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1 H NMR Quantification of Aromatic Monomers from Reductive Catalytic Fractionation

Reductive catalytic fractionation (RCF) can produce high yields of aromatic monomers from lignin in native biomass. Quantification of these aromatic monomers is a well-known but demanding task, in part due to the lack of commercially available standards. Here, we demonstrate 1 H NMR spectroscopy as a complementary method to rapidly quantify aromatic monomer concentrations in RCF oils. The method exhibited good agreement with measurements from ultrahigh pressure liquid chromatography (UHPLC) for 96 RCF oils with varying monomer selectivity, with average absolute deviations of individual monomer yields between 0.5 and 1.1 wt % (relative 11–17%) and R 2 values above 0.9 compared to conventional UHPLC quantification. Quantification of S-type monomers, including for 4-ethylsyringol and 4-propenylsyringol, was generally reliable. The validity of G-type monomer quantifications depended on reaction selectivity due to overlap between peaks of 4-ethylguaiacol and 4-(3-hydroxypropyl)-guaiacol. The method could be applied on crude RCF oils without needing to perform the liquid–liquid extraction typically done for RCF reactions, thereby providing a convenient way to quantify lignin extraction and aromatic monomer yield. Overall, 1 H NMR spectroscopy can serve as a rapid primary quantification or secondary validation method for RCF monomer yield and selectivity measurements.

1H NMR spectroscopy↗

Developing a new ethylene glycol/H 2 O pretreatment system to achieve efficient enzymatic hydrolysis of sugarcane bagasse cellulose and recover highly active lignin: Countercurrent extraction

Improving pretreatment efficiency is a critical premise in achieving efficient biomass conversion, and obtaining high-performance natural polymers is the guarantee of high-value conversion of biomass. Here, in this study, a new pilot-scale continuous countercurrent pretreatment reaction unit about ethylene glycol-alkali solution was designed for pretreating sugarcane bagasse in order to achieve efficient separation of the three major components of lignocellulose when expanding the scale of pretreatment, reduce lignin deposition on the fiber surface, and obtain highly active lignin and excellent enzymatic hydrolysis efficiency of cellulose. X-ray diffractometer (XRD), X-ray photoelectron spectrometer (XPS), brunauer-emmett-teller (BET) and scanning electron microscope (SEM) methods are used to analyze the structural properties of sugarcane bagasse before and after pretreatment, and high-performance liquid chromatography (HPLC) is used to analyze the monosaccharide components in the enzymatic solution. In addition, the structural properties of the recovered lignin are analyzed by gel permeation chromatography (GPC), 31 P NMR and 2D-HSQC-NMR methods. The results indicate that the system can gain a high cellulose recovery of 92.99% along with a lignin removal of 95.33%, and recovered lignin has low lignin carbohydrate complexes, low condensation, and rich in phenolic hydroxyl groups for 1.95 mmol/g. Meanwhile, the countercurrent pretreatment system can effectively reduce the deposition of lignin on the cellulose surface, which is evidently superior to the non-countercurrent pretreatment and facilitates the efficiency of enzymatic saccharification of substrate, achieving a high glucose yield of 99% as well as a total sugar yield of 91.11%. The method efficiently separates biomass in a green manner, and solid residues are easily hydrolyzed, showing potential for industrial-scale production.

