thermally activated ion hopping process. Recently, soft lattice, anharmonic phonon, and paddlewheel mechanism have been proposed to potentially benefit the ion transport, while the understanding of vibrational couplings of mobile ions and anions is still very limited but essential. Herein, we accessed the ionic conductivity, stability, and especially, lattice dynamics in LiM(SeO3)2 (M = Al, Ga, In, Sc, Y, and La) with two different types of oxygen anions within a LiO4 polyhedron, namely, edge-shared and corner-shared with MO6 polyhedra, the prototype of which, LiGa(SeO3)2, has been theoretically reported before with the similar structural features to NASICON and later experimentally synthesized with the room temperature conductivity ∼0.11 mS cm-1. It is interesting to note that LiM(SeO3)2 with a higher Li phonon band center shows higher Li conductivity, which is in contradiction to the conventional understanding of the importance for soft lattice to superionic conductors. The anharmonic and harmonic phonon interactions as well as the couplings between the vibration of the edge-bonded or corner-bonded anion in Li polyanions and the Li ion diffusion have been studied in detail. With transition metal M changing from La, Y, In, Ga, Al, and Sc, anharmonic phonons increase with reduced activation energy for Li diffusion. The phonon modes dominated by the edge-bonded oxygen anions contribute more to the migration of the Li ion than those dominated by the corner-bonded oxygen anions because of the greater atomic interaction between the Li ion and the edge-bonded anions. Thus, rather than the overall lattice softness, attention shall be given to reduce the frequency of the critical phonons contributing to Li ion diffusion as well as to increase the anharmonicity, i.e., through asymmetric Li polyhedra, for the design of Li ion superionic conductors for all-solid-state batteries.

B-282 Cost and Benefits of Utilization of Ion Mobility Mass Spectrometry Testing for Drugs of Abuse Compared to Immunoassay Screening in a Large Urban Hospital

Abstract Background Urine drugs of abuse testing (DOAU) in US hospitals are mainly orders from the emergency department performed by immunoassay screening. Testing can be relatively expensive, and results may suffer from non-idealities in sensitivity, specificity, and from panel limitations. A potential approach to these issues for immunoassays is instead to employ mass spectrometry (MS), where a large and flexible analyte list can be evaluated providing needed specificity and reducing send out costs for confirmatory testing. We compared results and cost impacts of a DOAU assay on a prototype, ion mobility mass spectrometry system to those obtained from an array of immunoassays offered as routine tests at a large urban hospital. Methods Immunoassay screen-positive and screen-negative urine samples were isolated from among those submitted for a DOAU panel (amphetamines, barbiturates, benzodiazepines, cannabis, cocaine, opiates, and methadone) or for additional single drug tests (fentanyl, oxycodone, phencyclidine, buprenorphine, propoxyphene). Sample aliquots (3 mL) were retrieved after not more than 5 days of refrigerated storage of the original sample and were subsequently frozen. These samples were then subjected to MS analysis using the prototype system where identification of 62 compounds was based on mass and ion mobility-derived Collision Cross Section (CCS). An established library of m/z, SLIMCCSHe, peak intensity, and peak width for each analyte was used, with acceptable method performance characteristics as based on applicable CLIA validation guidelines. The MS list included compounds covered by the immunoassay classes as well as additional drugs not expected to be positive among the immunoassays test results but of value for routine toxicological assessments. Results comparisons, utility of results, sample-to-result turnaround times, and overall financial implications were compared between the two workflows. Results Among immunoassay screen-negative samples, MS analysis showed additional positive results for metabolites of parent drugs as well as novel psychoactive substances and known adulterants in &amp;gt;10% of cases. Among the immunoassay screen-positive results, MS analysis confirmed immunoassay results (&amp;gt;90%) but picked up an additional positive component in over 15% of cases. Cost per complete patient result for the immunoassay was approximately $2.80 in comparison to an estimated cost of $5 for the MS method. Confirmation testing for positive immunoassay screen results (16% of all samples) would cost an additional $70 per sample, whereas the need for confirmation testing is eliminated for the MS method. Thus, use of the MS testing workflow would be superior to an immunoassay with reflex testing workflow while at the same time providing a clinically superior service of more diverse positive test results and elimination of often overlooked false negatives. Turnaround time between immunoassay (1h) and MS (50m) were judged to be similar. Conclusions The MS approach confirmed &amp;gt;90% of all immunoassay positive screen results. In addition, the MS method identified additional positive results not detected by the immunoassay despite an overall similar estimated time for sample to patient. Need for development of a user friendly, MS analyzer for use in hospitals is supported based on cost-effective and analytically superior tests for DOAU compared to screens performed using immunoassay panels.

