Results for “coordination complexes” — Page 61

DOE OSTI2022

Dilute Alloys Based on Au, Ag, or Cu for Efficient Catalysis: From Synthesis to Active Sites

The development of new catalyst materials for energy-efficient chemical synthesis is critical as over 80% of industrial processes rely on catalysts, with many of the most energy-intensive processes specifically using heterogeneous catalysis. Catalytic performance is a complex interplay of phenomena involving temperature, pressure, gas composition, surface composition and structure over multiple length and time scales. In response to this complexity, the integrated approach to heterogeneous dilute-alloy catalysis reviewed here brings together materials synthesis, mechanistic surface chemistry, reaction kinetics, in-situ and operando characterization, and theoretical calculations in a coordinated effort to develop design principles to predict and improve catalytic selectivity. Dilute alloy catalysts—in which isolated atoms or small ensembles of the minority metal on the host metal lead to enhanced reactivity while retaining selectivity—are particularly promising as selective catalysts. Several dilute alloy materials using Au, Ag and Cu as the majority host element, including more recently introduced support-free nanoporous metals and oxide-supported nanoparticle "raspberry colloid templated (RCT)" materials, are reviewed for selective oxidation and hydrogenation reactions. Progress in understanding how such dilute alloy catalysts can be used to enhance selectivity of key synthetic reactions is reviewed, including quantitative scaling from model studies to catalytic conditions. The dynamic evolution of catalyst structure and composition studied in surface science and catalytic conditions and their relationship to catalytic function are also discussed, followed by advanced characterization and theoretical modeling that have been developed to determine the distribution of minority metal atoms at or near the surface. Furthermore, the integrated approach demonstrates the success of bridging the divide between fundamental knowledge and design of catalytic processes in complex catalytic systems, which can accelerate the development of new and efficient catalytic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Ligand-coordinated Ir single-atom catalysts stabilized on oxide supports for ethylene hydrogenation and their evolution under a reductive atmosphere

In this work, we present a novel series of oxide-supported Ir-ligand single-atom catalysts (SACs) for ethylene hydrogenation. The SACs were created by a metal–ligand self-assembly strategy developed by our group, using one of two ligands, either 1,10-phenanthroline-5,6-dione (PDO) or 3,6-Di-2-pyridyl-1,2,4,5-tetrazine (DPTZ), on powder supports of either CeO 2 or MgO. Characterization by XAS, XPS, and CO adsorption proved that Ir exist principally as highly uniform, cationic single-atoms. Ir SACs show significantly higher durability and metal utilization efficiency than Ir nanoparticle (NP) catalysts during ethylene hydrogenation at 100 °C, as well as excellent stability, as no Ir aggregates were detected after >10 h reaction. The activity can be tuned by ligand and support effects: PDO and CeO 2 are superior to DPTZ and MgO, respectively. This tunability is attributed to differences in H 2 activation capability, which results from differences in support reducibility, electron density on Ir, and, potentially, the local coordination environment of Ir. The Ir SACs lose H 2 activation activity either under inert gas or under H 2 . Through XPS and in situ XAS studies, we attributed the former to the reversible loss of Ir hydride, which is the active species for H 2 activation, and the latter to irreversible over-hydrogenation and loss of Ir–O/N coordination. This work presents a new type of Ir hydrogenation SACs that are more durable, efficient, and tunable than supported Ir NPs, while more stable than homogeneous Ir complexes. It also offers fundamental understanding regarding ligand and support effects, as well as the evolution of Ir single-atoms under H 2 , instructing future design of stable, effective hydrogenation SACs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Derivative-free stochastic optimization via adaptive sampling strategies

In this paper, we present a novel derivative-free framework for solving unconstrained stochastic optimization problems. Many problems in fields ranging from simulation optimization to reinforcement learning to quantum computing involve settings where only stochastic function values are obtained via a zeroth-order oracle, which has no available gradient information and necessitates the usage of derivative-free optimization methodologies. Our approach includes estimating gradients using stochastic function evaluations and integrating adaptive sampling techniques to control the accuracy in these stochastic approximations. Our framework encapsulates several gradient estimation techniques, including standard finite-difference, Gaussian smoothing, sphere smoothing, randomized coordinate finite-difference, and randomized subspace finite-difference methods. We provide theoretical convergence guarantees for our framework and analyze the worst-case iteration and sample complexities associated with each gradient estimation method. Finally, we demonstrate the empirical performance of the methods on logistic regression and nonlinear least squares problems.

