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DOE OSTI2019

Elusive Intermediates in the Breakdown Reactivity Patterns of Prodrug Platinum(IV) Complexes

Kinetically inert platinum(IV) complexes are receiving growing attention as promising candidates in the effort to develop safe and valid alternatives to classical square-planar Pt(II) complexes currently used in antineoplastic therapy. Their antiproliferative activity requires intracellular Pt(IV)–Pt(II) reduction (activation by reduction). In the present work, a set of five Pt(IV) complexes has been assayed using mass spectrometry–based techniques, i.e., collision-induced dissociation (CID), and IR multiple photon dissociation (IRMPD) spectroscopy, together with ab initio theoretical investigations. Breakdown and reduction mechanisms are observed that lead to Pt(II) species. Evidence is found for typically transient Pt(III) intermediates along the dissociation paths of isolated, negatively charged (electron-rich) Pt(IV) prodrug complexes. .

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2025

Elucidating grain boundary energy minimization mechanisms in textured Ca-doped alumina with inclination-dependent Monte Carlo Potts simulations

The grain growth behavior of textured Ca-doped alumina is compared to Monte Carlo Potts (MCP) simulations to investigate the effect of anisotropic grain boundary (GB) properties on local boundary migration. Experimentally, the growth of textured Ca-doped alumina results in highly elongated grains. The relative GB energy distribution is measured using the thermal groove method before and after heat treating at 1600°C, finding that high energy GBs are eliminated during grain growth. No significant difference in the GB energy distributions is found between the long and short axes of the elongated grains, suggesting that anisotropic mobility may be responsible for the grain shape. However, MCP simulations with anisotropic mobility as a function of plane inclination do not result in grains with distinct morphologies, regardless of the degree of anisotropy introduced. The final grain shape after grain growth of textured Ca-doped alumina resembles that of the MCP simulations using an anisotropic GB energy as a cosine function of plane inclination. Several energy functions are tested and only those that mathematically impose a torque (second derivative of energy with respect to the plane inclination angle) result in elongated grains. Although area reduction is the dominant energy minimization mechanism, these results suggest that local GB migration is affected by anisotropic GB energy and torque and alternative mechanisms like GB replacement and reorientation.

36 MATERIALS SCIENCE↗

DOE OSTI2019

A decomposition approach based on meta-heuristics and exact methods for solving a two-stage stochastic biofuel hub-and-spoke network problem

An alternative to the production of fossil transportation fuels is the production of biofuels, particularly, bioethanol. One of the main opportunity areas is the reduction in the overall cost of biofuel. An approach to reduce this cost is to design and implement a supply chain (SC) that considers the quality-related properties of the biomass as well as the economies of scale to minimize the logistics and quality-related costs. This problem is formulated as a hub location problem, which has been classified as an NP-hard problem, thus, meta-heuristics are a suitable approach to solve this problem. We propose a hybrid meta-heuristic solution procedure to solve large-scale instances of a two-stage stochastic biomass-to-biorefinery hub-and-spoke network problem. This solution procedure is proposed to support the large-scale production and distribution of bioethanol by considering the variability in its moisture and ash contents. The hybrid method utilizes a simulated annealing-simplex method to find an initial solution and a tabu search-simplex method to improve the solution. Numerical experimentation was performed on a realistic case study in Texas. The findings demonstrate that the hybrid procedure outperforms the standard L-shaped (LS) method. The meta-heuristic combining simulated annealing and tabu search with the simplex method (SATS-SM) achieved 2.48% lower costs and required 96.57% less time, on average, when compared to the results from using the LS.

