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DOE OSTI2020

Low Temperature Oxidation of Methylpropyl Ether

Ethers are potential high-performance fuels that can be produced from renewable carbon sources such as biomass, but their combustion properties are not clearly understood. The cetane numbers (CN) for ethers, a measure of autoignition tendency, can range from less than 10 to greater than 100, and predictive tools based upon the molecular structures are desirable in order to focus fuel development research. In this study, we used molecular modeling, chemical kinetic modeling, and experimental measurements to understand the important reactions that lead to the autoignition of methylpropyl ether (MPE), a model for ethers containing alkyl chains long enough for intramolecular hydrogen transfer. These reactions are known to be important in the autoignition of alkanes and ethers and we propose to investigate the relationship between alkyl and ether reaction pathways. A reaction mechanism for MPE was created using MIT's Reaction Mechanism Generator (RMG) and G4 quantum calculation results and models were tested using the ChemKin Pro suite of software. Results from atmospheric pressure, flow tube reactor experiments and rapid compression machine (RCM) experiments were used to test the kinetic model and suggest refinements.

33 ADVANCED PROPULSION SYSTEMS↗

NASA NTRS2006

ISO 15859 Propellant and Fluid Specifications: A Review and Comparison with Military and NASA Specifications

This work presents an overview of the International Organization for Standardization (ISO) 15859 International Standard for Space Systems Fluid Characteristics, Sampling and Test Methods Parts 1 through 13 issued in June 2004. These standards establish requirements for fluid characteristics, sampling, and test methods for 13 fluids of concern to the propellant community and propellant characterization laboratories: oxygen, hydrogen, nitrogen, helium, nitrogen tetroxide, monomethylhydrazine, hydrazine, kerosene, argon, water, ammonia, carbon dioxide, and breathing air. A comparison of the fluid characteristics, sampling, and test methods required by the ISO standards to the current military and NASA specifications, which are in use at NASA facilities and elsewhere, is presented. Many ISO standards composition limits and other content agree with those found in the applicable parts of NASA SE-S-0073, NASA SSP 30573, military performance standards and details, and Compressed Gas Association (CGA) commodity specifications. The status of a current project managed at NASA Johnson Space Center White Sands Test Facility (WSTF) to rewrite these documents is discussed.

Greene, Ben↗

DOE OSTI2021

SN 2020bqj: A Type Ibn supernova with a long-lasting peak plateau

We report type Ibn supernovae (SNe Ibn) are a rare class of stripped envelope supernovae interacting with a helium-rich circumstellar medium (CSM). The majority of the SNe Ibn reported in the literature display a surprising homogeneity in their fast-evolving lightcurves and are typically found in actively starforming spiral galaxies. We present the discovery and the study of SN 2020bqj (ZTF20aalrqbu), a SN Ibn with a long-duration peak plateau lasting 40 days and hosted by a faint low-mass galaxy. We aim to explain its peculiar properties using an extensive photometric and spectroscopic data set. We compare the photometric and spectral evolution of SN 2020bqj with regular SNe Ibn from the literature, as well as with other outliers in the SN Ibn subclass. We fit the bolometric and multi-band lightcurves with powering mechanism models such as radioactive decay and CSM interaction. We also model the host galaxy of SN 2020bqj. The risetime, peak magnitude and spectral features of SN 2020bqj are consistent with those of most SNe Ibn, but the SN is a clear outlier in the subclass based on its bright, long-lasting peak plateau and the low mass of its faint host galaxy. We show through modeling that the lightcurve of SN 2020bqj can be powered predominantly by shock heating from the interaction of the SN ejecta and a dense CSM, combined with radioactive decay. The peculiar Type Ibn SN 2011hw is a close analog to SN 2020bqj in terms of lightcurve and spectral evolution, suggesting a similar progenitor and CSM scenario. In this scenario a very massive progenitor star in the transitional phase between a luminous blue variable and a compact Wolf-Rayet star undergoes core-collapse, embedded in a dense helium-rich CSM with an elevated opacity compared to normal SNe Ibn, due to the presence of residual hydrogen. This scenario is consistent with the observed properties of SN 2020bqj and the modeling results. SN 2020bqj is a compelling example of a transitional SN Ibn/IIn based on not only its spectral features, but also its lightcurve, host galaxy properties and the inferred progenitor properties. The strong similarity with SN 2011hw suggests this subclass may be the result of a progenitor in a stellar evolution phase that is distinct from those of progenitors of regular SNe Ibn.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1992