Diffusion and mobility measurements for propane gas with a nanodosimetric detector

For the operation of nanodosimetric detectors with propane gas, it is essential to know the gas properties at room temperature, such as drift velocity, ion mobility, longitudinal and transversal diffusion coefficients. For propane gas there is only limited experimental data available for the ion mobility and transverse diffusion coefficients. In this work, the drift velocities and ion mobilities for propane were obtained over the reduced electric field range E/N from 24 to 212 Td (1 Td = 10−17 Vcm2) based on arrival time measurements. The reduced ion mobility K0 for propane was determined to be (0.71±0.09) cm2/Vs. The longitudinal diffusion coefficients were determined from the widths of the experimental arrival time spectra and found to be NDL = (3.7 ± 0.5)⋅1019 1/ms in the low field limit below 30 Td.The results presented in this work extend the range of available experimental data for propane, as well as introduce first experimental measurements of the longitudinal diffusion coefficient of propane.

Recent additions and access to a multidimensional lipidomic database containing liquid chromatography, ion mobility spectrometry, and tandem mass spectrometry information.

The importance of lipids in biology continues to grow with their recent linkages to more diseases and conditions, microbiome fluctuations, and environmental exposures. These associations have motivated researchers to evaluate lipidomic changes in numerous matrices and studies. Lipidomic analyses, however, present numerous challenges as lipid species have broad chemistries that require different extraction methods and instrumental analyses to evaluate and separate their many isomers and isobars. Increasing knowledge about different lipid characteristics is therefore crucial for improving their separation and identification. Here, we present a multidimensional database for lipids analyzed on a platform combining reversed-phase liquid chromatography, drift tube ion mobility spectrometry, collision-induced dissociation, and mass spectrometry (RPLC-DTIMS-CID-MS). This platform and the different separation characteristics it provides enables more confident lipid annotations when compared to traditional tandem mass spectrometry platforms, especially when analyzing highly isomeric molecules such as lipids. This database expands on our previous publication containing only human plasma and bronchoalveolar lavage fluid lipids and provides experimental RPLC retention times, IMS collision cross section (CCS) values, and m/z information for 877 unique lipids from additional biofluids and tissues. Specifically, the database contains 1504 precursor [M + H]+, [M + NH4]+, [M + Na]+, [M-H]-, [M-2H]2-, [M + HCOO]-, and [M + CH3COO]- ion species and their associated CID fragments which are commonly targeted in clinical and environmental studies, in addition to being present in the chloroform layer of Folch extractions. Furthermore, this multidimensional RPLC-DTIMS-CID-MS database spans 5 lipid categories (fatty acids, sterols, sphingolipids, glycerolipids, and glycerophospholipids) and 24 lipid classes. We have also created a webpage (tarheels.live/bakerlab/databases/) to enhance the accessibility of this resource which will be populated regularly with new lipids as we identify additional species and integrate novel standards.

Reliable resistive switching and synaptic simulation behaviors in ammonium polyphosphate-based memristor with non-inert Al electrode

Abstract Memristive devices that integrate storage and computing capabilities are highly promising candidates for artificial synapses in neuromorphic systems. However, achieving both cost-effectiveness and high-performance in memristors remains a substantial challenge. Ammonium polyphosphate (APP), an all-inorganic ionic polymer, has been utilized in the fabrication of memristive devices due to its distinctive poly-ionic properties and exceptional ion mobility. In this study, a two-terminal APP-based memristor with an Al/APP/ITO structure was fabricated. The experimental results revealed improved bipolar resistive switching behavior, characterized by lower operating voltages, enhanced endurance performance, and extended retention time. Detailed data fitting and chemical bonding analysis suggest that the physical mechanism underlying resistive switching involves a combination of interfacial Schottky barrier and conductive filaments. Furthermore, adjustable device conductance is achieved by applying consecutive positive and negative voltage sweeps. Various synaptic functions, including excitatory postsynaptic current, short-term paired-pulse facilitation, long-term potentiation /depression, and spike-timing-dependent plasticity, are effectively emulated. This study presents an effective approach to enhancing the memristive characteristics of APP-based devices and positions APP as a viable candidate for innovative neuromorphic architectures.