09 BIOMASS FUELS↗

DOE OSTI2021

Photosynthetic adaptation to polar life: Energy balance, photoprotection and genetic redundancy

The persistent low temperature that characterize polar habitats combined with the requirement for light for all photoautotrophs creates a conundrum. The absorption of too much light at low temperature can cause an energy imbalance that decreases photosynthetic performance that has a negative impact on growth and can affect long-term survival. The goal of this review is to survey the mechanism(s) by which polar photoautotrophs maintain cellular energy balance, that is, photostasis to overcome the potential for cellular energy imbalance in their low temperature environments. Photopsychrophiles are photosynthetic organisms that are obligately adapted to low temperature (0⁰- 15 °C) but usually die at higher temperatures (≥20 °C). In contrast, photopsychrotolerant species can usually tolerate and survive a broad range of temperatures (5⁰- 40 °C). First, we summarize the basic concepts of excess excitation energy, energy balance, photoprotection and photostasis and their importance to survival in polar habitats. Second, we compare the photoprotective mechanisms that underlie photostasis and survival in aquatic cyanobacteria and green algae as well as terrestrial Antarctic and Arctic plants. We show that polar photopsychrophilic and photopsychrotolerant organisms attain energy balance at low temperature either through a regulated reduction in the efficiency of light absorption or through enhanced capacity to consume photosynthetic electrons by the induction of O 2 as an alternative electron acceptor. Finally, we compare the published genomes of three photopsychrophilic and one photopsychrotolerant alga with five mesophilic green algae including the model green alga, Chlamydomonas reinhardtii. We relate our genomic analyses to photoprotective mechanisms that contribute to the potential attainment of photostasis. Finally, we discuss how the observed genomic redundancy in photopsychrophilic genomes may confer energy balance, photoprotection and resilience to their harsh polar environment. Primary production in aquatic, Antarctic and Arctic environments is dependent on diverse algal and cyanobacterial communities. Although mosses and lichens dominate the Antarctic terrestrial landscape, only two extant angiosperms exist in the Antarctic. Furthermore, the identification of a single ‘molecular key’ to unravel adaptation of photopsychrophily and photopsychrotolerance remains elusive. Since these photoautotrophs represent excellent biomarkers to assess the impact of global warming on polar ecosystems, increased study of these polar photoautotrophs remains essential.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Proton-Coupled Group Transfer Enables Concerted Protonation Pathways Relevant to Small-Molecule Activation

The mechanistic identification of Nature's use of concerted reactions, in which all bond-breaking and bond-making occurs in a single step, has inspired rational designs for artificial synthetic transformations via pathways that bypass high energy intermediates that would otherwise be thermodynamically and kinetically inaccessible. Here, we electrochemically activate an organometallic Ruthenium(II) complex to show that, in acetonitrile solutions, the movement of protons from weak Brønsted acids, such as water and methanol, is coupled with the transfer of its negatively charged counterpart to carbon dioxide (CO 2 ) - a process termed proton-coupled group transfer - to stoichiometrically produce a metal-hydride complex and a carbonate species. These previously unidentified pathways have played key roles in CO 2 and proton reduction catalysis by enabling the generation of key intermediates such as hydrides and metallocarboxylic acids, while its applicability to carbon acids may provide alternative approaches in the electrosynthesis of chemical commodities via alkylation and carboxylation reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Human DNA polymerase θ grasps the primer terminus to mediate DNA repair

DNA polymerase θ protects against genomic instability via an alternative end-joining repair pathway for DNA double-strand breaks. Polymerase θ is overexpressed in breast, lung and oral cancers, and reduction of its activity in mammalian cells increases sensitivity to double-strand break–inducing agents, including ionizing radiation. Reported in this paper are crystal structures of the C-terminal polymerase domain from human polymerase θ, illustrating two potential modes of dimerization. One structure depicts insertion of ddATP opposite an abasic-site analog during translesion DNA synthesis. The second structure describes a cognate ddGTP complex. Polymerase θ uses a specialized thumb subdomain to establish unique upstream contacts to the primer DNA strand, including an interaction with the 3'-terminal phosphate from one of five distinctive insertion loops. Finally, these observations demonstrate how polymerase θ grasps the primer to bypass DNA lesions or extend poorly annealed DNA termini to mediate end-joining.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Enabling electrochemical N 2 reduction to NH 3 in the low overpotential region using non-noble metal Bi electrodes via surface composition modification