The anomalous extinction curve in the direction of Rho Ophiuchi from 950 to 1180 A

We report the interstellar extinction from 950 to 1180 A in the direction of Rho Oph. These data were obtained with a moderate-resolution sounding rocket observation of Ro Oph, and two lightly reddened B stars of identical spectral type. Unlike Voyager observations in this wavelength region, our spectral resolution is sufficient to directly measure the contribution of molecular hydrogen along the line of sight and unambiguously identify the dust contribution. The derived curves compare favorably with the extrapolation of functional fits to the Rho Oph derived from longer wavelengths. In addition, we have fitted a model of dust extinction to the derived curve and find that the best fits indicate that the line of sight exhibits a larger than average grain size and a preferential concentration of graphite relative to silicates. The sharp rise seen at the shortest wavelengths (below 1000 A) cannot be explained by standard silicate-graphite dust models and may be indicative of a nonstandard grain shape or a missing component in the extinction models.

Green, James C.↗

DOE OSTI2023

Non-Oxidative Ethane Dehydrogenation in a Packed-Bed DBD Plasma Reactor

Abstract Plasma-assisted conversion of ethane (C 2 H 6 ) can produce value-added chemical building blocks using green electricity. Here we employ a simple packed-bed coaxial dielectric barrier discharge (DBD) reactor to convert C 2 H 6 at mild operating conditions unattainable by conventional thermocatalysis. Ethylene (C 2 H 4 ), acetylene (C 2 H 2 ), and methane (CH 4 ) are the main products along with small fractions of C 3 and C 4 hydrocarbons. Interestingly, the C 2 H 4 selectivity is primarily correlated to C 2 H 6 conversion, dominated by electron dissociation and recombination reactions irrespective of the dielectric properties of the packed bed material (SiO 2 , Al 2 O 3 , ZrO 2 , TiO 2 , and BaTiO 3 ), packing material size, supplied power, and C 2 H 6 concentration. While a distortion of the electric field and discharge propagation results in varying dissipated power as materials change, the C 2 H 4 energy yield remains constant. The particle size appears to affect conversion mainly due to pressure alterations. Pd/SiO 2 catalyst can change the selectivity, favoring saturated species by expending hydrogen.

Engineering↗

DOE OSTI2026

Synthesis and characterization of 5,15-bis(hydroxymethyl)porphyrins – simple compounds distantly inspired by the chlorosomal bacteriochlorophylls

A self-assembly paradigm is provided in green photosynthetic bacteria by the chlorin macrocycle bacteriochlorophyll (BChl) c, which contains a 3-(1-hydroxyethyl) substituent, central magnesium ion, and 13-keto group. The assembled BChl c structure is a powerful light-harvesting apparatus that can support life even under extreme low-light conditions. Here, inspired by the work of Balaban, two far simpler porphyrins have been synthesized, 5,15-bis(hydroxymethyl)-10,20-diphenylporphinatozinc(II) (Ph/CH 2 OH) and 5,15-bis(hydroxymethyl)porphinatozinc(II) (H/CH 2 OH), and analogues wherein ethyl replaces hydroxymethyl (Ph/Et and H/Et). Examination of Ph/CH 2 OH and H/CH 2 OH by time-resolved spectroscopy showed an ∼2-fold enhancement in the singlet excited-state lifetime compared to meso-tetraphenylporphinatozinc(II) (ZnTPP). The single-crystal X-ray diffraction revealed distinct packing patterns. Porphyrin Ph/CH 2 OH exhibited double staircases wherein (1) each zinc is pentacoordinate (by apical coordination of one hydroxymethyl group of a porphyrin in the same staircase), (2) the second hydroxymethyl group is hydrogen-bonded to an apically coordinated hydroxymethyl oxygen atom in the adjacent staircase, (3) the porphyrins in a given staircase are coplanar but cofacially offset with each other, and (4) the adjacent staircases are oriented approximately 72° relative to each other. Porphyrin H/CH 2 OH assembled wherein (1) each zinc is hexacoordinate by ligation of hydroxymethyl moieties, (2) each hydroxymethyl –OH is hydrogen-bonded with an acetonitrile solvent molecule in the lattice, and (3) the planes of the four nearest neighbor porphyrins are essentially perpendicular to a given porphyrin. Study of the solid-state packing patterns of sparsely substituted porphyrins enables insights into how the structural design of tetrapyrroles can guide their aggregate self-assembly.