09 BIOMASS FUELS↗

Lignin molecular weights of Populus trichocarpa residues after CELF pretreatment

Here we present a dataset of molecular weights of lignin from a woody energy crop (Populus trichocarpa) residues after a series of co-solvent enhanced lignocellulosic fractionation (CELF) pretreatment. The natural poplar variant GW-9947 from the Center for Bioenergy Innovation (CBI) was used. The poplar was knife milled and passed through a 1 mm sieve and CELF pretreatment was performed in a Parr autoclave reactor with 7.5 wt % solids loading, 0.5 wt% H2SO4 as catalyst at 150°C with various time. Tetrahydrofuran was added in a 1:1 mass ratio with water as the pretreatment solvent. Lignin was isolated from the pretreated samples after ball-milling in a porcelain jar with ceramic balls via Retsch PM 200 at 580 rpm for 2.5 h followed by enzymatic hydrolysis in acetate buffer (pH 4.8, 50 °C) for 48 h. The solid residue was isolated by centrifugation and hydrolyzed again with freshly added buffer and enzymes for another 48 h. After filtration, the solid residue was extracted twice with 96% (v/v) 1,4-dioxane/water mixture at room temperature overnight. The extracts were combined, rotary evaporated, and freeze-dried to recover lignin. The lignin samples were then derivatized in an acetic anhydride/pyridine (1:1, v/v) mixture and stirred at room temperature for 24 h. Ethanol was added to the reaction mixture, left for 30 min and then removed with a rotary evaporator. The addition and removal of ethanol was repeated at least 3 times until all traces of acetic acid were removed. Acetylated lignin samples were then dissolved in tetrahydrofuran (THF) at a concentration of 1.0 mg/mL. The molecular weight of acetylated lignin was measured by a gel permeation chromatography (GPC) on a PSS-Polymer Standards Service (Warwick, RI, USA) GPC SECurity 1200 system featuring Agilent HPLC 1200 components equipped with four Waters Styragel columns (HR1, HR2, HR4 and HR6) and an UV detector (270 nm). Tetrahydrofuran was used as the mobile phase and flow rate was 0.3 mL/min. The Polymer Standards Service WinGPC Unity software (Build 6807) was used for data processing for all the samples. The data provides information about the effects of CELF pretreatment time at 150 ºC on lignin molecular weights.

09 BIOMASS FUELS↗

On the analysis of signal peaks in pulse-height spectra

The estimation of the signal location and intensity of a peak in a pulse height spectrum is important for X- ray and γ-ray spectroscopy, charged-particle spectrometry, liquid chromatography, and many other subfields. However, both the ‘‘centroid’’ and ‘‘signal intensity’’ of a peak in a pulse-height spectrum are ill-defined quantities and different methods of analysis will yield different numerical results. Here, we apply three methods of analysis. Method A is based on simple count summation and is likely the technique most frequently applied in practice. The analysis is straightforward and fast, and does not involve any statistical modeling. We find that it provides reliable results only for high signal-to-noise data, but has severe limitations in all other cases. Method B employs a Bayesian model to extract signal counts and centroid from the measured total and background counts. The resulting values are derived from the respective posteriors and, therefore, have a rigorous statistical meaning. The method makes no assumptions about the peak shape. It yields reliable and relatively small centroid uncertainties. However, it provides relatively large signal count uncertainties. Method C makes a strong assumption regarding the peak shape by fitting a Gaussian function to the data. Furthermore, the fit is based again on a Bayesian model. Although Method C requires careful consideration of the Gaussian width (usually given by the detector resolution) used in the fitting, it provides reliable values and relatively small uncertainties both for the signal counts and the centroid.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Harvesting 62 Zn from an aqueous cocktail at the NSCL

“Isotope harvesting” is a technique that offers access to exotic radionuclides created as by-products during nuclear science research. Ongoing exploratory work at the National Superconducting Cyclotron Laboratory (NSCL) is directed towards the production and extraction of rare radionuclides from a flowing-water target and intends to pave the way for future harvesting efforts at the upcoming Facility for Rare Isotope Beams (FRIB). Here in this paper, we present the collection of 62 Zn from an aqueous matrix irradiated with a 150 MeV/nucleon 78Kr beam, while synergistically capturing other gaseous reaction products. In addition to the production rate for 62 Zn (9.08(30)E-5 62 Zn per incoming 78 Kr), the rates of formation for several other radionuclides were determined as well. The purification of 62 Zn from a large number of co-produced radionuclides was performed by anion exchange chromatography, allowing the isolation of 80.5(5.2) % of the generated 62 Zn. With the decay of 62 Zn the radioactive daughter 62 Cu is generated, and with the isolation of pure 62 Cu eluate, the principle of a medical radionuclide generator could be demonstrated. To illustrate the applicability of the obtained 62 Zn, the isolated product was used in free and DTPA-labelled form in a proof of principle plant uptake study with garden cress employing phosphor imaging for visualization.