Tailoring optical and electrical properties of PVP-I2 complexes through gamma irradiation-induced structural defect Engineering for optoelectronic applications

This study investigates the complexation of iodine with polyvinylpyrrolidone (PVP) subjected to gamma irradiation at doses of 0, 10, 20, and 30 kGy. The complex formation involves I2 acting as a Lewis acid with electron-rich PVP as a Lewis base through a charge transfer mechanism. UV–visible spectroscopy revealed a red shift of the absorption peak at 337 nm for irradiated PVP-I2 samples, indicating stronger interactions between the triiodide ion (I3¯) and irradiated PVP. FTIR analysis confirmed the formation of new C≡N moieties arising from PVP-I2 complexation. The FT-Raman analysis revealed a new C≡N peak at 2360 cm−1 in irradiated PVP-I2 samples, with increasing intensity correlating to higher irradiation doses, indicating enhanced electron delocalization due to complex formation. XRD analysis showed that PVP-I2 samples irradiated at 0 and 10 kGy exhibited higher crystallinity than those irradiated at 20 and 30 kGy, suggesting that high-dose irradiation causes PVP radiolysis and ring opening. Dielectric measurements demonstrated enhanced polarizability and ionic conductivity of irradiated PVP-I2 films, related to structural disorder promoting charge dissociation and ion mobility. The direct bandgap decreased from 2.75 eV for unirradiated samples to 2.55 eV for samples irradiated at 30 kGy, indicating the creation of new optically active defect states. Urbach energy increased from 0.85 eV to 1.55 eV with increasing irradiation dose, confirming increased disorder in the PVP structure. These findings reveal that gamma irradiation significantly alters the optical and electrical properties of PVP-I2 films by creating defects and disrupting structure, offering new insights for tailoring these materials for optoelectronic applications.

An assessment of electroneutrality implementations for accurate electrochemical ion transport models

During the diffusion and migration of ions in electrolytes, the electrodynamic ion-ion interactions prevent charge separation despite different ionic mobilities, ultimately enforcing electroneutrality in the bulk electrolyte. To model ion transport accurately, a method to enforce electroneutrality must be implemented. In this study, four strategies to implement electroneutrality are discussed and evaluated. The ion distributions that result from a transport model with the different electroneutrality implementations are calculated, considering various electrolytes and sets of electrochemical parameters. The meaningfulness and applicability of each implementation are assessed through spatial charge accumulations, transference numbers, and experimental data from the literature. Combining the electrochemical ion transport models with the electroneutrality constraint for all ions is shown to result in an overdetermined system of equations if the driving forces are calculated under neglection of diffusion potentials. The often-reported model simplification of using the electroneutrality constraint to resolve the transport of one specific species explicitly results in non-physically correct mass transport. A practical approach to precisely describe the measured physicochemical ion movements is obtained by equilibrating spatial charges with the ion conduction for every time step in the ion transport model, which is reasonably applicable to multi-ion systems in three-dimensional frameworks. This comprehensive assessment aims to guide readers in selecting an appropriate electroneutrality implementation framework for ion transport models.

