Ion Mobility Research Articles

Met4DX: A Unified and Versatile Data Processing Tool for Multidimensional Untargeted Metabolomics Data.

Liquid chromatography-mass spectrometry (LC-MS) is a powerful tool in untargeted metabolomics, enabling the high-sensitivity and high-specificity characterization of metabolites. The integration of ion mobility (IM) with LC-MS, known as LC-IM-MS, enhances the analytical depth, facilitating more comprehensive metabolite profiling. However, the complexity of data generated by these technologies presents significant challenges in data processing. Addressing these challenges, we developed Met4DX, a unified and versatile software tool for processing both 3D and 4D untargeted metabolomics data. Met4DX incorporates a new MS1-oriented peak detection approach coupled with our bottom-up assembly algorithm, enabling highly sensitive and comprehensive peak detection in untargeted metabolomics data. Additionally, Met4DX employs a uniform quantification strategy to enhance the precision of peak integration across different samples. The software provides a user-friendly interface that simplifies data processing with default parameter sets, consolidating peak detection, alignment, quantification, and other procedures into a single streamlined workflow. Together, Met4DX offers a comprehensive solution for multidimensional metabolomics data processing, transforming raw data from diverse MS instruments into a final feature table containing quantification and identification results. We postulate Met4DX facilitates metabolite discovery in biological samples by deciphering the complex untargeted metabolomics data. Met4DX is freely available on the Internet (https://met4dx.zhulab.cn/).

Identification of Phospholipids Relevant to Cancer Tissue Using Differential Ion Mobility Spectrometry

Phospholipids are the main building components of cell membranes and are also used for cell signaling and as energy storages. Cancer cells alter their lipid metabolism, which ultimately leads to an increase in phospholipids in cancer tissue. Surgical energy instruments use electrical or vibrational energy to heat tissues, which causes intra- and extracellular water to expand rapidly and degrade cell structures, bursting the cells, which causes the formation of a tissue aerosol or smoke depending on the amount of energy used. This gas phase analyte can then be analyzed via gas analysis methods. Differential mobility spectrometry (DMS) is a method that can be used to differentiate malignant tissue from benign tissues in real time via the analysis of surgical smoke produced by energy instruments. Previously, the DMS identification of cancer tissue was based on a ‘black box method’ by differentiating the 2D dispersion plots of samples. This study sets out to find datapoints from the DMS dispersion plots that represent relevant target molecules. We studied the ability of DMS to differentiate three subclasses of phospholipids (phosphatidylcholine, phosphatidylinositol, and phosphatidylethanolamine) from a control sample using a bovine skeletal muscle matrix with a 5 mg addition of each phospholipid subclass to the sample matrix. We trained binary classifiers using linear discriminant analysis (LDA) and support vector machines (SVM) for sample classification. We were able to identify phosphatidylcholine, -inositol, and -ethanolamine with SVM binary classification accuracies of 91%, 73%, and 66% and with LDA binary classification accuracies of 82%, 74%, and 72%, respectively. Phosphatidylcholine was detected with a reliable classification accuracy, but ion separation setups should be adjusted in future studies to reliably detect other relevant phospholipids such as phosphatidylinositol and phosphatidylethanolamine and improve DMS as a microanalysis method and identify other phospholipids relevant to cancer tissue.

N-terminomics profiling of naïve and inflamed murine colon reveals proteolytic signatures of legumain.

Legumain is a cysteine protease broadly associated with inflammation. It has been reported to cleave and activate protease-activated receptor 2 to provoke pain associated with oral cancer. Outside of gastric and colon cancer, little has been reported on the roles of legumain within the gastrointestinal tract. Using a legumain-selective activity-based probe, LE28, we report that legumain is activated within colonocytes and macrophages of the murine colon, and that it is upregulated in models of acute experimental colitis. We demonstrated that loss of legumain activity in colonocytes, either through pharmacological inhibition or gene deletion, had no impact on epithelial permeability in vitro. Moreover, legumain inhibition or deletion had no obvious impacts on symptoms or histological features associated with dextran sulfate sodium-induced colitis, suggesting its proteolytic activity is dispensable for colitis initiation. To gain insight into potential functions of legumain within the colon, we performed field asymmetric waveform ion mobility spectrometry-facilitated quantitative proteomics and N-terminomics analyses on naïve and inflamed colon tissue from wild-type and legumain-deficient mice. We identified 16 altered cleavage sites with an asparaginyl endopeptidase signature that may be direct substrates of legumain and a further 16 cleavage sites that may be indirectly mediated by legumain. We also analyzed changes in protein abundance and proteolytic events broadly associated with colitis in the gut, which permitted comparison to recent analyses on mucosal biopsies from patients with inflammatory bowel disease. Collectively, these results shed light on potential functions of legumain and highlight its potential roles in the transition from inflammation to colorectal cancer.

