Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “coordinated optimization”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 1,441 records · Page 80
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Early stage structural development of prototypical zeolitic imidazolate framework (ZIF) in solution

Given the wide-ranging potential applications of metal organic frameworks (MOFs), an emerging imperative is to understand their formation with atomic scale precision. This will aid in designing syntheses for next-generation MOFs with enhanced properties and functionalities. Major challenges are to characterize the early-stage seeds, and the pathways to framework growth, which require synthesis coupled with in situ structural characterization sensitive to nanoscale structures in solution. Here we report measurements of an in situ synthesis of a prototypical MOF, ZIF-8, utilizing synchrotron X-ray atomic pair distribution function (PDF) analysis optimized for sensitivity to dilute species, complemented by mass spectrometry, electron microscopy, and density functional theory calculations. We observe that despite rapid formation of the crystalline product, a high concentration of Zn(2-MeIm) 4 (2-MeIm=2-methylimidazolate) initially forms and persists as stable clusters over long times. A secondary, amorphous phase also pervades during the synthesis, which has a structural similarity to the final ZIF-8 and may act as an intermediate to the final product.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2011

Mars Science Laboratory Entry Guidance

The Mars Science Laboratory will be the first Mars mission to attempt a guided entry with the objective of safely delivering the entry vehicle to a survivable parachute deploy state within 12.5 km of the pre-designated parachute deploy coordinates. The Entry Terminal Point Controller guidance algorithm is derived from the final phase Apollo Command Module guidance and, like Apollo, modulates the bank angle to control range based on deviations in range, altitude rate, and drag acceleration from a reference trajectory. For application to Mars landers which must make use of the tenuous Martian atmosphere, it is critical to balance the lift of the vehicle to minimize the range while still ensuring a safe deploy altitude. An overview of the process to generate optimized guidance settings is presented, discussing improvements made over the last nine years. Performance tradeoffs between ellipse size and deploy altitude will be presented, along with imposed constraints of entry acceleration and heating. Performance sensitivities to the bank reversal deadbands, heading alignment, attitude initialization error, and entry delivery errors are presented.

Mendeck, Gavin F.↗
DOE OSTI2020

Infrastructure and DFLAW Support at Hanford - 20443

Manhattan Project era infrastructure systems are degrading at an accelerated pace across the Department of Energy's (DOE) Environmental Management complex. Revitalizing, rejuvenating and right-sizing these systems to ensure reliability for ongoing cleanup missions is a major focus at the 580-square- mile Hanford Site in southeast Washington State. The push to complete construction, commissioning, startup, and operation of facilities and systems in the Direct-Feed Low-Activity Waste (DFLAW) program at Hanford by 2023 requires considerable coordination among site contractors and a significant investment in infrastructure. The passage of time also poses a challenge. It has been about 75 years since facilities were first operated at the site, and approximately 40 years of plutonium production created a legacy of unidentified active and abandoned underground obstacles and waste sites that must be avoided when building and upgrading the infrastructure. Converting infrastructure systems originally built to support plutonium production from the 1940's to the 1980's and upgrading those systems to optimize technology is an ever-changing balance of funding profiles, available resources and execution strategies. The DOE Richland Operations Office (RL) has long recognized the need for increased investment in Hanford Site infrastructure to support the future processing of approximately 56 million gallons of waste currently stored in large underground tanks. When DFLAW is fully operational, safe and reliable infrastructure systems will be needed to ensure continuity of operations around the clock, 365 days a year. These include roadways, water, power, sewer, information technology systems and facilities. To ensure the readiness of Hanford's infrastructure to support treating tank waste in the next three years, 15 projects were identified with a combined value of $133.8 million. Through calendar year 2019, 7 infrastructure projects have been substantially completed and the remaining 8 projects, with a remaining value of $103.8 million, are scheduled to be completed by December 2023. RL and its site services/infrastructure contractor, Mission Support Alliance (MSA), regularly evaluate the needs of the DFLAW program and other Hanford Site missions to ensure the highest priority systems are addressed. In addition to a fast-approaching deadline for round-the-clock treatment operations, RL and MSA face another significant infrastructure challenge. As cleanup is being completed in a 220-square-mile area called the River Corridor, most of the cleanup operations going forward will occur in a 20-square-mile area in the center of the Hanford Site, known as the Central Plateau. Infrastructure systems are becoming more congested in an already overcrowded area. This paper/presentation will outline some of the challenges Hanford faces while executing infrastructure reliability projects. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Load-balanced sparse MTTKRP on GPUs