Tran, Vy-Phuong [North Carolina State University, ↗

NASA NTRS2010

Propulsion Risk Reduction Activities for Nontoxic Cryogenic Propulsion

The Propulsion and Cryogenics Advanced Development (PCAD) Project s primary objective is to develop propulsion system technologies for nontoxic or "green" propellants. The PCAD project focuses on the development of nontoxic propulsion technologies needed to provide necessary data and relevant experience to support informed decisions on implementation of nontoxic propellants for space missions. Implementation of nontoxic propellants in high performance propulsion systems offers NASA an opportunity to consider other options than current hypergolic propellants. The PCAD Project is emphasizing technology efforts in reaction control system (RCS) thruster designs, ascent main engines (AME), and descent main engines (DME). PCAD has a series of tasks and contracts to conduct risk reduction and/or retirement activities to demonstrate that nontoxic cryogenic propellants can be a feasible option for space missions. Work has focused on 1) reducing the risk of liquid oxygen/liquid methane ignition, demonstrating the key enabling technologies, and validating performance levels for reaction control engines for use on descent and ascent stages; 2) demonstrating the key enabling technologies and validating performance levels for liquid oxygen/liquid methane ascent engines; and 3) demonstrating the key enabling technologies and validating performance levels for deep throttling liquid oxygen/liquid hydrogen descent engines. The progress of these risk reduction and/or retirement activities will be presented.

Smith, Timothy D.↗

NASA NTRS2000

Catalytic Decomposition of Propellant Hydrazines, N-Nitrosodimethylamine, and N-Nitrodimethylamine

Remediation of propellant hydrazine spills, waste treatment, or cleanup of water contaminated with these propellants and/or their oxidation products is a subject of great concern for safety and the environment. Current remediation technologies typically employ oxidative methods, such as chlorination or ozonation. Methylated hydrazines, in particular 1,1-dimethythydrazine (UDMH) and to some degree monomethy1hydrazine (MMH), form N-Nitrosodimethylamine (NDMA) and N-Nitrodimethylamine (DMNM) during oxidation. These compounds are highly toxic and may persist if oxidative conditions are not sufficiently harsh. Since NDMA and DMNM may also be formed from exposure of MMH or UDMH to air, a need exists for a method that will remediate hydrazine, MMH, UDMH, NDMA, and DMNM. In this work, aqueous solutions of propellant hydrazines, NDMA, and DMNM were found to degrade by catalytic reduction with nickel-aluminum (Ni-Al) alloy under basic conditions. The reaction is based upon dissolution of At from Ni-Al alloy in aqueous media to form aluminum ion and hydrogen gas; and the resultant finely divided nickel catalyzes reduction of the hydrazine, nitrosoamine, or nitroamine by the hydrogen produced. Greater than 99 percent of hydrazine, MMH, UDMH, NDMA, and DMNM in aqueous solutions were degraded under laboratory conditions when reacted with Ni-Al alloy. UDMH was identified as an intermediate reduction product of NDMA and DNNM. NDMA and UDMH were identified as intermediate reduction products of DMNM. Control experiments without nickel showed no degradation of hydrazine, MMH or UDMH, while NDMA and DMNM were reduced to UDMH. Spill pillows containing Ni-Al alloy and solid sodium hydroxide were also found effective in absorption and degradation of UDMH. The application of chemical reduction as a means to propellant hydrazines, NDMA, and DMNM spill remediation, waste treatment, and water decontamination appears highly attractive.

