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DOE OSTI2021

Local electronic structure of histidine in aqueous solution

Here, the local electronic structure of aqueous histidine, an amino acid important in nature and biology, is revealed by aerosol X-ray photoemission spectroscopy. A detailed picture of the photoionization dynamics emerges by tuning the pH of the aqueous solution from which the aerosols are generated, allowing us to report the X-ray photoelectron spectroscopy (XPS) of histidine. Assignment of the experimental photoelectron spectra of the C1s and N1s levels allows the determination of the protonation state of histidine in these aqueous aerosols and is confirmed by density functional calculations. XPS spectra show that at pH = 1, both imidazole and amine group nitrogens are protonated, at pH = 7, the amine group nitrogen is protonated and the carboxyl group carbon is deprotonated resulting in a zwitterionic structure, and at pH = 13, only the carboxyl group remains deprotonated. Comparison of these results with previous experimental and theoretical results suggests that X-ray spectroscopy on aqueous aerosols can provide a convenient and simple way of probing their electronic structure in aqueous solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

2017 Meander C and O floodplain groundwater chemistry from the East River, Colorado

This dataset includes groundwater geochemistry data from floodplain piezometers collected as a part of the Watershed Function Scientific Focus Area (SFA) located in the Upper Colorado River Basin. The data were collected in order to investigate the role of hyporheic exchange and other river corridor processes on riverine export of solutes. Floodplain piezometers in the Pumphouse vicinity (Meander C: MCP, MCB; Meander O: MOP) were sampled on daily to weekly time scales during summer-fall 2017. Data includes in-field measurements (pH, electrical conductivity [EC], oxidation reduction potential [ORP], dissolved oxygen [DO], Fe(II), and groundwater level) along with laboratory measurements (dissolved inorganic carbon [DIC], dissolved organic carbon [DOC], metals and major cations, anions [chloride, sulfate, nitrate], and dissolved ammonium). The chemistry data is contained in a csv file, sampling protocol in a pdf document, and sample locations in both a kmz file which can be opened in Google Earth and a csv file.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

2018 Meander C floodplain groundwater chemistry from the East River Watershed, Colorado

This dataset includes groundwater geochemistry data from floodplain piezometers collected as a part of the Watershed Function Scientific Focus Area (SFA) located in the Upper Colorado River Basin. The data were collected in order to investigate the role of hyporheic exchange and other river corridor processes on riverine export of solutes. Floodplain piezometers installed along two transects across Meander C in the Pumphouse vicinity (MCP and MCB wells) were sampled on daily to weekly time scales during summer-fall 2018. Some river water grab samples are also included. Data includes in-field measurements (pH, electrical conductivity [EC], oxidation reduction potential [ORP], dissolved oxygen [DO], Fe(II), and groundwater level) along with laboratory measurements (dissolved inorganic carbon [DIC], dissolved organic carbon [DOC], metals and major cations, anions [chloride, sulfate, nitrate], and dissolved ammonium). Five files are included in this dataset, including: sample locations and depths in both a kmz file which can be opened in Google Earth and a csv file, sampling protocol as a pdf document, aqueous geochemistry data in a csv file, and analytical detection limits in a csv file.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

2016 Floodplain Geochemistry from the East River Watershed, Colorado

This dataset includes groundwater geochemistry data from floodplain piezometers collected as a part of the Watershed Function Scientific Focus Area (SFA) located in the Upper Colorado River Basin. The data were collected in order to investigate the role of hyporheic exchange and other river corridor processes on riverine export of solutes. Floodplain piezometers installed in several meanders (Meander C, Meander D, and Meander O) in the vicinity of the Pumphouse were sampled at several dates in 2016. Data includes in-field measurements (pH, electrical conductivity, oxidation reduction potential, dissolved oxygen, dissolved Fe(II), dissolved sulfide, and groundwater level) along with laboratory measurements (dissolved inorganic carbon, dissolved organic carbon, metals and major cations). Five files are included in this dataset, including: sample locations and depths in a csv file (metadata.csv), aqueous geochemistry data in a csv file, analytical detection limits in a csv file, a file-level metadata (flmd.csv) file, and a data dictionary (dd.csv) file. Data that was below the detection limit is reported as one half of the detection limit and missing data is listed as "-9999".