Sparse matricized tensor times Khatri-Rao product (MT- TKRP) is one of the most computationally expensive kernels in sparse tensor computations. This work focuses on optimizing the MTTKRP for floating point operations, storage, and scalability. We begin by identifying the performance bottlenecks in directly extending the state-of-the-art CSF (compressed sparse fiber) formats from CPUs to GPUs. Our detailed analysis over the recently proposed formats shows that the lower bounds on storage and flop counts can vary significantly depending on the structure of the sparse tensor. To address this, we propose a load balanced, computation and storage-efficient scheme, HYB, which combines the best of COO (coordinate), CSF and CSL (compressed slice). With these enhancements, our GPU framework significantly out- performs the current formats on both CPU and GPU platforms.

Nisa, Israt↗
DOE OSTI2016

Metal oxide core shell nanostructures as building blocks for efficient light emission (SISGR)

The objective of this research is to synthesize core-shell nano-structured metal oxide materials and investigate their structural, electronic and optical properties to understand the microscopic pathways governing the energy conversion process, thereby controlling and improving their efficiency. Specifically, the goal is to use a single metal oxide core-shell nanostructure and a single excitation source to generate photons with long emission lifetime over the entire visible spectrum and when controlled at the right ratio, generating white light. In order to achieve this goal, we need to control the energy transfer between light emitting elements, which dictates the control of their interatomic spacing and spatial distribution. We developed an economical wet chemical process to form the nanostructured core and to control the thickness and composition of the shell layers. With the help from using DOE funded synchrotron radiation facility, we delineated the growth mechanism of the nano-structured core and the shell layers, thereby enhancing our understanding of structure-property relation in these materials. Using the upconversion luminescence and the lifetime measurements as effective feedback to materials sysnthes is and integration, we demonstrated improved luminescence lifetimes of the core-shell nano-structures and quantified the optimal core-multi-shell structure with optimum shell thickness and composition. We developed a rare-earths co-doped LaPO 4 core-multishell structure in order to produce a single white light source. It was decided that the mutli-shell method would produce the largest increase in luminescence efficiency while limiting any energy transfer that may occur between the dopant ions. All samples resulted in emission spectra within the accepted range of white light generation based on the converted CIE color coordinates. The white light obtained varied between warm and cool white depending on the layering architecture, allowing for the utilization into a wide range of applications. With DOE’s overall mandate to reduce the US’s dependence on rare-earth elements, this work demonstrated how to make every RE atom count toward white light generation by controlling their spatial distribution thereby significantly reducing the amount needed. This is one approach toward reducing the dependence on RE elements and the strategies we developed can be used in discovering RE-free systems. The project is of benefit to the general public as it improves the optical efficiency of these materials, while reducing US’s dependence on RE elements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

User-oriented Improvements in the MOOSE Framework in Support of Multiphysics Simulation

The Multiphysics Object-Oriented Simulation Environment (MOOSE) framework is a foundational capability used by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program to create over 15 different simulation tools for advanced nuclear reactors. Due to this ubiquity, improvements to the framework in support of modeling and simulation goals are critical to the program. These improvements can take many forms, including optimization, improved user experience, streamlined application programming interfaces (APIs), parallelism, and new capabilities. The work transcribed in this report was conducted in direct support of the simulation tools and has already been deployed or will be deployed in the coming months. The capabilities were implemented in the same order as they are covered in this report: chainable execution objects or executors, support for transfers between same-level applications in a coupling scheme, support for boundary/subdomain restricted transfers, support for transfers between applications with different coordinate or unit systems, support for MOOSE applications in the NEAMS Workbench, deployment of the MOOSE application of the Idaho National Laboratory (INL) high-performance computing (HPC) OnDemand platform, the addition of a triangular meshing library in libMesh, and increased support of face variables.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

Development of Advanced, Radiation Resistant, Optical-based Detector Technology for Future Experiments.