Adaptive sampling↗

DOE OSTI2024

Opportunities for fundamental physics research with radioactive molecules

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this paper, we review the scientific case for studying radioactive molecules, discuss recent atomic, molecular, nuclear, astrophysical, and chemical advances which provide the foundation for their study, describe the facilities where these species are and will be produced, and provide an outlook for the future of this nascent field.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

An interaction network in the polymerase active site is a prerequisite for Watson-Crick base pairing in Pol γ

The replication accuracy of DNA polymerase gamma (Pol γ) is essential for mitochondrial genome integrity. Mutation of human Pol γ arginine-853 has been linked to neurological diseases. Although not a catalytic residue, Pol γ arginine-853 mutants are void of polymerase activity. To identify the structural basis for the disease, we determined a crystal structure of the Pol γ mutant ternary complex with correct incoming nucleotide 2'-deoxycytidine 5'-triphosphate (dCTP). Opposite to the wild type that undergoes open-to-closed conformational changes when bound to a correct nucleotide that is essential for forming a catalytically competent active site, the mutant complex failed to undergo the conformational change, and the dCTP did not base pair with its Watson-Crick complementary templating residue. Our studies revealed that arginine-853 coordinates an interaction network that aligns the 3'-end of primer and dCTP with the catalytic residues. Disruption of the network precludes the formation of Watson-Crick base pairing and closing of the active site, resulting in an inactive polymerase.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Predictive analytics to direct clinical attention to complex patients with elevated suicide risk: enhancement of the Veterans Health Administration REACH VET model

Suicide is a major public health concern, particularly among Veterans. The U.S. Department of Veterans Affairs Veterans Health Administration (VHA) employs the Recovery Engagement and Coordination for Health–Veterans Enhanced Treatment (REACH VET) model to prioritise high-risk patients for targeted clinical attention. REACH VET 1.0 (RV 1.0) was developed on 2008–2011 data. To reflect changes in clinical practice and populations, VHA updated it to REACH VET 2.0 (RV 2.0). This study describes its development and validation. RV 2.0 used longitudinal data from 7,248,170 VHA patients (4,967 suicide deaths) in 2018–2019, with 650 time-varying demographic, clinical and area-level predictors derived from a 2-year lookback (2016–2019). An ensemble of Elastic-Net logistic regression models was trained on 2018 data and evaluated monthly at the population level in 2019, focusing on the top 0.1% intervention risk tier. Analyses assessed model discrimination, suicide detection, risk concentration, subgroup consistency (sex, age and race/ethnicity) and performance relative to RV 1.0 using the same percentile-based risk strata. RV 2.0 outperformed RV 1.0 across all risk strata, with better discrimination (C-statistic 0.76 vs 0.69) and consistent performance across demographic subgroups. Within the top 0.1% of predicted risk, RV 2.0 identified more deaths, higher suicide rates and greater mortality risk concentration both when averaged across the 12 monthly 2019 test sets (5.6 vs 3.6; 83.6 vs 53.7 per 100,000 person-years; 21.0 vs 14.1) and when annualised for 2019 (67 vs 43; 2.7% vs 1.7%; 1,003 vs 644 per 100,000 person-years; 26.7 vs 17.1). RV 2.0 improves suicide risk stratification among Veterans, demonstrating better performance and consistent prediction across subgroups and highlighting the need for regular model updates and evaluation.

Peluso, Alina [Oak Ridge National Laboratory (ORNL↗

DOE OSTI2021

Nuclear Material Process Modeling at the Y-12 National Security Complex

Dynamic simulation modeling is used at Y-12 to evaluate and forecast nuclear material inventories and production capacities to ensure that future supply can meet mission demand. Model outputs are analyzed by numerous Y-12 organizations and programs and coordinated with NNSA’s Office of Secondary Stage Production Modernization. Data-driven decisions for both short-term and long-term strategic planning for Y-12 mission execution are informed by the model. Dynamic simulation modeling capabilities for Y-12 nuclear material production continue to be expanded and refined.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Architecting the Grid Edge: Ensuring Reliability and Resilience