The electrochemical N 2 reduction reaction (ENRR) that can produce NH 3 using water as the hydrogen source at ambient temperature and pressure can be an exciting alternative to the Haber–Bosch process. The major challenge for electrochemical NH 3 production is the competing hydrogen evolution reaction (HER), which seriously limits the faradaic efficiency (FE) for NH 3 production. To date, noble metal electrocatalysts that are inactive for the HER have mainly been investigated for the ENRR. Studies reporting a FE greater than 10% for NH 3 production using non-noble metal catalysts in the low overpotential region (E ≤ 0.2 V vs. RHE) are very rare. This study reports effective electrochemical surface modification strategies that drastically increase the ENRR activity of a non-noble Bi electrode in the low overpotential region and achieve a FE for NH 3 production as high as 13.2% at -0.2 V vs. RHE in pH 7.5 phosphate buffer. Finally, the effect of each of the surface modifications on the activity for the ENRR and the electrode stability during the ENRR were systematically elucidated, which may be used to develop general strategies to enhance the ENRR activities of other non-noble metal electrodes in the low overpotential region.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Towards the next generation 23% efficient n-type cells with low cost manufacturing

Suniva, Inc., in collaboration with the University Center for Excellence in Photovoltaics (UCEP) at the Georgia Institute of Technology (GIT) proposed this comprehensive three year program to enable the development of an advanced high performance product that will help the US regain its competitive edge in PV. This project was designed to overcome cost and efficiency barriers through advances in PV science, technology innovation, low-cost manufacturing and full production of ~22.5% efficient n-type Si cells in Norcross, GA. At the heart of the project is the desire to complement the technology being developed concurrently under the Solarmat and ARPAe initiatives to develop a differentiated product superior in both performance and cost effectiveness to the competing alternatives available on the market, and push towards achieving SunShot objectives while ensuring a sustainable business model based on US manufacturing. A significant reduction of the costs in modules produced today will need to combine reductions in wafer costs, cell processing costs as well as module fabrication costs while delivering a product that is not only more efficient under test conditions but also increases the energy yield in outdoor operations. This project will result in a differentiated high performance product and technology that is consistent with sustaining PV manufacturing in the US for a longer term and further highlights the need for continued support for developing the next generation concepts that can keep US manufacturing thriving to support the growing demand for PV in the US and consistent with the US government’s mandates for energy independence.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

NASA NTRS1971

The quasi-inertial and wide-deadband modes as backup attitude options for the Skylab mission

The quasi-inertial (QI) and wide deadband (WDB) modes were investigated as alternatives to the solar inertial (SI) mode in case two control moment gyros fail during the Skylab mission. Both modes provide a substantial reduction in propellant requirements from the solar interial hold requirement with either the orbital assembly/thruster attitude control system or service module reaction control system. Spacecraft motion in the QI mode is produced by a command rate and results in a small amplitude oscillation (17 deg, maximum) about the SI orientation. In the WDB mode a somewhat similar, but larger amplitude motion (35 deg maximum) about the SI orientation is developed by appropriate choice of controller deadbands and switch line slopes.

Elrod, B. D.↗

NASA NTRS2000

Age and Stress Prediction

Genoa is a software product that predicts progressive aging and failure in a variety of materials. It is the result of a SBIR contract between the Glenn Research Center and Alpha Star Corporation. Genoa allows designers to determine if the materials they plan on applying to a structure are up to the task or if alternate materials should be considered. Genoa's two feature applications are its progressive failure simulations and its test verification. It allows for a reduction in inspection frequency, rapid design solutions, and manufacturing with low cost materials. It will benefit the aerospace, airline, and automotive industries, with future applications for other uses.