07 ISOTOPE AND RADIATION SOURCES↗

Broccoli seed extract rich in polysaccharides and glucoraphanin ameliorates DSS ‐induced colitis via intestinal barrier protection and gut microbiota modulation in mice

Abstract BACKGROUND Broccoli has received widespread attention because of its anti‐inflammatory and antioxidant effects. The present study aimed to explore the composition of broccoli seed extract (BSE) and its effect on colitis induced by dextran sulfate sodium (DSS). RESULTS BSE mainly comprises glucoraphanin and polysaccharides composed of arabinose, galactose, glucose and mannose. Animal experiments suggested that BSE intervention effectively reversed body weight loss, suppressed the levels of proinflammatory interleukin‐6, tumor necrosis factor‐α and interleukin‐1β, and elevated the levels of anti‐inflammatory interleukin‐10 and the activities of superoxide dismutase and glutathione in DSS‐induced colitis mice. According to histopathologic and immunohistochemical analysis of colon tissue, BSE intervention may repair the intestinal barrier by upregulating mRNA levels and the expression of tight junction proteins (claudin‐1, occludin and zonula occludens‐1). Gas chromatography–mass spectrometry (MS) analysis demonstrated that cecal short‐chain fatty acids in mice with BSE administration were significantly increased compared with the model group. Sulforaphane and sulforaphane‐ N ‐acetylcysteine were only detected in BSE group mice by ultra‐performance liquid chromatography‐MS analysis. In addition, BSE intervention evidently increased the abundance of Alistipeds , Coriobacteriaceae UCG‐002 and Bifidobacterium and decreased the abundance of Escheichia‐Shinella , Lachnospiraceae others , Parabacteroides , Ruminococcaceae others and Turicibacter , which possibly promoted carbohydrate metabolism and short‐chain fatty acid production. CONCLUSION The present study aimed to elucidate the effect of BSE on colitis and found that BSE, as a novel food ingredient, has great potential for the improvement of colitis. © 2022 Society of Chemical Industry.

Wu, Jiaying↗

Next Generation Solvent Vapor Pressure Testing

Previous work by Savannah River National Laboratory (SRNL) indicated that the actual Next Generation Solvent vapor pressure would be higher than the Original Caustic Side Solvent Extraction (CSSX) solvent vapor pressure, but below a bounding vapor pressure using Raoult’s Law. Since solvent vapor pressure has a significant impact on Composite Lower Flammability Limits (CLFL) and attendant accident analyses, obtaining an additional margin from the bounding NGS vapor pressure would be valuable. In order to quantify how much margin might be gained from the NGS bounding solvent, SRNL researchers were requested to perform vapor pressure testing with the Next Generation Solvent (NGS) by Savannah River Mission Completion (SRMC). The vapor pressure curve for the NGS formulation set to be deployed at the Salt Waste Processing Facility (SWPF) has been determined by SRNL up to 55°C (131°F) using headspace Gas Chromatography (GC). It was expected that NGS would have a higher vapor pressure than the Original CSSX solvent; however, experimental results indicate a lower vapor pressure. At this time, it is uncertain if this difference is due to the 7x increase in concentration of the large calixarene in the solvent (0.007M BOBCalix in Original CSSX solvent vs. 0.05M MaxCalix in NGS) or to minor batch-to-batch variations in Isopar-L constituents. The NGS and the Original CSSX solvent vapor pressure data were fitted to the Antoine Equation. The Antoine equation gives a more accurate representation of the expected vapor pressure of the solvents outside of the temperature range tested. The Antoine equation fitting for NGS is given below: $P=10^{6.364⁻\frac{1788.4}{T+219.3}}$. Where, p is the vapor pressure (partial pressure) of NGS in mmHg and T is the temperature in °C. It is recommended that SRMC either continue using the more conservative Isopar-L vapor pressure calculations at SWPF with the equation developed for the Original CSSX solvent, or the equation presented above for the NGS solvent. Additionally, it is recommended to study the variability in Isopar-L vapor pressure between lots.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Trimethyloxonium-mediated methylation strategies for the rapid and simultaneous analysis of chlorinated phenols in various soils by electron impact gas chromatography–mass spectrometry