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Stability of the particle-hole Pfaffian state and the 5 2 -fractional quantum Hall effect

Here we present a method for the exact construction of the fully particle-hole symmetric Pfaffian (PH-Pfaffian) ground state and its charged excitations on a sphere. We adopt the Moore-Read state, but with a nonholomorphic pairing component as in previous studies, and project it to the lowest Landau level. We study the energetics as well as other properties of these states and find that in a pure system interacting with the Coulomb forces the PH-Pfaffian cannot compete with either the Moore-Read state or its particle-hole conjugate, the anti-Pfaffian state, as an explanation for the 5/2 effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Heterosynaptic plasticity in biomembrane memristors controlled by pH

Abstract In biology, heterosynaptic plasticity maintains homeostasis in synaptic inputs during associative learning and memory, and initiates long-term changes in synaptic strengths that nonspecifically modulate different synapse types. In bioinspired neuromorphic circuits, heterosynaptic plasticity may be used to extend the functionality of two-terminal, biomimetic memristors. In this article, we explore how changes in the pH of droplet interface bilayer aqueous solutions modulate the memristive responses of a lipid bilayer membrane in the pH range 4.97–7.40. Surprisingly, we did not find conclusive evidence for pH-dependent shifts in the voltage thresholds ( V* ) needed for alamethicin ion channel formation in the membrane. However, we did observe a clear modulation in the dynamics of pore formation with pH in time-dependent, pulsed voltage experiments. Moreover, at the same voltage, lowering the pH resulted in higher steady-state currents because of increased numbers of conductive peptide ion channels in the membrane. This was due to increased partitioning of alamethicin monomers into the membrane at pH 4.97, which is below the pKa (~5.3–5.7) of carboxylate groups on the glutamate residues of the peptide, making the monomers more hydrophobic. Neutralization of the negative charges on these residues, under acidic conditions, increased the concentration of peptide monomers in the membrane, shifting the equilibrium concentrations of peptide aggregate assemblies in the membrane to favor greater numbers of larger, increasingly more conductive pores. It also increased the relaxation time constants for pore formation and decay, and enhanced short-term facilitation and depression of the switching characteristics of the device. Modulating these thresholds globally and independently of alamethicin concentration and applied voltage will enable the assembly of neuromorphic computational circuitry with enhanced functionality. Impact statement We describe how to use pH as a modulatory “interneuron” that changes the voltage-dependent memristance of alamethicin ion channels in lipid bilayers by changing the structure and dynamical properties of the bilayer. Having the ability to independently control the threshold levels for pore conduction from voltage or ion channel concentration enables additional levels of programmability in a neuromorphic system. In this article, we note that barriers to conduction from membrane-bound ion channels can be lowered by reducing solution pH, resulting in higher currents, and enhanced short-term learning behavior in the form of paired-pulse facilitation. Tuning threshold values with environmental variables, such as pH, provide additional training and learning algorithms that can be used to elicit complex functionality within spiking neural networks. Graphical abstract

36 MATERIALS SCIENCE↗

DOE OSTI2021

Energetics and kinetics of various cyano radical hydrogen abstractions

The cyano radical (CN) is an abundant, open-shell molecule found in a variety of environments, including the atmosphere, the interstellar medium and combustion processes. In these environments, it often reacts with small, closed-shell molecules via hydrogen abstraction. Both carbon and nitrogen atoms of the cyano radical are reactive sites, however the carbon is more reactive with reaction barrier heights generally between 2–15 kcal mol -1 lower than those of the analogous nitrogen. The CN + HX → HCN/HNC + X, with X = H, CH 3 , NH 2 , OH, F, SiH 3 , PH 2 , SH, Cl, C 2 H, CN reactions have been studied at a high-level of theory, including CCSD(T)-F12a. Finally, kinetics were obtained over the 100–1000 K temperature range, showing excellent agreement with those rate constants that have been determined experimentally.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Modest functional diversity decline and pronounced composition shifts of microbial communities in a mixed waste-contaminated aquifer

Background: Microbial taxonomic diversity declines with increased environmental stress. Yet, few studies have explored whether phylogenetic and functional diversities track taxonomic diversity along the stress gradient. Here, we investigated microbial communities within an aquifer in Oak Ridge, Tennessee, USA, which is characterized by a broad spectrum of stressors, including extremely high levels of nitrate, heavy metals like cadmium and chromium, radionuclides such as uranium, and extremely low pH (< 3). Results: Both taxonomic and phylogenetic α-diversities were reduced in the most impacted wells, while the decline in functional α-diversity was modest and statistically insignificant, indicating a more robust buffering capacity to environmental stress. Differences in functional gene composition (i.e., functional β-diversity) were pronounced in highly contaminated wells, while convergent functional gene composition was observed in uncontaminated wells. The relative abundances of most carbon degradation genes were decreased in contaminated wells, but genes associated with denitrification, adenylylsulfate reduction, and sulfite reduction were increased. Compared to taxonomic and phylogenetic compositions, environmental variables played a more significant role in shaping functional gene composition, suggesting that niche selection could be more closely related to microbial functionality than taxonomy. Conclusions: Overall, we demonstrated that despite a reduced taxonomic α-diversity, microbial communities under stress maintained functionality underpinned by environmental selection.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1997