Simultaneous detection of myostatin-targeting monoclonal antibodies in dried blood spots and plasma using liquid chromatography-tandem mass spectrometry with field asymmetric ion mobility spectrometry

Transforming growth factor-β superfamily members, such as myostatin, growth/differentiation factor 11, and activin A, negatively regulate skeletal muscle mass. Inhibitors targeting these cytokines or activin receptor type IIB have the potential to treat muscular diseases and enhance physical performance. However, because of their effects on muscle mass and potential misuse, they are strictly prohibited in sports. Given the high potential for misuse as a doping agent in sports, effective analytical methods for these prohibited antibodies targeting these specific cytokines or their receptor are critically needed. In this study, we aimed to develop and validate a multitarget method to detect the prohibited transforming growth factor-β superfamily-targeting monoclonal antibodies, such as landogrozumab, domagrozumab, and the activin receptor type IIB-targeting antibody, bimagrumab, in human plasma and dried blood spot (DBS) samples using liquid chromatography-tandem mass spectrometry. Antibodies were purified from both the DBS and plasma samples using protein G magnetic beads and field-asymmetric ion mobility spectrometry (FAIMS) to minimize interference, followed by liquid chromatography-tandem mass spectrometry analysis. The validation process included tests for specificity, selectivity, linearity, limit of detection (LOD), limit of identification, precision, recovery, carryover effect, and matrix effect. The LODs for the target antibodies were identical in both DBS and plasma samples at 0.1 µg/mL for landogrozumab heavy and light chains, as well as 0.25 µg/mL for the domagrozumab light chain and 0.25 µg/mL for the bimagrumab heavy chain. However, the heavy chain of domagrozumab exhibited an LOD of 0.5 µg/mL in DBS and 1 µg/mL in plasma. The analytical method demonstrated strong linearity, with R² values greater than 0.99 for both plasma and DBS, and no carryover effect. Precision (CV%) was below 15 % at both middle (1 or 5 µg/mL; specific to the heavy chain of domagrozumab in plasma) and high (10 µg/mL) concentrations and was less than 20 % at the LOD. The selectivity and specificity indicated no interference in the analysis of target mAbs in different blood samples. Recovery was 31.6–49.8 % for DBS and 51.4–85.3 % for plasma, with no significant matrix effect. This study provides an effective method for doping analysis and novel protein detection.

Preparation and investigation of structural, optical, and dielectric properties of PVA/PVP blend films boosted by MWCNTs/AuNPs for dielectric capacitor applications

With the rising global energy demands, there is a pressing need for the invention of efficient and reliable energy storage systems. This research centers on the creation and analysis of flexible dielectric capacitors composed of polymer nanocomposites (PNCs), incorporating a blend of polyvinyl alcohol (PVA) and polyvinyl pyrrolidone (PVP) as the base polymer, with multi-walled carbon nanotubes (MWCNTs) and gold nanoparticles (AuNPs) serving as nanofillers. The AuNPs were produced through an environmentally friendly synthesis method. Films made from PVA/PVP blended with MWCNTs and AuNPs were fabricated using the casting approach. Various characterization methods, including TEM, XRD, FTIR, and UV–Vis spectroscopy, were utilized to evaluate the samples. A detailed analysis of their electrical/dielectric characteristics was conducted. XRD analysis revealed a significant decrease in crystallinity from 55% for the pure PVA/PVP blend to 37% for the 1.6 wt% nanofiller composite, indicating increased amorphous content, which facilitates better ion mobility. FTIR confirmed strong interactions between the polymer matrix and nanofillers, with intensified vibrational peaks pointing to enhanced molecular dynamics. UV–Vis spectroscopy demonstrated a red shift in the absorption edge, and Tauc plot analysis showed a reduction in the indirect/direct optical band gap from 4.84 eV/5.68 eV for the pure blend to 4.26/5.35 eV for the nanocomposite with 1.6 wt% nanofillers. The addition of nanofillers resulted in improvements in their dielectric features, which exhibited a significant performance improvement, with the dielectric constant (ε′) reaching approximately 1100 at low frequency for the 1.6 wt% nanofiller sample, compared to 9 for the pure blend. Additionally, the dielectric loss (ε'') and tangent loss (tan δ) were reduced, with tan δ showing a decrease from 15 for the pure blend to 2 for the 1.6 wt% nanofiller composite at low frequency, indicating enhanced dielectric efficiency and reduced energy dissipation. The capacitors' functionality was assessed through capacitance-frequency and conductance-frequency analyses. The capacitors exhibited stable high capacitance across a broad frequency spectrum, making them alternatives for energy storage solutions.