Abstract The efficient methylation of a panel of five industrial and environmentally-relevant chlorophenols (CPs) employing trimethyloxonium tetrafluoroborate (TMO) for their qualitative detection and identification by electron impact gas chromatography–mass spectrometry (EI-GC–MS) is presented. The protocol’s execution is simple and smoothly converts the phenols into their O-methylated counterparts conveniently at ambient temperature. The efficiency of two versions of the protocol was successfully tested in their ability to simultaneously derivatize five CPs (2-chlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol, pentachlorophenol and triclosan) in six distinct, separate soil matrices (Nebraska EPA standard soil, Virginia Type A soil, Ottawa sand, Baker sand, Silt and Georgia EPA standard soil) when present at low levels (~ 10 μgg −1 ). The first version involves the direct derivatization of the spiked soils with the methylating salt while the second one involves an initial soil extraction step of the CPs followed by methylation. The MDL values for each methylated CP were determined and lower values were found (4.1–13.2 ng . mL −1 ) for both sand matrices (Ottawa and Baker) as well as for the Georgia EPA standard soil, while larger values (8.2–21.8 ng . mL −1 ) were found for the Virginia Type soil, Nebraska EPA standard soil and Silt. The presented protocol offers a safer and more practical alternative to the universally employed diazomethane method and can be readily applicable to matrices other than soils. Furthermore, the protocols described herein may find applicability to the methylation of other analytes bearing acidic protons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Preprocessing Tool for Enhanced Ion Mobility–Mass Spectrometry-Based Omics Workflows

The ability to improve the data quality of ion mobility–mass spectrometry (IM-MS) measurements is of great importance for enabling modular and efficient computational workflows and gaining better qualitative and quantitative insights from complex biological and environmental samples. We developed the PNNL PreProcessor, a standalone and user-friendly software housing various algorithmic implementations to generate new MS-files with enhanced signal quality and in the same instrument format. Different experimental approaches are supported for IM-MS based on Drift-Tube (DT) and Structures for Lossless Ion Manipulations (SLIM), including liquid chromatography (LC) and infusion analyses. The algorithms extend the dynamic range of the detection system, while reducing file sizes for faster and memory-efficient downstream processing. Specifically, multidimensional smoothing improves peak shapes of poorly defined low-abundance signals, and saturation repair reconstructs the intensity profile of high-abundance peaks from various analyte types. Further, other functionalities are data compression and interpolation, IM demultiplexing, noise filtering by low intensity threshold and spike removal, and exporting of acquisition metadata. Several advantages of the tool are illustrated, including an increase of 19.4% in lipid annotations and a two-times faster processing of LC-DT IM-MS data-independent acquisition spectra from a complex lipid extract of a standard human plasma sample. The software is freely available at https://omics.pnl.gov/software/pnnl-preprocessor.

59 BASIC BIOLOGICAL SCIENCES↗

Glycosylated stigmasterol from the rind of Napoleonaea imperialis

Napoleonaea imperialis rinds were separated from the seeds and extracted via maceration using methanol. The crude methanol extract was partitioned with n-hexane and dichloromethane to yield n-hexane fraction (11.01 g), dichloromethane fraction (35.16 g) and methanol fraction (101.75 g). Dichloromethane fraction was chromatographed and purified to give a compound whose structure was elucidated using one-dimension and two-dimension nuclear magnetic resonance (NMR) experiments. The isolated compound was characterized as glycosylated stigmasterol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Acylation as a successful derivatization strategy for the analysis of pinacolyl alcohol in a glycerol-rich matrix by GC-MS: application during an OPCW Proficiency Test

A derivatization protocol based on the acylation of pinacolyl alcohol (PA), an important marker for the nerve agent soman, is presented. The procedure provides a convenient means of detecting, by gas chromatography-mass spectrometry (GC-MS), PA when present at a low concentration in a complex glycerol/alcohol-rich matrix. While there are only two reports describing the specific analysis of PA in matrices at low concentrations, the protocol described herein represents the first of its kind in the analysis of PA in a highly reactive matrix. Two alternative paths for the protocol’s execution are presented. The first involves the direct derivatization of the PA with either acetyl or benzoyl chloride; both reactions yield ester products with significantly different retention times than those of the interferences of the reactive glycerol-rich matrix and in areas of the GC-chromatogram featuring lower levels of matrix interferences. A second procedure involved an initial diethyl ether/aqueous extraction of the matrix; while the extraction was found to substantially remove many of the hydrophilic matrix components and improve the overall derivatization, it also led to some loss of PA available for the derivatization. Both protocols were applied to the successful derivatization and analysis of PA by GC-MS when present at a 5 μg.mL -1 concentration in a glycerol-rich matrix sample administered during the 48th Proficiency Test administered by the Organisation for the Prohibition of Chemical Weapons (OPCW).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Increasing the Carbohydrate Output of Bamboo Using a Combinatorial Pretreatment