Source record↗

NASA NTRSDate not supplied

Evaluation of Finite Impulse Response Filters for Turbulence Effects on Sonic Booms

Turbulence effects on sonic booms lead to random variability of sonic boom waveforms measured on the ground, complicating the prediction of such waveforms using sonic boom propagation codes that do not account for turbulence effects. The NASA PCBoom software is one such code shown to accurately predict sonic booms above the atmospheric boundary layer but not those on the ground. Analyses of measured sonic booms show that, on average, the turbulence effects result in sonic boom loudness reduction, on average, that increases with propagation distance and turbulence strength. To efficiently account for such effects, a signal processing-based approach has been developed at NASA using finite impulse response filters derived from predicted waveforms by solving a nonlinear parabolic equation. Analyses indicate that the mean loudness reduction obtained using the filters does not increase with propagation distance or with increasing turbulence strength, in disagreement with flight test data. An alternative approach to the filters is currently under development employing the multiple scattering theory (MST) of wave propagation. Available results from the physics-based MST approach are used to evaluate the predictive capability of the filters, suggesting that the filters can severely underestimate the prediction of the MST approach.

sonic booms↗

NASA NTRSDate not supplied

Evaluation of Finite Impulse Response Filters for Turbulence Effects on Sonic Booms

sonic booms↗

DOE OSTI2011

Selective Electrocatalytic Activity of Ligand Stabilized Copper Oxide Nanoparticles

Ligand stabilization can influence the surface chemistry of Cu oxide nanoparticles (NPs) and provide unique product distributions for electrocatalytic methanol (MeOH) oxidation and CO{sub 2} reduction reactions. Oleic acid (OA) stabilized Cu{sub 2}O and CuO NPs promote the MeOH oxidation reaction with 88% and 99.97% selective HCOH formation, respectively. Alternatively, CO{sub 2} is the only reaction product detected for bulk Cu oxides and Cu oxide NPs with no ligands or weakly interacting ligands. We also demonstrate that OA stabilized Cu oxide NPs can reduce CO{sub 2} into CO with a {approx}1.7-fold increase in CO/H{sub 2} production ratios compared to bulk Cu oxides. The OA stabilized Cu oxide NPs also show 7.6 and 9.1-fold increases in CO/H{sub 2} production ratios compared to weakly stabilized and non-stabilized Cu oxide NPs, respectively. Our data illustrates that the presence and type of surface ligand can substantially influence the catalytic product selectivity of Cu oxide NPs.

10 SYNTHETIC FUELS↗

DOE OSTI2012

EFFECTS OF VEGETATION ON TURBULENCE, SEDIMENT TRANSPORT AND STREAM MORPHOLOGY

Vegetation, from an individual stem to multiple stems in various configurations, profoundly alters turbulent flows. These alterations influence sediment transport and stream morphology, but depend on complex interactions and relationships between flow, plants and sediment properties. This is illustrated for three case studies that represent a variety of macrophyte patterns and scales in the environment: flows through simulated uniformly distributed plant stems, emergent and submerged; flows with alternating simulated stem patches; and flow around an isolated stem in a flood plain. The emergent case demonstrates that when density is sparse the mean velocity and turbulence intensities vary horizontally around the stems, which would promote a heterogeneous bedform morphology. However, it is still unclear how density, submergence ratio, and flow Reynolds number, in combination, influence interference effects, vortex shedding and dissipation, and velocity, pressure and lift fluctuations that affect sediment entrainment. The submerged case demonstrates significant reduction of the mean velocity, turbulence intensities, and turbulent shear near the bed compared to an unobstructed flow and supports numerous observations that vegetation promotes deposition or stabilizes bed sediments. The case of alternating emergent vegetation patches illustrates how vegetation adjusts the bed promoting scour in open water and deposition within the patches. The isolated stem case illustrates the variety of coherent structures generated, their complex interaction, and their role in specific sediment transport phenomena observed. Additional research is required, however, to quantify thresholds and relationships for flow-vegetation-sediment interactions so that aquatic macrophyte plantings can be used more effectively in water resource management.