Greene, Ben↗

NASA NTRS2004

Reformer Fuel Injector

Today's form of jet engine power comes from what is called a gas turbine engine. This engine is on average 14% efficient and emits great quantities of green house gas carbon dioxide and air pollutants, Le. nitrogen oxides and sulfur oxides. The alternate method being researched involves a reformer and a solid oxide fuel cell (SOFC). Reformers are becoming a popular area of research within the industry scale. NASA Glenn Research Center's approach is based on modifying the large aspects of industry reforming processes into a smaller jet fuel reformer. This process must not only be scaled down in size, but also decrease in weight and increase in efficiency. In comparison to today's method, the Jet A fuel reformer will be more efficient as well as reduce the amount of air pollutants discharged. The intent is to develop a 10kW process that can be used to satisfy the needs of commercial jet engines. Presently, commercial jets use Jet-A fuel, which is a kerosene based hydrocarbon fuel. Hydrocarbon fuels cannot be directly fed into a SOFC for the reason that the high temperature causes it to decompose into solid carbon and Hz. A reforming process converts fuel into hydrogen and supplies it to a fuel cell for power, as well as eliminating sulfur compounds. The SOFC produces electricity by converting H2 and CO2. The reformer contains a catalyst which is used to speed up the reaction rate and overall conversion. An outside company will perform a catalyst screening with our baseline Jet-A fuel to determine the most durable catalyst for this application. Our project team is focusing on the overall research of the reforming process. Eventually we will do a component evaluation on the different reformer designs and catalysts. The current status of the project is the completion of buildup in the test rig and check outs on all equipment and electronic signals to our data system. The objective is to test various reformer designs and catalysts in our test rig to determine the most efficient configuration to incorporate into the specific compact jet he1 reformer test rig. Additional information is included in the original extended abstract.

Suder, Jennifer L.↗

NASA NTRS1987

Plasma observations at the earth's magnetic equator

New observations of particle and wave data from the magnetic equator from the DE 1 spacecraft are reported. The results demonstrate that the equatorial plasma population is predominantly hydrogen and that the enhanced ion fluxes observed at the equator occur without an increase in the total plasma density. Helium is occasionally found heated along with the protons, and forms about 10 percent of the equatorially trapped population at such times. The heated H(+) ions can be characterized by a bi-Maxwellian with kT(parallel) = 0.5-1.0 eV and kT = 5-50 eV, with a density of 10-100/cu cm. The total plasma density is relatively constant with latitude. First measurements of the equatorially trapped plasma and coincident UHR measurements show that the trapped plasma is found in conjunction with equatorial noise.

Olsen, R. C.↗

DOE OSTI2019

Interconnection of the Antenna Pigment 8-HDF and Flavin Facilitates Red-Light Reception in a Bifunctional Animal-like Cryptochrome

Cryptochromes are ubiquitous flavin-binding light sensors closely related to DNA-repairing photolyases. The animal-like cryptochrome CraCRY from the green alga Chlamydomonas reinhardtii challenges the paradigm of cryptochromes as pure blue-light receptors by acting as a (6-4) photolyase, using 8-hydroxy-5-deazaflavin (8-HDF) as a light-harvesting antenna with a 17.4 Å distance to flavin and showing spectral sensitivity up to 680 nm. The expanded action spectrum is attributed to the presence of the flavin neutral radical (FADH•) in the dark, despite a rapid FADH• decay observed in vitro in samples exclusively carrying flavin. Herein, the red-light response of CraCRY carrying flavin and 8-HDF was studied, revealing a 3-fold prolongation of the FADH• lifetime in the presence of 8-HDF. Millisecond time-resolved ultraviolet-visible spectroscopy showed the red-light-induced formation and decay of an absorbance band at 458 nm concomitant with flavin reduction. Time-resolved Fourier transform infrared (FTIR) spectroscopy and density functional theory attributed these changes to the deprotonation of 8-HDF, challenging the paradigm of 8-HDF being permanently deprotonated in photolyases. FTIR spectra showed changes in the hydrogen bonding network of asparagine 395, a residue suggested to indirectly control flavin protonation, indicating the involvement of N395 in the stabilization of FADH•. Fluorescence spectroscopy revealed a decrease in the energy transfer efficiency of 8-HDF upon flavin reduction, possibly linked to 8-HDF deprotonation. Finally, the discovery of the interdependence of flavin and 8-HDF beyond energy transfer processes highlights the essential role of the antenna, introducing a new concept enabling CraCRY and possibly other bifunctional cryptochromes to fulfill their dual function.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Thermal stability and coalescence dynamics of exsolved metal nanoparticles at charged perovskite surfaces