The primary objective of this project has been to advance the design of high-performance electromagnetic (EM) calorimeters for future particle physics experiments, to identify and measure the timing, position and energy of electrons, positrons and gamma rays, particularly in high-luminosity environments with intense radiation and pileup conditions. To meet such challenges, the proposed research has focused on the development of ultra-compact, radiation-hard calorimeter modules, to provide excellent timing, spatial, and energy resolution. The work aligns with the DOE’s Basic Research Needs (BRN) for High Energy Physics (HEP) Instrumentation and the research team contributes actively to the Coordinating Panel on Advanced Detectors (CPAD) RDC9 calorimetry collaboration in the USA and the European Committee on Future Accelerators (ECFA) DRD-CALO calorimetry collaboration at CERN, the European Laboratory for Particle Physics located in Geneva, Switzerland. The research builds on the RADiCAL (radiation-hard, ultra-compact) modular sampling calorimeter approach, developed by the research team, which employs dense and very bright optical materials such as LYSO:Ce scintillator plates that are interleaved with very dense tungsten plates to minimize detector size while optimizing performance. The modules are comparable in size to a human index finger, dimensionally 14 mm x 14 mm in cross section and 135 mm in length. And despite the small size, the structure is capable of providing excellent timing and energy resolution. This is facilitated through the use of specialized quartz capillaries filled with wavelength-shifting filaments, positioned at various depths along the length of a module, to collect and guide light signals to silicon photomultipliers (SiPMs) which detect and convert the optical signals to electronic signals for analysis. The primary goals of this project have been: (1) Achieve a timing resolution to σ t ≤ 30 ps for high-energy electrons and photons, important for their association with specific events produced in colliding-beam experiments and for the detection of decays-in-flight of long-lived particles. The project has achieved this goal in beam tests of a single RADiCAL module at CERN, during which a timing resolution of σ t = 27 ps was measured for electrons of energy E = 150 GeV. Based upon a mathematical fit to the data measured over a broad energy range from low energy to high energy, a resolution of σ t ≤ 18 ps has been estimated for electrons of very high (TeV) energy. From these measurements and with further expected technical improvements, the timing resolution should reach σ t ≤ 10 ps, important for searches for discovery physics in upcoming and future experiments. (2) Achieve an energy resolution of σ E / E ≤ 10% / $\sqrt{E}$. The project has yet to achieve this goal, but is close to it, having measured a value of σ E / E ≤ 15.9% / $\sqrt{E}$ using a modular array. Ultimately, the resolution goal is expected to be reached by adjustments to material thicknesses within the modules, which will improve the sampling fraction to measure more precisely the shower energy for lower energy particles. The versatility of the modular RADiCAL approach enables the testing of advanced materials, photosensors and electronics, developed in collaboration with CPAD RDC and ECFA DRD-CALO groups. The structure can distinguish electrons, positrons and gamma rays from hadrons and muons and beam-induced backgrounds, making it a valuable tool in a variety of detector environments, including future circular colliders (FCC-ee, FCC-hh) proposed for the European Laboratory for Particle Physics (CERN), the muon-collider proposed for Fermi National Accelerator Laboratory (Fermilab), and searches for new physics in beam-dump, fixed target and forward-physics experiments. And, while designed with particle physics applications in mind, the technologies developed in this project have the potential for application more broadly in particle and nuclear physics, materials science, and medical physics, underscoring the far-reaching potential of this line of instrumentation research and development.

47 OTHER INSTRUMENTATION↗
NASA NTRS1986

Engineering calculations for communications satellite systems planning

Observed solution times were analyzed for the extended gradient and cyclic coordinate search procedures. The times used in the analysis come from computer runs made during a previously-reported experiment conducted to assess the quality of the solutions to a BSS synthesis problem found by the two search methods. The results of a second experiment with a Fixed Satellite Service (FSS) test problem are also presented. Computational results are summarized for mixed integer programming approaches for solving FSS synthesis problems. A promising heuristic algorithm is described. A synthesis model is discussed for orbital arc allotment optimization. Research plans for the near future are also presented.