Bamboo represents a family of highly lignified biomass with significant resistance to cellulolytic enzyme degradation, and typically, a severe thermochemical pretreatment is needed to overcome its recalcitrance for producing fermentable sugars. Combinatorial pretreatments with a low holding temperature and low alkali dosage were investigated in this study in an attempt to remove the impediments to the accessibility of bamboo cellulose to enzymes and enable the efficient conversion of hemicellulose. Upon autohydrolysis at 180 °C, more than half of the hemicellulose (~58%) was solubilized, contributing to further delignification in the subsequent dilute alkali extraction (DAE). The solubilized hemicellulose mainly existed in the form of soluble xylan, which, after a novel endo-β-1,4-xylanase hydrolysis, generated a large amount of xylo-oligosaccharides with the xylobiose and xylotriose proportion reaching 72.99%. After the fractionation with combinatorial pretreatments, cellulose and xylose enzymatic hydrolysis yields were 73.36 and 86.98%, respectively, representing increments of 22.42 and 43.15% compared with the sole autohydrolysis process. Fluorescence microscopy (FM) and confocal Raman microscopy (CRM) images revealed that these dramatic improvements were caused by the deconstruction of the bamboo cell walls, including separation of the adjacent cell walls, removal of hemicellulose and lignin, migration and redistribution of lignin, and the increased exposure of cellulose. In addition, lignin chemical structure variations during the combinatorial pretreatment were analyzed with gel permeation chromatography (GPC), 2D HSQC NMR, and 31 P NMR, and the correlation between the lignin structure and enzymatic hydrolysis efficiency was investigated. In summary, this study highlighted the application of combinatorial pretreatments to maximize the carbohydrate output of bamboo and unveiled their mechanism that enabled the high-efficiency utilization of bamboo.

09 BIOMASS FUELS↗

Solvent Selection for the Separation of Lignin-Derived Monomers Using the Conductor-like Screening Model for Real Solvents

The separation of desired monomers from a liquid-phase mixture of lignin depolymerization products is necessary to facilitate their upscaling and upgrading for industrial applications. One effective method to separate multiple liquid-phase products is countercurrent chromatography (CCC), which is a common liquid chromatography technique that separates target solutes based on differences in their partitioning in a biphasic solvent system. Effective CCC separation requires the selection of solvent compositions to tune solute partition coefficients. Here, to alleviate the experimental burden of selecting optimal solvent systems, we apply the conductor-like screening model for real solvents (COSMO-RS) method to compute partition coefficients of representative lignin monomers from four currently used depolymerization strategies in standard solvent systems. We further design new ternary and quaternary solvent systems that are predicted to further improve separation efficacy. On the basis of these predicted partition coefficients and empirical solvent selection criteria for CCC measurements, we suggest a range of solvent systems that would be suitable for the effective separation of aromatic lignin-derived products via CCC or similar liquid–liquid extraction methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Changes in environmental and engineered conditions alter the plasma membrane lipidome of fractured shale bacteria

ABSTRACT Microorganisms that persist in fractured shale reservoirs cause several problems including secreting foul gases and forming biofilms. Current biocontrol measures often fail due to limited knowledge of their in situ activities. The plasma membrane protects the cell, mediates many of its critical functions, and responds to intracellular cues and ecological perturbations through physicochemical modifications. As such, it provides valuable insight into the physiological adaptation of microorganisms in disturbed environmental systems. Here, we (i) demonstrate how changes in salinity and hydraulic retention time (HRT) influence the plasma membrane intact polar lipid (IPL) chemistry of model bacterium, Halanaerobium congolense WG10, and mixed microbial consortia enriched from shale-produced fluids and (ii) elucidate adjustments in membrane IPL chemistry during biofilm growth relative to planktonic cells. We incubated H. congolense WG10 in chemostats under three salinities (7%, 13%, and 20% NaCl), operated under three HRTs (19.2, 24, and 48 h), and in drip flow biofilm reactors under the same salinity gradients. Also, mixed microbial consortia in produced fluids were enriched in triplicate chemostat vessels under three HRTs (19.2, 24, and 72 h) and biofilm reactors. Lipids were analyzed by ultra high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). Our results show that phosphatidylglycerols, cardiolipins, and phosphatidylethanolamines were predominantly enriched in planktonic H. congolense WG10 cells grown at hypersalinity (20%) compared to optimum (13%). In addition, several zwitterionic phosphatidylcholines and phosphatidylethanolamines were higher in abundance during biofilm growth. These observations suggest that microbial adaptation and biofilm formation in fractured shale are enabled by strategic plasma membrane IPL chemistry adjustments. IMPORTANCE Microorganisms inadvertently introduced into the shale reservoir during fracturing face multiple stressors including brine-level salinities and starvation. However, some anaerobic halotolerant bacteria adapt and persist for long periods of time. They produce hydrogen sulfide, which sours the reservoir and corrodes engineering infrastructure. In addition, they form biofilms on rock matrices, which decrease shale permeability and clog fracture networks. These reduce well productivity and increase extraction costs. Under stress, microbes remodel their plasma membrane to optimize its roles in protection and mediating cellular processes such as signaling, transport, and energy metabolism. Hence, by observing changes in the membrane lipidome of model shale bacteria, Halanaerobium congolense WG10, and mixed consortia enriched from produced fluids under varying subsurface conditions and growth modes, we provide insight that advances our knowledge of the fractured shale biosystem. We also offer data-driven recommendations for improving biocontrol efficacy and the efficiency of energy recovery from unconventional formations.