Low-pressure oxidation for improving interface properties and voltage instability of SiO2/4H-SiC MOS capacitor

The impact of high-temperature sub-atmospheric oxidation pressure on the interface properties of n-type 4H-SiC metal–oxide–semiconductor capacitors has been systematically investigated in this report. The bias temperature instability measurement was used to calculate the mobile ions and near-interface trap density that led to device instability at high temperatures. The density of near interface traps decreased from 88.3 × 1011 cm−2 to 10.2 × 1011 cm−2 when the growth pressure of SiO2 was reduced from 1 atm to 0.1 atm, while the mobile ions density decreased from 83.5 × 1011 to 4.18 × 1011 cm−2. The results show that SiO2 growing under lower oxidation pressure has better interfacial quality. The underlying mechanism was explored by secondary ion mass spectrometry (SIMS) and x-ray photoelectron spectroscopy (XPS). It is speculated that the SiO2/SiC interface was reconstructed under low-pressure oxidation: the excess Si-related defects near the interface, such as SiOxCy, were released while O atoms were accumulated to promote a complete oxidation reaction, thereby effectively reducing the number of defects in the SiO2 film and improving device performance.

Diethylenetriaminepentaacetic Acid-based Conducting Solid Polymer Electrolytes Impede Lithium Dendrites and Impart Antioxidant Capacity in Lithium-Ion Batteries.

In the development of lithium-ion batteries (LIBs), cheaper and safer solid polymer electrolytes are expected to replace combustible organic liquid electrolytes to meet the larger market demand. However, low ionic conductivity and inadequate cycling stability impede their commercial viability. Herein, a novel flexible conducting solid polymer electrolytes (CSPEs) based on polyvinyl alcohol (PVA) and ion-polarized diethylenetriaminepentaacetic acid (P-DETP) is developed for the first time and applied in LIBs. PVA and P-DETP form a compact polymer network through hydrogen bonding, enhancing the thermomechanical stability of CSPE while restricting the migration of larger anions. Furthermore, density functional theory calculations confirm that P-DETP can facilitate the dissociation of Li+-TFSI- via electrostatic attraction, resulting in increased mobility of lithium ions. Additionally, P-DETP contributes to the formation of a stable electrode-electrolyte interface layer, effectively suppressing the growth of lithium dendrites and improving antioxidant capacity. These synergistic effects enable CSPE to exhibit remarkable properties including high ionic conductivity (2.8 × 10-4 S cm-1), elevated electrochemical potential (5.1V), and excellent lithium transference number (0.869). Notably, the P-DETP/LiTFSI CSPE demonstrates stable performance not only in LiFePO4 batteries but also adapts to high-nickel ternary LiNi0.88Co0.06Mn0.06O2 cathode, highlighting its immense potential for application in high energy density LIBs.

High-performance ZnO:CuO composite-based fiber-shaped electrode for non-enzymatic glucose sensing in biological fluids

The growing diabetes epidemic necessitates new glucose sensors, as traditional enzyme-based and planar electrodes face limitations in environmental stability and seamless integration into wearable technology. This research tackles these issues by designing a flexible, enzyme-free glucose sensor utilizing a co-deposited ZnO:CuO (CZ) composite on PET monofilament. This approach improves the tensile strength (55 mm at 2.7 kg.f) and electrical conductance (0.32 S), of the Ni-coated PET fiber, resulting in a strong and reliable sensing platform. The electrode's enlarged electrochemical surface area (0.11 cm2), offer a high density of active sites for glucose interaction, and the synergistic interface significantly enhances both ion and charge mobility. This results in exceptional sensitivity (35.05 mA.cm−2.mM−1), a rapid response (24 s), and a low detection limit (0.15 mM). Durability tests demonstrate that the sensor retains 80% of its sensitivity after 500 bending cycles, making it well-suited for wearable applications. Furthermore, the sensor accurately detects glucose in biological samples, such as saliva, highlighting its potential for non-invasive, real-time glucose monitoring in wearable healthcare systems.

Ion transport properties and performance of gellan gum based composite polymer membrane electrolytes in proton battery and PEMFC applications