Exsolution reactions enable the synthesis of oxide-supported metal nanoparticles, which are desirable as catalysts in green energy conversion technologies. It is crucial to precisely tailor the nanoparticle characteristics to optimize the catalysts’ functionality, and to maintain the catalytic performance under operation conditions. We use chemical (co)-doping to modify the defect chemistry of exsolution-active perovskite oxides and examine its influence on the mass transfer kinetics of Ni dopants towards the oxide surface and on the subsequent coalescence behavior of the exsolved nanoparticles during a continuous thermal reduction treatment. Nanoparticles that exsolve at the surface of the acceptor-type fast-oxygen-ion-conductor SrTi 0.95 Ni 0.05 O 3–δ (STNi) show a high surface mobility leading to a very low thermal stability compared to nanoparticles that exsolve at the surface of donor-type SrTi 0.9 Nb 0.05 Ni 0.05 O 3–δ (STNNi). Our analysis indicates that the low thermal stability of exsolved nanoparticles at the acceptor-doped perovskite surface is linked to a high oxygen vacancy concentration at the nanoparticle-oxide interface. For catalysts that require fast oxygen exchange kinetics, exsolution synthesis routes in dry hydrogen conditions may hence lead to accelerated degradation, while humid reaction conditions may mitigate this failure mechanism.

25 ENERGY STORAGE↗

NASA NTRS2010

Propulsion Risk Reduction Activities for Non-Toxic Cryogenic Propulsion

The Propulsion and Cryogenics Advanced Development (PCAD) Project s primary objective is to develop propulsion system technologies for non-toxic or "green" propellants. The PCAD project focuses on the development of non-toxic propulsion technologies needed to provide necessary data and relevant experience to support informed decisions on implementation of non-toxic propellants for space missions. Implementation of non-toxic propellants in high performance propulsion systems offers NASA an opportunity to consider other options than current hypergolic propellants. The PCAD Project is emphasizing technology efforts in reaction control system (RCS) thruster designs, ascent main engines (AME), and descent main engines (DME). PCAD has a series of tasks and contracts to conduct risk reduction and/or retirement activities to demonstrate that non-toxic cryogenic propellants can be a feasible option for space missions. Work has focused on 1) reducing the risk of liquid oxygen/liquid methane ignition, demonstrating the key enabling technologies, and validating performance levels for reaction control engines for use on descent and ascent stages; 2) demonstrating the key enabling technologies and validating performance levels for liquid oxygen/liquid methane ascent engines; and 3) demonstrating the key enabling technologies and validating performance levels for deep throttling liquid oxygen/liquid hydrogen descent engines. The progress of these risk reduction and/or retirement activities will be presented.

Smith, Timothy D.↗

NASA NTRS1985

Accelerated and real-time geosynchronous life cycling test performance of nickel-hydrogen batteries

RCA Astro-Electronics currently has four nickel-hydrogen storage battery modules (11 cells each) on test in simulated geosynchronous life cycle regimes. These battery modules are of identical design to those used on the GSTAR (GTE Satellite Corp.) and Spacenet (GTE Spacenet Corp.) communications satellites. The batteries are being tested using an automated test station equipped with computer-controlled environmental chambers and recording equipment. The two battery types, 30 ampere-hours and 40 ampere-hours (GSTAR and Spacenet, respectively), are being electrically cycled using identical 44-day eclipse sequences at 5 C and vary with respect to depth of discharge, recharge ratio, duration of accumulated suntime, and the use of a reconditioning sequence. The test parameters are outlined and the preliminary test data and results are presented.