03 NATURAL GAS↗

Comparability of Liquid Chromatography Tandem Mass Spectrometry Analysis of Dissolved Organic Matter across Laboratories

Non-targeted liquid chromatography tandem highresolution mass spectrometry (LC−MS/MS) is increasingly applied for the structure-resolved chemical analysis of dissolved organic matter (DOM). With new developments in MS instrumentation and analysis software, the approach has gained substantial momentum over the past decade. However, achieving high-quality analytical data that is reproducible and comparable across laboratories can be a bottleneck in non-targeted metabolomics and organic matter chemical analysis, especially for data reuse in repository-scale analyses. Understanding the capabilities as well as challenges of comparing LC−MS/MS data from different laboratories is necessary for inferring global trends from public data sets. To illuminate instrumentation factors that drive differences and variability, we used a standardized data analysis pipeline, including classical (CMN) and featurebased molecular networking (FBMN), to analyze data from a ring trial by 24 laboratories on identical sample sets of algal and DOM extracts that were mixed in predefined concentrations and spiked with standards. Our results showed that data sets from similar mass spectrometer types with unified instrument parameters were qualitatively comparable, resolving the same general trends and shared mass spectral features. Interlaboratory comparability was best for high-intensity features, while low-intensity features showed greater detection variability. Our analysis also highlights challenges when comparing data from instruments with different acquisition rates or operating with less standardized methods. Lastly, we provide recommendations for data integration, public data sharing, standardization, and best practices for standardized LC−MS/MS data acquisition, which will be critical for long-term time series and intercomparability of DOM chemical analyses.

DOM↗

Sulfur-functionalized solid-phase materials for the selective separation of arsenic and selenium

Radioactive arsenic (As) isotopes are of growing interest for applications in nuclear medicine, national security, and environmental research. Recent efforts at the Facility for Rare Isotope Beams (FRIB) have focused on aqueous harvesting of selenium-72,73 ( 72,73 Se) and their daughter isotopes, arsenic-72,73 ( 72,73 As), which are particularly valuable for medical applications and nuclear data studies, respectively. Both conventional isotope production and harvesting methods require chemical separations to purify radioactive As from parent and co-produced Se radioisotopes. While several solid-phase separation methods for As and Se exist, many depend on complex oxidation state control or highly acidic conditions. This study presents results for sulfur-based solid-phase materials selected to enable uptake at lower acidity and eliminate the need for intricate redox chemistry. Specifically, the performance of three covalently bound sulfur-based ligands were evaluated: (1) thiophenol-polystyrene, (2) propanethiol-silica, and (3) thiourea-silica. Uptake characteristics—including distribution coefficients (Dw), kinetics, and column separation behavior—were assessed using 75 Se and 73 As in hydrochloric (HCl) acid and nitric (HNO 3 ) solutions. The resins demonstrated high-yield (>95%) and high-purity As recovery across a range of HCl concentrations. Comparable results in HNO 3 were achieved when combined with anion exchange chromatography. Furthermore, the potential application of these materials for medical isotope generators was also investigated through ligand stability and repeated elution studies. Overall, sulfur leaching from the resins was negligible at the concentrations relevant for these separations but increased with higher acid concentrations.