Changes in technology, customer expectations, and business and regulatory environments are rapidly evolving causing fundamental changes in the nation’s electrical infrastructure. Nowhere is this more apparent that at the “grid edge”, where there is an increasing number of new devices and systems, as well as complex new interactions between them. This is leading to the traditional relationship between the end-use customers and their utilities being expanded by an increasing number of stakeholders, each with their own operational and financial objectives, governed by regulatory policy. While there are concerns about the rapidly increasing complexity negatively impacting reliable and resilience of the electrical infrastructure, these changes are also bringing new resources and opportunities that hold great potential if they can be properly coordinated. This white paper outlines the considerations for the coordination of multi-stakeholder objectives with electric utility requirements using the concept of grid services. Describing a framework that enables new stakeholders to achieve their local technical and economic objectives, while simultaneously delivering operational benefits to the electrical infrastructure. The concepts of grid architecture are presented as a tool to evaluate how stakeholders might participate in, and benefit from, services, and how utilities can make decision on the reliance on services to ensure reliability and resilience, translating abstract concepts into actionable information for utilities and grid edge stakeholders. The end result of proper coordination, informed by grid architecture, will be a range of new devices and systems, operated by new stakeholders, achieving their local objectives while also increasing the reliability, resilience, security, and affordability of the nation’s critical electrical infrastructure.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2025

Architecting the Grid Edge: Ensuring Reliability and Resilience

Changes in technology, customer expectations, and business and regulatory environments are rapidly evolving causing fundamental changes in the nation’s electrical infrastructure. Nowhere is this more apparent that at the “grid edge”, where there is an increasing number of new devices and systems, as well as complex new interactions between them. This is leading to the traditional relationship between the end-use customers and their utilities being expanded by an increasing number of stakeholders, each with their own operational and financial objectives, governed by regulatory policy. While there are concerns about the rapidly increasing complexity negatively impacting reliable and resilience of the electrical infrastructure, these changes are also bringing new resources and opportunities that hold great potential if they can be properly coordinated. This white paper outlines the considerations for the coordination of multi-stakeholder objectives with electric utility requirements using the concept of grid services. Describing a framework that enables new stakeholders to achieve their local technical and economic objectives, while simultaneously delivering operational benefits to the electrical infrastructure. The concepts of grid architecture are presented as a tool to evaluate how stakeholders might participate in, and benefit from, services, and how utilities can make decision on the reliance on services to ensure reliability and resilience, translating abstract concepts into actionable information for utilities and grid edge stakeholders. The end result of proper coordination, informed by grid architecture, will be a range of new devices and systems, operated by new stakeholders, achieving their local objectives while also increasing the reliability, resilience, security, and affordability of the nation’s critical electrical infrastructure.

24 POWER TRANSMISSION AND DISTRIBUTION↗

NASA NTRS1989

NASA-Enhanced Version Of Automatically Programmed Tool Software (APT)

APT code one of most widely used software tools for complex numerically-controlled machining. Both a programming language and software that processes language. Upgrades include super pocket for concave polygon pockets and editor to reprocess cutter location coordinates according to user-supplied commands.

Purves, L. R.↗

NASA NTRS1989

Integrated aerodynamic-structural design of a forward-swept transport wing

The introduction of composite materials is having a profound effect on aircraft design. Since these materials permit the designer to tailor material properties to improve structural, aerodynamic and acoustic performance, they require an integrated multidisciplinary design process. Futhermore, because of the complexity of the design process, numerical optimization methods are required. The utilization of integrated multidisciplinary design procedures for improving aircraft design is not currently feasible because of software coordination problems and the enormous computational burden. Even with the expected rapid growth of supercomputers and parallel architectures, these tasks will not be practical without the development of efficient methods for cross-disciplinary sensitivities and efficient optimization procedures. The present research is part of an on-going effort which is focused on the processes of simultaneous aerodynamic and structural wing design as a prototype for design integration. A sequence of integrated wing design procedures has been developed in order to investigate various aspects of the design process.

Haftka, Raphael T.↗

NASA NTRS2005

Critical Propulsion Components: Exhaust Nozzle - Volume 3

Several studies have concluded that a supersonic aircraft, if environmentally acceptable and economically viable, could successfully compete in the 21st century marketplace. However, before industry can commit to what is estimated as a 15 to 20 billion dollar investment, several barrier issues must be resolved. In an effort to address these barrier issues, NASA and Industry teamed to form the High-Speed Research (HSR) program. As part of this program, the Critical Propulsion Components (CPC) element was created and assigned the task of developing those propulsion component technologies necessary to: (1) reduce cruise emissions by a factor of 10 and (2) meet the ever-increasing airport noise restrictions with an economically viable propulsion system. The CPC-identified critical components were ultra-low emission combustors, low-noise/high-performance exhaust nozzles, low-noise fans, and stable/high-performance inlets. Propulsion cycle studies (coordinated with NASA Langley Research Center sponsored airplane studies) were conducted throughout this CPC program to help evaluate candidate components and select the best concepts for the more complex and larger scale research efforts. The propulsion cycle and components ultimately selected were a mixed-flow turbofan (MFTF) engine employing a lean, premixed, prevaporized (LPP) combustor coupled to a two-dimensional mixed compression inlet and a two-dimensional mixer/ejector nozzle. Due to the large amount of material presented in this report, it was prepared in four volumes; Volume 1: Summary, Introduction, and Propulsion System Studies, Volume 2: Combustor, Volume 3: Exhaust Nozzle, and Volume 4: Inlet and Fan/Inlet Acoustic Team.