Development and Validation of RoboCap, a Robotic Capillary Platform to Automate Capillary Electrophoresis Mass Spectrometry En Route to High-Throughput Single-Cell Proteomics.

Current developments in single-cell mass spectrometry (MS) aim to deepen proteome coverage while enhancing analytical speed to study entire cell populations, one cell at a time. Custom-built microanalytical capillary electrophoresis (μCE) played a critical role in the foundation of discovery single-cell MS proteomics. However, requirements for manual operation, substantial expertise, and low measurement throughput have so far hindered μCE-based single-cell studies on large numbers of cells. Here, we design and construct a robotic capillary (RoboCap) platform that grants single-cell CE-MS with automation for proteomes limited to less than ∼100 nL. RoboCap remotely controls precision actuators to translate the sample to the fused silica separation capillary, using vials in this work. The platform is hermetically enclosed and actively pressurized to inject ∼1-250 nL of the sample into a CE separation capillary, with errors below ∼5% relative standard deviation (RSD). The platform and supporting equipment were operated and monitored remotely on a custom-written Virtual Instrument (LabView). Detection performance was validated empirically on ∼5-250 nL portions of the HeLa proteome digest using a trapped ion mobility mass spectrometer (timsTOF PRO). RoboCap improved CE-ESI sample utilization to ∼20% from ∼3% on the manual μCE, the closest reference technology. Proof-of-principle experiments found proteome identification and quantification to robustly return ∼1,800 proteins (∼13% RSD) from ∼20 ng of the HeLa proteome digest on this earlier-generation detector. RoboCap automates CE-MS for limited sample amounts, paving the way to electrophoresis-based high-throughput single-cell proteomics.

Unraveling the Formation of Ternary AgCuSe Crystalline Nanophases and Their Potential as Antibacterial Agents.

AgCuSe nanoparticles could contribute to the growth of strongly light-absorbing thin films and solids with fast ion mobility, among other potential properties. Nevertheless, few methods have been developed so far for the synthesis of AgCuSe nanoparticles, and those reported deliver nanostructures with relatively large sizes and broad size and shape distributions. In this work, a colloidal cation exchange method is established for the easy synthesis of AgCuSe NPs with ca. 8 nm diameters and narrow size dispersion. Notably, in this lower size range the conucleation and growth of two stoichiometric ternary compounds are generally observed, namely the well-known eucairite AgCuSe compound and the novel fischesserite-like Ag3CuSe2 phase, the latter being less thermodynamically stable as predicted computationally and assessed experimentally. An optimal range of Cu/Ag precursor molar ratio has been identified to ensure the growth of ternary nanoparticles and, more specifically, that of the metastable Ag3CuSe2 nanophase isolated for the first occasion. The attained size range for the material paves the way for utilizing AgCuSe nanoparticles in new ways within the field of biomedicine: the results obtained here confirm the antibacterial activity of the new Ag x Cu y Se z nanoparticles against Gram-positive bacteria, with significantly low values of the minimal inhibitory concentration.

Metagenomic, metabolomic, and lipidomic shifts associated with fecal microbiota transplantation for recurrent Clostridioides difficile infection.