A Method for Preparation, Storage and Activation of Large Populations of Immotile Sea Urchin Sperm

Reversible protein phosphorylation is associated with initiation and modulation of sperm flagellar motility. Many studies aimed at examining the signal transduction mechanisms underlying the expression of motility have relied on detergent-permeabilized sperm reactivated with exogenous 32 P-ATP. However, the reactivation conditions allow variable levels of motility to be expressed and phosphorylation of many proteins that appear to be unrelated to sperm motility. Thus, identification of the few relevant proteins is difficult. We have developed a method to collect and keep sperm immotile until reactivated for analysis to normal motility levels. Artificial sea water (ASW) buffered with 5 mM 2-[N-morpholino]ethanesulfonic acid at pH 6.0 and containing 50 mM KCI, allows collection and storage of immotile sea urchin sperm for up to 96 h at 4-5 C. Motility under these conditions is essentially zero, but sperm is rapidly reactivated to normal motility by diluting with ASW to standard pH (8.0) and KCI concentration (10 mM).

Bracho, Geracimo E.↗

DOE OSTI2021

Accessing the Subsurface Biosphere Within Rocks Undergoing Active Low-Temperature Serpentinization in the Samail Ophiolite (Oman Drilling Project)

The Oman Drilling Project established an “Active Alteration” multi-borehole observatory in peridotites undergoing low-temperature serpentinization in the Samail Ophiolite. The highly serpentinized rocks are in contact with strongly reducing fluids. Distinct hydrological regimes, governed by differences in rock porosity and fracture density, give rise to steep redox (Eh +200 to –750 mV) and pH (pH range 8.5–11.2) gradients within the 300–400 m deep boreholes. The serpentinites and fluids host an active subsurface ecosystem. Microbial cell abundances in serpentinite vary at least six orders of magnitude, from ≤3.5 × 10 1 to 2.9 × 10 7 cells/g. Low levels of biological sulfate reduction (2–1,000 fmol/cm 3 /day) can be detected in rock cores, particularly in rocks in contact with reduced groundwaters with pH < 10.5. Thermodesulfovibrio is the predominant sulfate reducer identified via metagenomic sequencing of adjacent groundwater communities. Here, we infer that transport and reaction of microbially generated sulfide with the serpentine and brucite assemblages gives rise to optical darkening and sulfide overprinting, including the formation of tochilinite-vallerite group minerals, potentially serving as an indicator that this system is inhabited by microbial life. Olivine mesh-cores replaced with ferroan brucite and minor awaruite, abundant veins containing hydroandradite garnet and polyhedral serpentine, and late-stage carbonate veins are suggested as targets for future spatially resolved life-detection investigations. The high-quality whole-round core samples that have been preserved can be further probed to define how life distributes itself and functions within a system where chemical disequilibria are sustained by low-temperature water/rock interaction, and how biosignatures of in situ microbial activity are generated.

58 GEOSCIENCES↗

DOE OSTI2023

Resolving dynamic mineral-organic interactions in the rhizosphere by combining in-situ microsensors with plant-soil reactive transport modeling

Associations between minerals and organic matter represent one of the most important carbon storage mechanisms in soils. Plant roots are major sources of soil carbon, and resolving the dynamics and dominance of microbial consumption versus mineral sorption of root-derived carbon is critical to understanding soil carbon storage. Here we integrate in-situ rhizosphere microsensor and plant physiological measurements with a 3-D plant-soil reactive transport model to explore the fate of dissolved organic carbon (DOC) in the rhizosphere, particularly its microbial consumption and interaction with Fe oxide minerals. Over several days, a microdialysis probe sampling pore water at the root-soil interface of growing Vicia faba roots in live soil, revealed clear diel patterns of DOC concentration. Daytime DOC spikes coincided with peaks in leaf-level photosynthesis rates and were accompanied by declining redox potential and dissolved oxygen as well as increasing pH in the rhizosphere. Incorporating microsensor data into our modeling framework showed that the measured rapid loss of DOC after each mid-day spike could not be explained by consumption via aerobic respiration, nor via anaerobic respiration dominated by Fe oxide reduction. Rather, in the model, a large fraction of rhizosphere DOC was rapidly immobilized each day by adsorption to Fe oxides. Further, modeled microbial Fe reduction (fueled by DOC) did not mobilize significant organic carbon from Fe oxides during the day. Instead, the model predicted equilibrium desorption of organic carbon from Fe oxides at night. This new mechanistic modeling framework, which couples aboveground plant physiological measurements with non-destructive high-resolution monitoring of rhizosphere processes, has great potential for exploring the dynamics and balance of the various microbial reactions and mineral interactions controlling carbon transformations and storage in soils.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1981