Reilly, C. H.↗
DOE OSTI2026

Agentic traffic intelligence: Augmented human-in-the-loop scenario generation for microscopic traffic simulation

Traditional microscopic traffic simulation generation often relies on static datasets and manual design, limiting its ability to simulate complex conditions easily. This paper presents a novel framework, Agentic Traffic Intelligence, which combines human approval large language models (LLMs), the Real-Twin tool, and multi-agent systems to perform realistic microscopic traffic simulation scenario generation. The proposed framework incorporates human-in-the-loop (HIL) control, retrieval-augmented generation (RAG), and multi-agent control mechanisms. HIL mechanisms are used to guide multiple LLMs focused on attributes for microscopic simulation generation and to improve the interpretability and transparency of LLM execution for users. RAG enhances context extraction by dynamically integrating external knowledge sources for traffic scenario generation foundations. A multi-agent architecture with supervisory control coordinates the interaction of simulation components, including traffic simulators, control logic, and calibration tools. This enables the synthesis of simulation-ready scenarios that reflect dynamic demand profiles and behavior controls. Furthermore, the framework fuses multisource traffic data with unstructured context and supports iterative refinement through interactive user feedback. Validated through microscopic simulation using Simulation of Urban Mobility, the generated scenarios demonstrate high-fidelity network generation with inflow and turn movement and behavioral calibration, offering a robust and efficient tool for stress-testing and optimizing urban mobility systems.

Hierarchical multi-agent control↗
DOE OSTI2024

Low-Temperature Activation and Coupling of Methane on MgO Nanostructures Embedded in Cu 2 O/Cu(111)

Here, the efficient conversion of methane into valuable hydrocarbons such as ethane and ethylene at relatively low temperatures without deactivation issues is crucial for advancing sustainable energy solutions. Herein, AP-XPS and STM studies show that MgO nanostructures (0.2-0.5 nm wide, 0.4-0.6 Å high) embedded in a Cu 2 O/Cu(111) substrate activate methane at room temperature, mainly dissociating it into CH x (x = 2 or 3) and H adatoms, with minimal conversion to C adatoms. These MgO nanostructures in contact with Cu 2 O/Cu(111) exhibit unique reactivity, enabling C-C coupling into ethane and ethylene at 500 K, a significantly lower temperature than that required for bulk MgO catalysts (>700 K), with negligible carbon deposition and no deactivation. DFT calculations corroborate these experimental findings. The CH 4,gas → *CH 3 +*H reaction is a downhill process on MgO/Cu 2 O/Cu(111) surfaces. The activation of methane is facilitated by an electron transfer from copper to MgO and the existence of Mg and O atoms with a low coordination number in the oxide nanostructures. The formation of O-CH 3 and O-H bonds overcomes the energy necessary for the cleavage of a C-H bond in methane. DFT studies reveal that smaller Mg 2 O 2 model clusters provide stronger binding and lower activation barriers for C-H dissociation in CH 4 , while larger Mg 3 O 3 clusters promote C-C coupling due to weaker *CH 3 binding. All these results emphasize the importance of size when optimizing the catalytic performance of MgO nanostructures in the selective conversion of methane.

36 MATERIALS SCIENCE↗
NASA NTRS2004

NASA Tech Briefs, October 2004

Topics include: Relative-Motion Sensors and Actuators for Two Optical Tables; Improved Position Sensor for Feedback Control of Levitation; Compact Tactile Sensors for Robot Fingers; Improved Ion-Channel Biosensors; Suspended-Patch Antenna With Inverted, EM-Coupled Feed; System Would Predictively Preempt Traffic Lights for Emergency Vehicles; Optical Position Encoders for High or Low Temperatures; Inter-Valence-Subband/Conduction-Band-Transport IR Detectors; Additional Drive Circuitry for Piezoelectric Screw Motors; Software for Use with Optoelectronic Measuring Tool; Coordinating Shared Activities; Software Reduces Radio-Interference Effects in Radar Data; Using Iron to Treat Chlorohydrocarbon-Contaminated Soil; Thermally Insulating, Kinematic Tensioned-Fiber Suspension; Back Actuators for Segmented Mirrors and Other Applications; Mechanism for Self-Reacted Friction Stir Welding; Lightweight Exoskeletons with Controllable Actuators; Miniature Robotic Submarine for Exploring Harsh Environments; Electron-Spin Filters Based on the Rashba Effect; Diffusion-Cooled Tantalum Hot-Electron Bolometer Mixers; Tunable Optical True-Time Delay Devices Would Exploit EIT; Fast Query-Optimized Kernel-Machine Classification; Indentured Parts List Maintenance and Part Assembly Capture Tool - IMPACT; An Architecture for Controlling Multiple Robots; Progress in Fabrication of Rocket Combustion Chambers by VPS; CHEM-Based Self-Deploying Spacecraft Radar Antennas; Scalable Multiprocessor for High-Speed Computing in Space; and Simple Systems for Detecting Spacecraft Meteoroid Punctures.