Source record↗

NASA NTRS2005

Critical Propulsion Components: Inlet and Fan/Inlet Accoustics Team - Volume 4

Several studies have concluded that a supersonic aircraft, if environmentally acceptable and economically viable, could successfully compete in the 21st century marketplace. However, before industry can commit to what is estimated as a 15 to 20 billion dollar investment, several barrier issues must be resolved. In an effort to address these barrier issues, NASA and Industry teamed to form the High-Speed Research (HSR) program. As part of this program, the Critical Propulsion Components (CPC) element was created and assigned the task of developing those propulsion component technologies necessary to: (1) reduce cruise emissions by a factor of 10 and (2) meet the ever-increasing airport noise restrictions with an economically viable propulsion system. The CPC-identified critical components were ultra-low emission combustors, low-noise/high-performance exhaust nozzles, low-noise fans, and stable/high-performance inlets. Propulsion cycle studies (coordinated with NASA Langley Research Center sponsored airplane studies) were conducted throughout this CPC program to help evaluate candidate components and select the best concepts for the more complex and larger scale research efforts. The propulsion cycle and components ultimately selected were a mixed-flow turbofan (MFTF) engine employing a lean, premixed, prevaporized (LPP) combustor coupled to a two-dimensional mixed compression inlet and a two-dimensional mixer/ejector nozzle. Due to the large amount of material presented in this report, it was prepared in four volumes; Volume 1: Summary, Introduction, and Propulsion System Studies, Volume 2: Combustor, Volume 3: Exhaust Nozzle, and Volume 4: Inlet and Fan/Inlet Acoustic Team.

Source record↗

NASA NTRS2005

Critical Propulsion Components: Summary, Introduction, and Propulsion Systems Studies - Volume 1

Several studies have concluded that a supersonic aircraft, if environmentally acceptable and economically viable, could successfully compete in the 21st century marketplace. However, before industry can commit to what is estimated as a 15 to 20 billion dollar investment, several barrier issues must be resolved. In an effort to address these barrier issues, NASA and Industry teamed to form the High-Speed Research (HSR) program. As part of this program, the Critical Propulsion Components (CPC) element was created and assigned the task of developing those propulsion component technologies necessary to: (1) reduce cruise emissions by a factor of 10 and (2) meet the ever-increasing airport noise restrictions with an economically viable propulsion system. The CPC-identified critical components were ultra-low emission combustors, low-noise/high-performance exhaust nozzles, low-noise fans, and stable/high-performance inlets. Propulsion cycle studies (coordinated with NASA Langley Research Center sponsored airplane studies) were conducted throughout this CPC program to help evaluate candidate components and select the best concepts for the more complex and larger scale research efforts. The propulsion cycle and components ultimately selected were a mixed-flow turbofan (MFTF) engine employing a lean, premixed, prevaporized (LPP) combustor coupled to a two-dimensional mixed compression inlet and a two-dimensional mixer/ejector nozzle. Due to the large amount of material presented in this report, it was prepared in four volumes; Volume 1: Summary, Introduction, and Propulsion System Studies, Volume 2: Combustor, Volume 3: Exhaust Nozzle, and Volume 4: Inlet and Fan/ Inlet Acoustic Team.

Source record↗

NASA NTRS2005

Critical Propulsion Components: Combustor - Volume 2

Several studies have concluded that a supersonic aircraft, if environmentally acceptable and economically viable, could successfully compete in the 21st century marketplace. However, before industry can commit to what is estimated as a 15 to 20 billion dollar investment, several barrier issues must be resolved. In an effort to address these barrier issues, NASA and Industry teamed to form the High-Speed Research (HSR) program. As part of this program, the Critical Propulsion Components (CPC) element was created and assigned the task of developing those propulsion component technologies necessary to: (1) reduce cruise emissions by a factor of 10 and (2) meet the ever-increasing airport noise restrictions with an economically viable propulsion system. The CPC-identified critical components were ultra-low emission combustors, low-noise/high-performance exhaust nozzles, low-noise fans, and stable/high-performance inlets. Propulsion cycle studies (coordinated with NASA Langley Research Center sponsored airplane studies) were conducted throughout this CPC program to help evaluate candidate components and select the best concepts for the more complex and larger scale research efforts. The propulsion cycle and components ultimately selected were a mixed-flow turbofan (MFTF) engine employing a lean, premixed, prevaporized (LPP) combustor coupled to a two-dimensional mixed compression inlet and a two-dimensional mixer/ejector nozzle. Due to the large amount of material presented in this report, it was prepared in four volumes; Volume 1: Summary, Introduction, and Team. Propulsion System Studies, Volume 2: Combustor, Volume 3: Exhaust Nozzle, and Volume 4: Inlet and Fan/Inlet Acoustic Team.