Ambient ammonia measurements using laser photo-acoustic spectroscopy

Ammonia concentrations reached minimal levels (approximately 0.1 ppb) in early winter, followed by a sudden later winter increase. A direct relationship between ambient ammonia levels and air temperature was inferred from the data (linear correlation coefficient r=0.53). Ammonia concentrations were determined to be directly related to the absolute humidity of the air (r=0.72); a weaker relationship between ammonia concentrations and relative humidity was discovered (r=0.37). The data also indicated that ammonia levels were generally higher within continental air masses than those of maritime origin. Soil parameters such as pH and moisture content were found to have a major bearing on the release of gaseous ammonia from soils in the region.

Aldridge, M. D., III↗

NASA NTRS2003

Ultrasonic Spectroscopy of Stainless Steel Sandwich Panels

Enhanced, lightweight material systems, such as 17-4PH stainless steel sandwich panels are being developed for use as fan blades and fan containment material systems for next generation engines. In order to improve the production for these systems, nondestructive evaluation (NDE) techniques, such as ultrasonic spectroscopy, are being utilized to evaluate the brazing quality between the 17-4PH stainless steel face plates and the 17-4PH stainless steel foam core. Based on NDE data, shear tests are performed on sections representing various levels of brazing quality from an initial batch of these sandwich structures. Metallographic characterization of brazing is done to corroborate NDE findings and the observed shear failure mechanisms.

Cosgriff, Laura M.↗

NASA NTRS2008

Near-Infrared Spectroscopic Measurements of Calf Muscle during Walking at Simulated Reduced Gravity - Preliminary Results

Consideration for lunar and planetary exploration space suit design can be enhanced by investigating the physiologic responses of individual muscles during locomotion in reduced gravity. Near-infrared spectroscopy (NIRS) provides a non-invasive method to study the physiology of individual muscles in ambulatory subjects during reduced gravity simulations. PURPOSE: To investigate calf muscle oxygen saturation (SmO2) and pH during reduced gravity walking at varying treadmill inclines and added mass conditions using NIRS. METHODS: Four male subjects aged 42.3 +/- 1.7 years (mean +/- SE) and weighing 77.9 +/- 2.4 kg walked at a moderate speed (3.2 +/- 0.2 km/h) on a treadmill at inclines of 0, 10, 20, and 30%. Unsuited subjects were attached to a partial gravity simulator which unloaded the subject to simulate body weight plus the additional weight of a space suit (121 kg) in lunar gravity (0.17G). Masses of 0, 11, 23, and 34 kg were added to the subject and then unloaded to maintain constant weight. Spectra were collected from the lateral gastrocnemius (LG), and SmO2 and pH were calculated using previously published methods (Yang et al. 2007 Optics Express ; Soller et al. 2008 J Appl Physiol). The effects of incline and added mass on SmO2 and pH were analyzed through repeated measures ANOVA. RESULTS: SmO2 and pH were both unchanged by added mass (p>0.05), so data from trials at the same incline were averaged. LG SmO2 decreased significantly with increasing incline (p=0.003) from 61.1 +/- 2.0% at 0% incline to 48.7 +/- 2.6% at 30% incline, while pH was unchanged by incline (p=0.12). CONCLUSION: Increasing the incline (and thus work performed) during walking causes the LG to extract more oxygen from the blood supply, presumably to support the increased metabolic cost of uphill walking. The lack of an effect of incline on pH may indicate that, while the intensity of exercise has increased, the LG has not reached a level of work above the anaerobic threshold. In these preliminary studies, 30% incline walking at reduced gravity may not require anaerobic LG activity due to the low exercise intensity (42.8 +/- 1.6% of VO(sub 2max)). It is also possible that at reduced gravity additional work is being done by muscle groups other than the calf.