Biopolymer Gellan gum (GG) incorporated with ammonium iodide (NH₄I) salts and inorganic filler nano-TiO2 improved the ion transport facility in the salt-polymer matrix. The crystalline/amorphous nature of the membranes and the presence of n-TiO2 are evident from XRD analysis. The vibration modes corresponding to the characteristic functional groups and bonding interactions within the polymer matrix and incorporated filler materials present in the as-prepared membranes were analyzed using FTIR technique respectively. The ion transport parameters such as ionic conductivity (σ), diffusion coefficient (D), and mobility (μ), were studied using Ac impedance, transference number measurement, and FTIR deconvolution. The biopolymer membrane with the composition, 1 g GG: 0.3 M.wt% of NH4I (GGAI-3) shows the highest ionic conductivity of 2.65 ± 0.03×10−3 S/cm and on addition of 0.1 M.wt% of n-TiO2 (GGAIT-1) the increase in ionic conductivity of 4.07 ± 0.02×10−2 S/cm was observed. The H¹NMR studies help in understanding the mobility of charge carriers upon their chemical shifts. The glass transition temperature values of the as-prepared membranes were determined using DSC studies. The morphological change on the surface of the GG polymer membrane due to the addition of NH4I and n-TiO2 were analyzed using the SEM technique. The thermal, mechanical, and chemical stability of the highest ion-conducting biopolymer and composite polymer membranes were assessed using TGA, mechanical stability tests, and chemical stability tests. The IEC test exhibits the number of exchangeable ions in the polymer matrix. Utilizing the GGAI-3 and GGAIT-1 membranes as electrolytes, proton batteries were constructed and observed to have the pseudocapacitive behaviour; as the electrodes experience surface limited redox reaction at the electrode-electrolyte interface. The PEMFC cell using the GGAI- 3 and GGAIT-1 as proton exchange membrane exhibits the OCV of 646 mV and 682 mV respectively. Their performances were analyzed using the I-V polarization curve resulted with the power density of 0.14 mW/cm2and 0.34 mW/cm2 respectively.

Optimization of field asymmetric ion mobility spectrometry-based assessment of Aphanomyces root rot in pea

When plants are infected with pathogens, disease response can result in changes in the profiles of volatile organic compounds (VOC). These changes in volatile organic compounds (VOC) profiles can be utilized for disease detection and quantification. In this study, field asymmetric ion mobility spectrometry (FAIMS) was used to evaluate the VOC profile variability in a pea near isogenic line (Pisum sativum L.) inoculated with zoospores of Aphanomyces euteiches Drechs, which causes Aphanomyces root rot disease. Pots were filled with silica sand and six plants per pot were grown under controlled conditions in a randomized complete block design with four replications. Four treatments, namely non-inoculated, 1 x 105, 1 x 106, and 2.79 x 106 zoospores ml−1 were applied to plants at 5 and 7 days after emergence. FAIMS was used to collect volatile profiles at 2, 4, 7 and 9 days after inoculation. Specific regions of interest – extracted from the 3D ion current intensity from the FAIMS spectra – were analyzed using ANOVA, Similarly, multiple regions of interest were evaluated using principal component analysis and k-means clustering. Ion current profiles and curvature profiles were incorporated into the analysis using k-means clustering. Other ground reference data such as root rot index and physiological parameters were also recorded. The results showed a biomarker in a specific region of interest demonstrating ample ability to quantify and differentiate treatment effects during non-destructive sampling at 14 DAE (7 DAI). Data from this region could be used for early and non-destructive quantification and differentiation of treatment effects based on zoospore inoculation levels. The k-means clustering of ion current and curvature profiles showed patterns based on the treatments. These findings demonstrated that FAIMS could be used as a tool to assess plant-pathogen interactions using volatile biomarkers to evaluate disease responses and severity under controlled conditions.

Development of LC-FAIMS-MS and its application to lipidomics study of Acinetobacter baumannii infection

The recent advances in mass spectrometry (MS) technologies have enabled comprehensive lipid profiling in biological samples. However, the robustness and efficiency of MS-based lipidomics is compromised by the complexity of biological samples. High-field asymmetric waveform ion mobility spectrometry (FAIMS) is a technology that can continuously transmit one type of ion, independent of the mass-to-charge ratio. Here we present the development and application of LC-FAIMS-MS/MS-based platform for untargeted lipidomics. We used 3 optimally balanced compensation voltages, i.e., 29 V, 34 V and 39 V, to analyze all subclasses of glycerophospholipids. The reproducibility of the method was evaluated using reference standards. The reproducibility of retention times ranged from 0.9% to 1.5% RSD; whereas RSD values of 5%–10% were observed for peak areas. More importantly, the coupling of a FAIMS device can significantly improve the robustness and efficiency. We exploited this NPLC-FAIMS-HRMS to analyze the serum lipid profiles in mice infected intranasally with Acinetobacter baumannii. The temporal profiles of serum lipids after A. baumannii inoculation were obtained for 4 h, 8 h, and 24 h. We found that nearly all ether PC and ether PE lipids were significantly decreased 8 h after inoculation. The resultant volcano plot illustrated the distribution of 28 increased and 28 decreased lipid species in mouse sera 24 h after inoculation. We also found that a single ether PE composition can comprise multiple isomeric structures, and the relative abundance of each isomer could be quantified using the newly developed NPLC-FAIMS-PRM method.