42 ENGINEERING↗

DOE OSTI2016

Data Validation Package November 2015 Groundwater and Surface Water Sampling at the Old and New Rifle, Colorado, Processing Sites February 2016

Water samples were collected from 36 locations at New Rifle and Old Rifle, Colorado, Processing Sites. Duplicate samples were collected from New Rifle locations 0659 and 0855, and Old Rifle location 0304. One equipment blank was collected after decontamination of non-dedicated equipment used to collect one surface water sample. Sampling and analyses were conducted as specified in the Sampling and Analysis Plan for U.S. Department of Energy Office of Legacy Management Sites (LMS/PRO/S04351, continually updated). New Rifle Site Samples were collected at the New Rifle site from 16 monitoring wells and 7 surface locations in compliance with the December 2008 Groundwater Compliance Action Plan [GCAP] for the New Rifle, Colorado, Processing Site (LMS/RFN/S01920), with one exception: New Rifle location 0635 could not be sampled because it was inaccessible; a fence installed by the Colorado Department of Transportation prevents access to this location. DOE is currently negotiating access with the Colorado Department of Transportation. Analytes measured at the New Rifle site included contaminants of concern (COCs) (arsenic, molybdenum, nitrate + nitrite as nitrogen, selenium, uranium, and vanadium) ammonia as nitrogen, major cations, and major anions. Field measurements of total alkalinity, oxidation- reduction potential, pH, specific conductance, turbidity, and temperature were made at each location, and the water level was measured at each sampled well. A proposed alternate concentration limit (ACL) for vanadium of 50 milligrams per liter (mg/L), specific to the compliance (POC) wells (RFN-0217, -0659, -0664, and -0669) is included in the New Rifle GCAP. Vanadium concentrations in the POC wells were below the proposed ACL as shown in the time-concentration graphs in the Data Presentation section (Attachment 2). Time-concentration graphs from all other locations sampled are also included in Attachment 2. Sampling location RFN-0195 was misidentified for the June/August 2014 and November 2014 sampling events. (Well RFN-0609 was inadvertently sampled instead of RFN-0195 in 2014.) The results for RFN-0195 have been corrected, and are included in associated time-concentration graphs for this location. Recent results for RFN-0195 are consistent with established trends with the possible exception of vanadium. The most recent result for vanadium showed an increase over recent values. Vanadium concentrations at RFN-0195 and other locations will continue to be evaluated in the future to determine the potential for deviations from established trends. The surface water locations were sampled to monitor the impact of groundwater discharge. COC concentrations at Colorado River surface water locations RFN-0324 and RFN-0326, downgradient of the site, remained low and were consistent with historical results, as shown in the time-concentration graphs. COC concentrations did not indicate there are any impacts related to groundwater discharge to the river. In many cases, elevated COC concentrations at the New Rifle site pond locations were observed, as shown in the time-versus concentration graphs. As noted in the GCAP, this indicates impacts from groundwater discharge to the ponds. Old Rifle Site Samples were collected at the Old Rifle site from eight monitoring wells and five surface locations in compliance with the December 2001 Groundwater Compliance Action Plan for the Old Rifle, Colorado, UMTRA Project Site (GJ0-2000-177-TAR). Analytes measured at the Old Rifle site included COCs (selenium, uranium, and vanadium), major cations, and major anions. Field measurements of total alkalinity, oxidation-reduction potential, pH, specific conductance, turbidity, temperature, were made at each location, and the water level was measured at each sampled well. The monitoring strategy described in the GCAP is designed to determine progress of the natural flushing process in meeting compliance standards for site COCs. Standards for selenium and vanadium are the proposed ACLs of0.05 mg/L and 1.0 mg/L, respectively. For uranium the cleanup goal is the UMTRA standard of 0.044 mg/L or background, whichever is higher. As shown in the time concentration graphs, the uranium concentration exceeds the cleanup goal at groundwater monitoring locations RF0-0304, -0305, -0310, -0655, and -0656. The surface water locations were sampled to monitor the impact of groundwater discharge at Colorado River surface water locations adjacent to (RF0-0396) and downgradient of the site (RF0-0741). COC concentrations remain low and consistent with historical concentrations as shown in the time-concentration graphs (Attachment 2), which indicate no impacts from groundwater discharge to the river.