Ellerby, Gwenn E. C.↗

NASA NTRS2010

International Space Station (ISS) Internal Active Thermal Control System (IATCS) New Biocide Selection, Qualification and Implementation

The Internal Active Thermal Control System (IATCS) aboard the International Space Station (ISS) is primarily responsible for the removal of heat loads from payload and system racks. The IATCS is a water based system which works in conjunction with the EATCS (External ATCS), an ammonia based system, which are interfaced through a heat exchanger to facilitate heat transfer. On-orbit issues associated with the aqueous coolant chemistry began to occur with unexpected increases in CO2 levels in the cabin. This caused an increase in total inorganic carbon (TIC), a reduction in coolant pH, increased corrosion, and precipitation of nickel phosphate. These chemical changes were also accompanied by the growth of heterotrophic bacteria that increased risk to the system and could potentially impact crew health and safety. Studies were conducted to select a biocide to control microbial growth in the system based on requirements for disinfection at low chemical concentration (effectiveness), solubility and stability, material compatibility, low toxicity to humans, compatibility with vehicle environmental control and life support systems (ECLSS), ease of application, rapid on-orbit measurement, and removal capability. Based on these requirements, ortho-phthalaldehyde (OPA), an aromatic dialdehyde compound, was selected for qualification testing. This paper presents the OPA qualification test results, development of hardware and methodology to safely apply OPA to the system, development of a means to remove OPA, development of a rapid colorimetric test for measurement of OPA, and the OPA on-orbit performance for controlling the growth of microorganisms in the ISS IATCS since November 3, 2007.

Wilson, Mark E.↗

NASA NTRS2011

International Space Station (ISS) Internal Active Thermal Control System (IATCS) New Biocide Selection, Qualification and Implementation

Wilson, Mark E.↗

DOE OSTI2025

pH adjustment increases biofuel production from inhibitory switchgrass hydrolysates

Biofuels derived from renewable and sustainable lignocellulosic biomass, such as switchgrass, offer a promising means to limit greenhouse gas emissions. However, switchgrass grown under drought conditions contains high levels of chemical compounds that inhibit microbial conversion to biofuels. Fermentation of drought switchgrass hydrolysates by engineered Saccharomyces cerevisiae and Zymomonas mobilis results in lower ethanol production than does fermentation of hydrolyzed switchgrass from a typical rainfall year. Here, it is demonstrated that this inhibitory effect can be alleviated by altering the pH of drought switchgrass hydrolysates produced by two different pretreatment methods: Ammonia Fiber Expansion (AFEX) and Soaking in Aqueous Ammonia (SAA). Fermentation rates and biofuel production by Saccharomyces cerevisiae and Zymomonas mobilis were higher at pH 5.8 than at pH 5.0 from all feedstock years and following both pretreatment methods. SAA pretreatment of drought switchgrass furthermore enabled increased fermentation rates and biofuel titers compared to AFEX pretreatment. A synthetic mimic of switchgrass hydrolysate was developed and identified relief from pH-dependent inhibition by lignocellulose-derived inhibitors as the cause of increased biofuel production above a pH of 5.0. These results demonstrate that SAA pretreatment and pH adjustment can significantly improve fermentation and biofuel production from inhibitory feedstocks by industrial microorganisms.

09 BIOMASS FUELS↗

DOE OSTI2022

Stirred-Reactor Coupon Analysis: An International Round Robin Study

The objective of this task was to determine the precision of the SRCA technique when used to determine the dilute condition corrosion rate. To this end, an interlaboratory round robin study was conducted per the instructions in ASTM Practice E691 to measure the precision with which the SRCA test method can be conducted. Twelve independent labs from eleven different institutions each evaluated four glass compositions in three different conditions. The ASTM procedures recommend at least 6 labs participate in a round robin testing the same 3 materials in the same conditions to determine precision. In this case, 12 labs each performed 12 independent tests. This was only possible thanks to the multi-glass testing capability of the SRCA test. A total of 108 duplicate pairs were used to calculate the repeatability of the tests, with the same glass tested in the same vessel, producing as identical conditions as possible for the replicates. These test results were quite tightly clustered, with a median difference from the average value of the pair of only 2.9%. Based on the calculations outlined in ASTM E177-20 and a measured standard deviation of 4.74%, the intralaboratory repeatability limit (r) was calculated to be within 13.3% of the expected value with 95% confidence level. The reproducibility limit (R) of the test was examined using all 277 data points from the round robin. Because of the differences in dissolution rates due to pH variability and intrinsically for the 12 conditions tested, the reproducibility limits for each condition and overall were calculated from the percent relative residual value for each test. The SRCA test is expected to be reproducible within 64% of the expected value with a 95% confidence level.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