Advancing Protein Analysis: A Low-Pressure Drift Tube Orbitrap Mass Spectrometer for Ultraviolet Photodissociation-Based Structural Characterization.

Owing to its ability to generate extensive fragmentation of proteins, ultraviolet photodissociation (UVPD) mass spectrometry (MS) has emerged as a versatile ion activation technique for the structural characterization of native proteins and protein complexes. Interpreting these fragmentation patterns provides insight into the secondary and tertiary structures of protein ions. However, the inherent complexity and diversity of proteins often pose challenges in resolving their numerous conformations. To address this limitation, we combined UVPD-MS with drift tube ion mobility, offering potential to acquire conformationally selective MS/MS information. A low-pressure drift tube (LPDT) Orbitrap mass spectrometer equipped with 193 nm UVPD capabilities enables the analysis of protein conformers through the analysis of arrival time distributions (ATDs) of individual fragment ions. ATDs of fragment ions are compared for different backbone cleavage sites of the protein or different precursor charge states to give information about regions of potential folding or elongation. This integrated platform offers promise for advancing our understanding of protein structures in the gas phase.

Photoionization ion mobility analyzer for on-site measurement of exhaled acetone by coupling miniature thermoelectric cooling dehydration

The breath concentration of acetone holds significant clinical importance, the development of on-site and accurate analyzer for exhaled acetone is highly demanded. A photoionization ion mobility analyzer based on a low-pressure krypton discharge lamp has been developed for direct and rapid determination of the acetone concentration. The difficulty for sensitive measurement of acetone by vacuum ultraviolet photoionization was the strong absorption of water molecules in the breath air. An online dehydration device with a miniature thermoelectric cooling quartz trap has been developed, which was capable for reducing the relative humidity from over 90 % to below 1 %. The dehydration could enhance the signal intensity of acetone about 85 times. The response time of current thermoelectric cooling dehydration was only 1/20 of the Nafion tube dehydration. A limit of detection 0.02 ppmV and linear response up to 2.0 ppmV were achieved. The interferences from ammonia in exhaled breath was eliminated using a calibration method based on ion number density, achieving recoveries ranging from 90 % to 110 %. In the final, the variation trends of exhaled acetone level in healthy individuals following the ingestion of glucose under fasting conditions were carried out to demonstrate the potential application of the analyzer.

Photothermally enhanced ion-transport in solid-state, non-Faradic energy storage devices for sub-freezing operability

The universal direct dependence of ionic mobility on temperature severely restricts the low-temperature operation of energy storage devices. We overcome this limitation by synergizing photothermal conversion with electrochemical energy storage, using non-graphitizable nanocarbon florets (NCF) as multi-functional electrodes. NCF-based supercapacitors leverage the photothermal energy, directing it to the High Internal Phase Emulsion polymer (poly-HIPE) infused ionic conductor [BMIm]-[TFSI], resulting in 15% increase in specific capacitance (Csp) at 30 °C and a 45% at −30 °C. This is the first solid-state energy storage device usable at sub-freezing conditions (< − 4 °C) without compromising its performance. Importantly, the device exhibits identical characteristics at 10 °C (with sunlight) and 30 °C (in the dark), thereby offsetting a temperature difference of 20 °C. Experimental evidences points to the reduction in electrolyte resistance by 86% and 34% in relaxation time constant as the origin of such improved functioning. Furthermore, the advantage of processability is translated to configurational form-factor to efficiently heat the ionic conductor and thereby realise a 15% increase in Csp.