Source record↗
NASA NTRSDate not supplied

Space Radiation Technologies for Human Missions beyond Low-Earth-Orbit

Ionizing radiation exposure is a pervasive occupational risk to astronauts and remains a major health risk associated with human exploration beyond low-Earth-orbit. Sustained lunar and Mars exploration crew will be at increased risk of radiogenic cancers and cardiovascular disease, as well as, the potential for in-mission performance decrements, immune system decrements, and late neurodegenerative conditions impacting crew health. Optimizing astronaut space radiation protection will incorporate both physical and biological radiological aspects and will implement protection strategies that span pre-mission, in-flight, and post mission timelines. Major facets of physical risk mitigation include accuracy in predicting the space radiation solar environment, monitoring environmental and human exposures, and minimizing exposure through vehicle shielding and design. Biological mitigation facets include understanding and predicting biological response to the space environment, developing advanced medical countermeasures, and identifying appropriate surveillance strategies to preserve long-term health. Coordinated investments in these major capability areas will support development of an integrated radiation protection solution to minimize astronaut risk for moon to Mars exploration missions.

Lisa C Simonsen↗
DOE OSTI2018

Florida International University Research on Soil and Groundwater Contamination at DOE's Hanford and Savannah River Sites - 18547

Nuclear weapons production and other defense-related activities at U.S. Department of Energy (DOE) sites have resulted in radionuclide and heavy metal contamination in surface and subsurface environments nationwide. The DOE Office of Environmental Management (DOE EM) faces a number of environmental challenges that are technically complex and unique to EM with tremendous associated cleanup costs. The success of the DOE EM mission will require development and insertion of innovative approaches and novel technologies to address the significant challenges associated with the remaining cleanup of contaminated sites. A key focus of the applied research portfolio addresses data gaps related to the behavior and chemistry of radionuclides of concern as well as the co-mingling of these contaminants in groundwater at EM sites such as Hanford, Savannah River, Oak Ridge and others. Florida International University (FIU) is conducting research in conjunction with Pacific Northwest National Laboratory (PNNL) and savannah River National Laboratory (SRNL) scientists to support environmental remediation efforts at Hanford and SRS. This research is focused on remediation technologies for contaminated soil and groundwater as well as the assessment of the fate and transport of contaminants in the environment. The overall objective is to reduce contaminant mobility through the development and application of state-of-the-art scientific and environmental remediation technologies. The FIU strategy is to conduct basic science research that fills knowledge gaps and complements work conducted at DOE sites. Support to Hanford includes contributing to the understanding of {sup 99}Tc chemistry and the fate and transport mechanisms of co-mingled contaminants including {sup 99}Tc, U(VI), Cr, and iodine (I). FIU has also provided basic science research that supports a treatability study currently underway at Hanford, which uses ammonia gas injection to manipulate pH and immobilize U(VI) in the subsurface. In addition, support for long-term monitored natural attenuation is provided through geophysical research that monitors subsurface contaminant and microbial responses. Research to evaluate the environmental factors that control the fate and transport of contaminants and co-contaminants in soil and groundwater is being performed for SRS. This research has contributed to the development, design, and deployment of innovative strategies to enhance the natural attenuation processes and to validate novel in situ remediation technologies. The SRS EM test bed demonstrations directly benefit SRS cleanup initiatives. Current investigations focus on natural organic compounds, such as humate, as a potential amendment for the treatment of uranium in groundwater associated with the SRS F-Area Seepage Basins plume, investigates the synergy between humate and silica to optimize the pH adjustment strategy for uranium remediation and investigates the interaction of Tc and I with soil from the Four Mile Branch wetland. Collaborative relationships between FIU and the national laboratories have provided synergy and benefits over the years to FIU, the national laboratories, the DOE complex, and the DOE EM mission. By working closely with the national laboratories, FIU research is not only closely aligned with the cleanup mission priorities at the DOE sites, but complements and supports the work at national laboratories. This coordination and leveraging of research efforts results in time- and cost-savings, and accelerates progress in the DOE EM environmental restoration mission. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Synthesis of fluorescent core-shell nanomaterials and strategies to generate white light