Green, R. S.↗

DOE OSTI2023

Deterministic-Monte Carlo Hybrid Methods for Eigenvalue Sensitivity Coefficient Calculations

The TSUNAMI suite within the SCALE code package includes several methods for generating sensitivity data, including multigroup (MG) and continuous-energy (CE) capabilities. For generating sensitivities with CE data, three methods are available in SCALE 6.3.0: (1) the iterated fission probability (IFP) method with the KENO Monte Carlo transport solver, (2) IFP with the Shift Monte Carlo transport solver, and (3) the Contributon-Linked eigenvalue sensitivity/Uncertainty estimation via Tracklength importance Characterization (CLUTCH) with the KENO Monte Carlo transport solver. Currently, it is difficult to generate accurate sensitivities with large reflectors when using the CLUTCH method, specifically with fissionable and hydrogenous materials. To address this issue, the work presented herein examines a methodology to calculate the adjoint flux externally with the 3D deterministic SN transport code DENOVO in SCALE; the result is then read directly into the CLUTCH-TSUNAMI sequence. This hybridization method replaces the Monte Carlo F*(r) calculation in CLUTCH while still utilizing the forward calculation. The critical benchmark HEU-MET-FAST-028-001 is used to generate sensitivities based on the inability of CLUTCH to generate accurate sensitivities. Results from the hybrid method appear to generate sensitivity values that are in excellent agreement with direct perturbations. Although further testing is needed, the method provides promising results for the development and utility of a hybrid method for use in TSUNAMI.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Mechanism and dynamics of fatty acid photodecarboxylase

Photoenzymes are rare biocatalysts driven by absorption of a photon at each catalytic cycle; they inspire development of artificial photoenzymes with valuable activities. Fatty acid photodecarboxylase (FAP) is a natural photoenzyme that has potential applications in the bio-based production of hydrocarbons, yet its mechanism is far from fully understood. RATIONALE To elucidate the mechanism of FAP, we studied the wild-type (WT) enzyme from Chlorella variabilis (CvFAP) and variants with altered active-site residues using a wealth of techniques, including static and time-resolved crystallography and spectroscopy, as well as biochemical and computational approaches. RESULTS A 1.8-Å-resolution CvFAP x-ray crystal structure revealed a dense hydrogen-bonding network positioning the fatty acid carboxyl group in the vicinity of the flavin adenine dinucleotide (FAD) cofactor. Structures solved from free electron laser and low-dose synchrotron x-ray crystal data further highlighted an unusual bent shape of the oxidized flavin chromophore, and showed that the bending angle (14°) did not change upon photon absorption (step 1) or throughout the photocycle. Calculations showed that bending substantially affected the energy levels of the flavin. Structural and spectroscopic analysis of WT and mutant proteins targeting two conserved active-site residues, R451 and C432, demonstrated that both residues were crucial for proper positioning of the substrate and water molecules and for oxidation of the fatty acid carboxylate by 1 FAD* (~300 ps in WT FAP) to form FAD ∙– (step 2). Time-resolved infrared spectroscopy demonstrated that decarboxylation occured quasi-instantaneously upon this forward electron transfer, consistent with barrierless bond cleavage predicted by quantum chemistry calculations and with snapshots obtained by time-resolved crystallography. Transient absorption spectroscopy in H 2 O and D 2 O buffers indicated that back electron transfer from FAD ∙– was coupled to and limited by transfer of an exchangeable proton or hydrogen atom (step 3). Unexpectedly, concomitant with FAD ∙– reoxidation (to a red-shifted form FAD RS ) in 100 ns, most of the CO 2 product was converted, most likely into bicarbonate (as inferred from FTIR spectra of the cryotrapped FAD RS intermediate). Calculations indicated that this catalytic transformation involved an active-site water molecule. Cryo-Fourier transform infrared spectroscopy studies suggested that bicarbonate formation (step 4) was preceded by deprotonation of an arginine residue (step 3). At room temperature, the remaining CO 2 left the protein in 1.5 μs (step 4'). The observation of residual electron density close to C432 in electron density maps derived from time-resolved and cryocrystallography data suggests that this residue may play a role in stabilizing CO 2 and/or bicarbonate. Three routes for alkane formation were identified by quantum chemistry calculations; the one shown in the figure is favored by the ensemble of experimental data. CONCLUSION Finally, we provide a detailed and comprehensive characterization of light-driven hydrocarbon formation by FAP, which uses a remarkably complex mechanism including unique catalytic steps. We anticipate that our results will help to expand the green chemistry toolkit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1983