Recurrent C. difficile infection (rCDI) is an urgent public health threat, for which the last resort and lifesaving treatment is a fecal microbiota transplant (FMT). However, the exact mechanisms that mediate a successful FMT are not well-understood. Here, we use longitudinal stool samples collected from patients undergoing FMT to evaluate intra-individual changes in the microbiome, metabolome, and lipidome after successful FMTs relative to their baselines pre-FMT. We show changes in the abundance of many lipids, specifically a decrease in acylcarnitines post-FMT, and a shift from conjugated bile acids pre-FMT to deconjugated secondary bile acids post-FMT. These changes correlate with a decrease in Enterobacteriaceae, which encode carnitine metabolism genes, and an increase in Lachnospiraceae, which encode bile acid altering genes such as bile salt hydrolases (BSHs) and the bile acid-inducible (bai) operon, post-FMT. We also show changes in gut microbe-encoded amino acid biosynthesis genes, of which Enterobacteriaceae was the primary contributor to amino acids C. difficile is auxotrophic for. Liquid chromatography, ion mobility spectrometry, and mass spectrometry (LC-IMS-MS) revealed a shift from microbial conjugation of primary bile acids pre-FMT to secondary bile acids post-FMT. Here, we define the structural and functional changes associated with a successful FMT and generate hypotheses that require further experimental validation. This information is meant to help guide the development of new microbiota-focused therapeutics to treat rCDI.IMPORTANCERecurrent C. difficile infection is an urgent public health threat, for which the last resort and lifesaving treatment is a fecal microbiota transplant. However, the exact mechanisms that mediate a successful FMT are not well-understood. Here, we show changes in the abundance of many lipids, specifically acylcarnitines and bile acids, in response to FMT. These changes correlate with Enterobacteriaceae pre-FMT, which encodes carnitine metabolism genes, and Lachnospiraceae post-FMT, which encodes bile salt hydrolases and baiA genes. There was also a shift from microbial conjugation of primary bile acids pre-FMT to secondary bile acids post-FMT. Here, we define the structural and functional changes associated with a successful FMT, which we hope will help aid in the development of new microbiota-focused therapeutics to treat rCDI.

Impact of laterally mobile surface charge on diffusiophoresis of hydrophobic rigid colloids

The diffusiophoresis of charged hydrophobic nanoparticles (NPs) governed by an imposed ionic concentration gradient is analysed. The main objective is to elucidate the impact of the laterally mobile adsorbed surface ions at the interface on the propulsion of the hydrophobic NPs in diffusiophoresis. In addition, the dielectric polarization due to the difference in dielectric constant between the NPs and the suspension medium is also considered. The mobile surface ions create a friction as well as an electric force at the hydrophobic surface, which leads to a modification of the slip velocity condition and the slip length. We obtain an exact numerical solution of the governing electrokinetic equations in their full form by adopting a control volume formulation. The numerical model is supplemented by analytical solutions derived based on the Debye–Hückel linearization. We find that the lateral mobility of the surface ions obstruct the coions to diffuse from the higher concentration side to the lower concentration side, which results in a repulsive force to the particle leading to the occurrence of a negative mobility. Based on the numerical results and analytical solutions, we have shown that for a fully mobile surface charge, the diffusiophoresis of a hydrophobic NP is identical to the diffusiophoresis of a liquid droplet whose viscosity is related to the slip length of the hydrophobic particle. We establish that the dielectric polarization enhances the velocity of a hydrophobic particle, which has potential applications in the practical context.

Development and Manufacturing Method of Electrodes for a High Temperature Oxygen Sensor

The article discusses the use of zirconium dioxide stabilized with yttria as an electrolyte for the formation of a high-temperature ceramic oxygen concentration sensor. The fundamental possibility of using such a material is due to the high electrical conductivity caused by the mobility of oxygen ions in the vacancies of the solid electrolyte. The operating principle of such a sensor as an electrochemical concentration element is discussed. It has been shown that the use of such sensors is relevant for various industries (including chemical, metallurgical, oil and gas, energy and others). Options for forming electrodes of an electrochemical sensor using various materials and deposition methods are considered. A method for forming a platinum coating using a chemical method using isopropyl alcohol and subsequent pyrolysis was tested. It has been experimentally shown that the chemical method is applicable for the formation of electrodes of an electrochemical sensor. The electrical characteristics of the resulting coatings were measured. The optimal composition of the reaction mixture and the required number of layers to create a stable operating electrochemical sensor have been determined. The dependence of the potential of the formed electrochemical sensor from stabilized zirconium oxide on oxygen concentration in a wide temperature range has been studied. It has been shown that when using a scheme of sequential transformations, hydrolysis of platinum tetrachloride - deposition on a substrate - reductive pyrolysis, it is possible to obtain a high-quality conductive coating for the formation of gas sensor electrodes. The optimal composition of the reaction mixture for the formation of platinum electrodes has been selected. The optimal number of layers was determined to ensure the required level of electrical conductivity of the electrodes. It has been shown that an electrochemical element based on zirconium dioxide and platinum electrodes, formed according to the scheme developed in this work, can be used as a high-temperature oxygen sensor.