Arsenic↗

Advancing Enhanced Raman Spectroscopy to Detect and Measure NOW Pheromones (CPRB 2022 proposal)

Insect sex pheromones are chemical compounds that insects release to attract their partners over distances of hundreds of meters or even kilometers, in complete darkness and without any audible signals. Use of synthetic forms of key compounds have in some cases become an essential component of monitoring and/or managing key pests of agricultural crops, including navel orangeworm (Amyelois transitella) (NOW) in California tree nuts. These pheromone-based strategies can include monitoring, mating disruption, mass trapping, attract-and-kill and push-pull. There are currently multiple commercially available mating disruption products available for NOW and recent studies have demonstrated that they can be effectively used to reduce crop damage by this pest. Just how mating disruption works is not fully established and likely varies across products and target species. For instance, the extent to which synthetic pheromones compete with natural pheromone is not well understood, or in the case of monitoring, how efficaciously the insect follows the diffusing plumes, especially across large blocks and at plot borders. Furthermore, there may be specific conditions under which poor or impeded diffusion of synthetic pheromone diminishes the disruption effect, which could result in some males effectively locating females for reproduction. At the same time, many commercially available synthetic lures are also available, and growers have been effectively using them to track population development – although the attractive range of these lures remains unclear. That is, while pheromone lures can attract many moths, the relationship between trap capture and local populations, much less crop damage, remains unclear. Regardless of the emission source (aerosol puffers, meso emitters, lures etc.), we currently lack the ability to fully understand how these synthetic pheromone compounds diffuse away from their point-source of emission – and subsequently how this might affect the efficacy of mating disruption and/or the accuracy of monitoring efforts. Raman spectroscopy (RS) may offer a means to detect synthetic pheromone because of its analytical properties and recent technological advancements. In combination with nanostructured probes, RS has a demonstrated capability to detect volatiles at extremely low concentrations. While other methods for detecting pheromones have proven to be successful, such analytical methods like mass spectrometry (MS) gas chromatography (GC) require sampling in the fields and are not real-time. Other methods such as EAG/ EAD are also invasive (use antennas) but are of course valuable. Opto-electronic, micro and nano sensors just recently enticed interest. We fall in this latter category, proposing the use of optical spectroscopy (Raman) in a fiber aided by nanostructures to provide a chemical fingerprint without transductions and in real-time (i.e. no sampling). To date, we have been able to generate Raman signatures for the main chemicals in synthetic pheromones (a first for science, to the best of our knowledge), observe their trends at different concentrations, and also provide a clear distinction of such signatures in mixed samples via Principal Component Analysis (PCA) – all of which strengthens our conclusions on the ability of RS to detect emissions in more realistic conditions. We also established processes to enhance the detection sensitivity via preconcentration with Solid Phase Micro Extraction (SPME) fibers and Surface Enhanced Raman Spectroscopy (SERS) to increase the overall optical signals. Furthermore, we explored limitations and requirements for detecting from dispensers, lures, or live moths, including Dept. of Energy and CA State regulatory approvals. Finally, we setup some of our first “orchard in a box” experiments to measure pheromone diffusion along with developing appropriate models.

42 ENGINEERING↗

LipidOz enables automated elucidation of lipid carbon–carbon double bond positions from ozone-induced dissociation mass spectrometry data

Lipids play essential roles in many biological processes and disease pathology, but unambiguous identification of lipids is complicated by the presence of multiple isomeric species differing by fatty acyl chain length, stereospecifically numbered (sn) position, and position/stereochemistry of double bonds. Conventional liquid chromatography-mass spectrometry (LC-MS/MS) analyses enable the determination of fatty acyl chain lengths (and in some cases sn position) and number of double bonds, but not carbon-carbon double bond positions. Ozone-induced dissociation (OzID) is a gas-phase oxidation reaction that produces characteristic fragments from lipids containing double bonds. OzID can be incorporated into ion mobility spectrometry (IMS)-MS instruments for the structural characterization of lipids, including additional isomer separation and confident assignment of double bond positions. The complexity and repetitive nature of OzID data analysis and lack of software tool support have limited the application of OzID for routine lipidomics studies. Here, we present an open-source Python tool, LipidOz, for the automated determination of lipid double bond positions from OzID-IMS-MS data, which employs a combination of traditional automation and deep learning approaches. Our results demonstrate the ability of LipidOz to robustly assign double bond positions for lipid standard mixtures and complex lipid extracts, enabling practical application of OzID for future lipidomics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