2015 Old and New Rifle↗

DOE OSTI2024

Delivering Clean Air in Denver: Propane Trucks and Infrastructure in Mail Delivery Application

In 2021, Drive Clean Colorado, a Denver-based Clean Cities coalition, initiated the deployment of five Class 6 medium-duty propane autogas delivery trucks into a United States Postal Service (USPS) mail delivery contractor fleet with the goal of providing a proof-of-concept demonstration for mail delivery fleets nationwide. Funded by the U.S. Department of Energy's Office of Energy Efficiency & Renewable Energy, the project, titled "Delivering Clean Air in Denver: Propane Trucks and Infrastructure in Mail Delivery Application," enabled the purchase and deployment of the propane-powered trucks, refueling infrastructure, and supporting analysis by the National Renewable Energy Laboratory (NREL). Key objectives of the analysis included calculating the propane vehicles' emissions reductions, analyzing the costs and operational performance of the propane fleet compared to conventional diesel-powered vehicles, and evaluating the viability of propane as a clean and cost-effective alternative to conventional diesel trucks (AFDC 2023b, 2023c). The primary goal of the project was to demonstrate alternative fuel vehicles in a mail transport application and evaluate the viability of propane as a clean and cost-effective alternative to conventional diesel trucks. This proof-of-concept demonstration is expected to lead to improved understanding of the performance attributes, costs, and operational issues to inform technology adoption decisions, helping to spur market transformation toward lower-emission truck fleets. By reducing the risk of first adoption, potential exists to transform the U.S. Postal Service (USPS) mail delivery system into a lower-carbon national fleet. This technical report details the vehicle duty cycle characterization and fleet cost and performance comparison performed by the National Renewable Energy Laboratory, in addition to estimated emissions reductions for delivery operations.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2023

IPL-Annealed Mixed-Cation Perovskites with Robust Coating Window toward Scalable Manufacturing of Commercial Perovskite Solar Cells

Perovskite solar cells (PSCs) are a promising alternative solar technology, but the technical challenges of (1) stability/durability, (2) efficiency at scale, and (3) manufacturability must be overcome to achieve widespread PSC commercialization. The challenge of balancing solution ink formulation and scalable manufacturing is often overlooked in the literature, where focus is on adopting inks from processes that will not scale. In this study, we apply a classical roll-to-roll manufacturing perspective, utilizing both compositional engineering and intense pulsed light (IPL) annealing, to develop a mixed-cation perovskite ink with a robust coating window that simultaneously solve issues of stability and manufacturability for PSCs. Our method resulted in blade-coated, flexible, mixed-cation PSCs on ITO-PET substrates with a champion power conversion efficiency (PCE) efficiency of 16.7% using IPL annealing of the absorber layer and, to our knowledge, is one of the fastest processing methods for the perovskite layer. This overall reduction in processing time with a stable ink represents an advance toward the scaled production of perovskite solar cells on flexible substrates.

flexible perovskite solar cells↗

DOE OSTI2011

Operating Reserve Implication of Alternative Implementations of an Energy Imbalance Service on Wind Integration in the Western Interconnection: Preprint

During the past few years, there has been significant interest in alternative ways to manage power systems over a larger effective electrical footprint. Large regional transmission organizations in the Eastern Interconnection have effectively consolidated balancing areas, achieving significant economies of scale that result in a reduction in required reserves. Conversely, in the WesternInterconnection there are many balancing areas, which will result in challenges if there is significant wind and solar energy development in the region. A recent proposal to the Western Electricity Coordinating Council suggests a regional energy imbalance service (EIS). To evaluate this EIS, a number of analyses are in process or are planned. This paper describes one part of an analysis of theEIS's implication on operating reserves under several alternative scenarios of the market footprint and participation. We improve on the operating reserves method utilized in the Eastern Wind Integration and Transmission Study and apply this modified approach to data from the Western Wind and Solar Integration Study.

17 WIND ENERGY↗