Source record↗

NASA NTRS2009

Synthesis and Control of Flexible Systems with Component-Level Uncertainties

An efficient and computationally robust method for synthesis of component dynamics is developed. The method defines the interface forces/moments as feasible vectors in transformed coordinates to ensure that connectivity requirements of the combined structure are met. The synthesized system is then defined in a transformed set of feasible coordinates. The simplicity of form is exploited to effectively deal with modeling parametric and non-parametric uncertainties at the substructure level. Uncertainty models of reasonable size and complexity are synthesized for the combined structure from those in the substructure models. In particular, we address frequency and damping uncertainties at the component level. The approach first considers the robustness of synthesized flexible systems. It is then extended to deal with non-synthesized dynamic models with component-level uncertainties by projecting uncertainties to the system level. A numerical example is given to demonstrate the feasibility of the proposed approach.

Maghami, Peiman G.↗

NASA NTRS2012

Cloud Computing for Mission Design and Operations

The space mission design and operations community already recognizes the value of cloud computing and virtualization. However, natural and valid concerns, like security, privacy, up-time, and vendor lock-in, have prevented a more widespread and expedited adoption into official workflows. In the interest of alleviating these concerns, we propose a series of guidelines for internally deploying a resource-oriented hub of data and algorithms. These guidelines provide a roadmap for implementing an architecture inspired in the cloud computing model: associative, elastic, semantical, interconnected, and adaptive. The architecture can be summarized as exposing data and algorithms as resource-oriented Web services, coordinated via messaging, and running on virtual machines; it is simple, and based on widely adopted standards, protocols, and tools. The architecture may help reduce common sources of complexity intrinsic to data-driven, collaborative interactions and, most importantly, it may provide the means for teams and agencies to evaluate the cloud computing model in their specific context, with minimal infrastructure changes, and before committing to a specific cloud services provider.

cloud computing↗

NASA NTRS2012

Development of Waypoint Planning Tool in Response to NASA Field Campaign Challenges

Airborne real time observations are a major component of NASA's Earth Science research and satellite ground validation studies. For mission scientists, planning a research aircraft mission within the context of meeting the science objectives is a complex task because it requires real time situational awareness of the weather conditions that affect the aircraft track. Multiple aircrafts are often involved in NASA field campaigns. The coordination of the aircrafts with satellite overpasses, other airplanes and the constantly evolving, dynamic weather conditions often determines the success of the campaign. A flight planning tool is needed to provide situational awareness information to the mission scientists, and help them plan and modify the flight tracks. Scientists at the University of Alabama-Huntsville and the NASA Marshall Space Flight Center developed the Waypoint Planning Tool, an interactive software tool that enables scientists to develop their own flight plans (also known as waypoints) with point -and-click mouse capabilities on a digital map filled with real time raster and vector data. The development of this Waypoint Planning Tool demonstrates the significance of mission support in responding to the challenges presented during NASA field campaigns. Analysis during and after each campaign helped identify both issues and new requirements, and initiated the next wave of development. Currently the Waypoint Planning Tool has gone through three rounds of development and analysis processes. The development of this waypoint tool is directly affected by the technology advances on GIS/Mapping technologies. From the standalone Google Earth application and simple KML functionalities, to Google Earth Plugin and Java Web Start/Applet on web platform, and to the rising open source GIS tools with new JavaScript frameworks, the Waypoint Planning Tool has entered its third phase of technology advancement. The newly innovated, cross ]platform, modular designed JavaScript ]controlled Way Point Tool is planned to be integrated with NASA Airborne Science Mission Tool Suite. Adapting new technologies for the Waypoint Planning Tool ensures its success in helping scientists reach their mission objectives. This presentation will discuss the development processes of the Waypoint Planning Tool in responding to field campaign challenges, identify new information technologies, and describe the capabilities and features of the Waypoint Planning Tool with the real time aspect, interactive nature, and the resultant benefits to the airborne science community.

He, Matt↗