Effect of succinonitrile on the structural, ion conductivity, and dielectric properties of PVDF‐HFP based solid polymer electrolytes

AbstractA detailed account of the poly(vinylidene difluoride‐co‐hexafluoropropylene) (PVDF‐HFP)/succinonitrile (SN)/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) based solid polymer electrolytes (SPEs) of various compositions is reported. SN is incorporated as plasticizer, while LiTFSI is employed as the source of lithium ions. Fourier transfer infrared (FTIR) spectroscopy reveals the formation of polar and electroactive γ crystal phase by PVDF in pristine PVDF‐HFP and the prepared SPE films. FTIR further confirms the interaction between the host polymer and the salt and between the salt and the plasticizer. The interaction between the salt and plasticizer suggests that SN not only offers the plasticization effect but also facilitates salt dissociation. The ion conductivity increases with increasing salt content up to 20 wt% but beyond that concentration a decline in ion conductivity is observed, which could be attributed to the ion pair association or cluster formation due to the excess salt concentration that reduces the availability of free ions and ultimately leads to the reduction in ion conductivity. After including SN in the SPE formulation, electrochemical impedance spectroscopy reveals a substantial increase in room temperature ion conductivity of the SPE from ~1.08 × 10−5 S cm−1 for pristine SPE with 20 wt% salt to ~2.7 × 10−4 S cm−1 for plasticized SPE with 40 wt% SN and 20 wt% salt. This is attributed to the plasticizing effect of SN that enhances ion mobility through the matrix and to the increased charge carrier concentration (SN facilities salt dissociation). The fabricated SPEs exhibit a significant enhancement in ion conductivity with increasing temperature and the maximum ion conductivity of 1.1 × 10−3 S cm−1 is attained at 393 K by plasticized SPE with 40 wt% SN content. The ion conductivity of all the prepared SPEs follows the temperature dependent Arrhenius behavior, suggesting the thermally activated ion hopping mechanism of ionic conduction. Further, the plasticized SPEs display near unity ion transference number indicating the predominance of the ionic mode of conduction. The dielectric and electric modulus analysis reveal a faster relaxation phenomenon and hence higher ion conductivity of the prepared SPEs with increasing salt and plasticizer content.

New Processes for Ionizing Nonvolatile Compounds in Mass Spectrometry: The Road of Discovery to Current State-of-the-Art.

This Perspective covers discovery and mechanistic aspects as well as initial applications of novel ionization processes for use in mass spectrometry that guided us in a series of subsequent discoveries, instrument developments, and commercialization. Vacuum matrix-assisted ionization on an intermediate pressure matrix-assisted laser desorption/ionization source without the use of a laser, high voltages, or any other added energy was simply unbelievable, at first. Individually and as a whole, the various discoveries and inventions started to paint, inter alia, an exciting new picture and outlook in mass spectrometry from which key developments grew that were at the time unimaginable, and continue to surprise us in its simplistic preeminence. We, and others, have demonstrated exceptional analytical utility. Our current research is focused on how best to understand, improve, and use these novel ionization processes through dedicated platforms and source developments. These ionization processes convert volatile and nonvolatile compounds from solid or liquid matrixes into gas-phase ions for analysis by mass spectrometry using, e.g., mass-selected fragmentation and ion mobility spectrometry to provide accurate, and sometimes improved, mass and drift time resolution. The combination of research and discoveries demonstrated multiple advantages of the new ionization processes and established the basis of the successes that lead to the Biemann Medal and this Perspective. How the new ionization processes relate to traditional ionization is also presented, as well as how these technologies can be utilized in tandem through instrument modification and implementation to increase coverage of complex materials through complementary strengths.

Multi-proxy investigations of Bronze Age diet and environment in the hyper-arid eastern Tarim Basin (Lop Nur), northwest China

Humans have a long history of occupying ecologically marginal regions, and the ancient cultural mechanisms of adaptation to these challenging environments remain poorly understood. We examine archaeological deposits from a Bronze Age settlement in the hyper-arid eastern Tarim Basin (Lop Nur), identifying well-preserved plant remains and bone fragments that shed light on the palaeodiet and past environmental setting. We use the newly developed peptide mass fingerprinting method of ZooMS (zooarchaeology by mass spectrometry) and TimsTOF MS (trapped ion mobility time of flight mass spectrometry) to identify fragments of ancient fish bones as Cyprinidae and possible Salmonidae, indicating both their consumption and the former presence of intra-settlement fresh water-bodies. Remains of littoral and aquatic plants attest to a marshy palaeo-delta at the confluence of the Tarim and Kongque rivers, testifying to a former biodiverse oasis in the Lop Desert when humans occupied the site. We conclude that the use of both aquatic and desert peripheral resources, combined with the intentional management of local environments, were all essential prehistoric adaptations. In addition, we show that radiocarbon dates of aquatic remains have an offset spanning hundreds to thousands of years, due to a freshwater reservoir effect, requiring careful consideration of ages for archaeological bones in the broader region.

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.