Ablation of carbonaceous materials in a hydrogen-helium arc-jet flow

The stagnation-point ablation rates of a graphite, a carbon-carbon composite, and four carbon-phenolic materials are measured in an arc-jet wind tunnel with a 50% hydrogen-50% helium mixture as the test gas. Flow environments are determined through measurements of static and impact pressures, heat-transfer rates to a calorimeter, and radiation spectra, and through numerical calculation of the flow through the wind tunnel, spectra, and heat-transfer rates. The environments so determined are: impact pressure approx. 3 atm, Mach number approx. 2.1, convective heat-transfer rate approx. 14 kw/sq cm, and radiative heat-transfer rate approx. 7 kw/sq cm in the absence of ablation. Ablation rates are determined from the measured rates of mass loss and recession of the ablation specimens. Compared with the predicted ablation rates obtained by running RASLE and CMA codes, the measured rates are higher by about 15% for all tested materials.

Park, C.↗

DOE OSTI2023

Evolutionary diversity of proton and water channels on the oxidizing side of photosystem II and their relevance to function

One of the reasons for the high efficiency and selectivity of biological catalysts arise from their ability to control the pathways of substrates and products using protein channels, and by modulating the transport in the channels using the interaction with the protein residues and the water/hydrogen-bonding network. Here, this process is clearly demonstrated in Photosystem II (PS II), where its light-driven water oxidation reaction catalyzed by the Mn 4 CaO 5 cluster occurs deep inside the protein complex and thus requires the transport of two water molecules to and four protons from the metal center to the bulk water. Based on the recent advances in structural studies of PS II from X-ray crystallography and cryo-electron microscopy, in this review we compare the channels that have been proposed to facilitate this mass transport in cyanobacteria, red and green algae, diatoms, and higher plants. The three major channels (O1, O4, and Cl1 channels) are present in all species investigated; however, some differences exist in the reported structures that arise from the different composition and arrangement of membrane extrinsic subunits between the species. Among the three channels, the Cl1 channel, including the proton gate, is the most conserved among all photosynthetic species. We also found at least one branch for the O1 channel in all organisms, extending all the way from Ca/O1 via the ‘water wheel’ to the lumen. However, the extending path after the water wheel varies between most species. The O4 channel is, like the Cl1 channel, highly conserved among all species while having different orientations at the end of the path near the bulk. The comparison suggests that the previously proposed functionality of the channels in T. vestitus (Ibrahim et al., Proc Natl Acad Sci USA 117:12624–12635, 2020; Hussein et al., Nat Commun 12:6531, 2021) is conserved through the species, i.e. the O1-like channel is used for substrate water intake, and the tighter Cl1 and O4 channels for proton release. The comparison does not eliminate the potential role of O4 channel as a water intake channel. However, the highly ordered hydrogen-bonded water wire connected to the Mn 4 CaO 5 cluster via the O4 may strongly suggest that it functions in proton release, especially during the S 0 → S 1 transition (Saito et al., Nat Commun 6:8488, 2015; Kern et al., Nature 563:421–425, 2018; Ibrahim et al., Proc Natl Acad Sci USA 117:12624–12635, 2020; Sakashita et al., Phys Chem Chem Phys 22:15831–15841, 2020; Hussein et al., Nat Commun 12:6531, 2021).

59 BASIC BIOLOGICAL SCIENCES↗