In this work, cadmium free core-shell ZnS:X/ZnS (X = Mn, Cu) nanoparticles have been synthesized and used for white light generation. First, the doping concentration of Manganese (Mn) was varied from 1% to 4% to optimize the dopant related emission and its optimal value was found to be 1%. Then, ZnS shell was grown over ZnS:Mn(1%) core to passivate the surface defects. Similarly, the optimal concentration of Copper (Cu) was found to be 0.8% in the range varied from 0.6% to 1.2%. In order to obtain an emission in the whole visible spectrum, dual doping of Mn and Cu was done in the core and the shell, respectively. A solid-solid mixing in different ratios of separately doped quantum dots (QDs) emitting in the blue green and the orange region was performed. Results show that the optimum mixture of QDs excited at 300 nm gives Commission Internationale del'Éclairage color coordinates of (0.35, 0.36), high color rendering index of 88, and correlated color temperature of 4704 K with minimum self-absorption.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Effects of surface charge and cluster size on the electrochemical dissolution of platinum nanoparticles using COMB3 and continuum electrolyte models

We study the site-dependent dissolution of platinum nanoparticles under electrochemical conditions to assess their thermodynamic stability as a function of shape and size using empirical molecular dynamics and electronic-structure models. The third-generation charge optimized many-body potential is employed to determine the validity of uniform spherical representations of the nanoparticles in predicting dissolution potentials (the Kelvin model). To understand the early stages of catalyst dissolution, implicit solvation techniques based on the self-consistent continuum solvation method are applied. It is demonstrated that interfacial charge and polarization can shift the dissolution energies by amounts on the order of 0.74 eV depending on the surface site and nanoparticle shape, leading to the unexpected preferential removal of platinum cations from highly coordinated sites in some cases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1991

Range optimization for a supersonic aircraft

Range optimal trajectories for an aircraft flying in the vertical plane are obtained from Pontryagin's Minimum Principle. Control variables are load factor n which appears nonlinearly in the equations of motion and throttle setting eta, which appears only linearly. Both controls are subject to fixed bounds, namely eta between values of 0 and 1 and absolute value of n not greater than n(max). Additionally, a dynamic pressure limit is imposed, which represents a first-order state-inequality constraint. For fixed flight time, fixed initial coordinates, and partially fixed final coordinates, the effect of the load factor limit absolute value of n not greater than n(max) is studied. Upon varying n(max), six different switching structures are obtained. All trajectories involve singular control along arcs with active dynamic pressure limit.

Seywald, Hans↗
DOE OSTI2020

Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts

Abstract Atomically dispersed and nitrogen coordinated single metal sites (M‐N‐C, M=Fe, Co, Ni, Mn) are the popular platinum group‐metal (PGM)‐free catalysts for many electrochemical reactions. Traditional wet‐chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M‐N‐C catalysts. The deposition of gaseous 2‐methylimidazole onto M‐doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD‐derived Fe‐N‐C catalyst exclusively contains atomically dispersed FeN 4 sites with increased Fe loading relative to other catalysts from wet‐chemistry synthesis. The catalyst exhibited outstanding oxygen‐reduction activity in acidic electrolytes, which was further studied in proton‐exchange membrane fuel cells with encouraging performance.

Liu, Shengwen↗
DOE OSTI2024

Critical role of solvation on CC13 porous organic cages for design of porous liquids

Efficient carbon capture requires the design of new materials with high CO 2 selectivity and gas adsorption capacity that can be incorporated into existing industrial processes. Porous liquids (PLs) are promising candidate materials that consist of a nanoporous host and a solvent forming a liquid with permanent porosity based on exclusion of the solvent from the interior of the nanoporous host. Stable PLs are based on solvent-nanoporous host interactions, which can be evaluated through molecular simulations. Here, time- and temperature-dependent density functional theory simulations were performed between four solvents, 2-bromophenol, 4-methylphenol, 2,4-dimethylphenol, and cyclohexanone and the CC13 porous organic cage (POC) as a prototypical PL composition. Overall, minimal reactions occurred in the PL including no changes in the POC structure. Additionally, POC-solvent coordination occurred through interactions of neighboring functional groups such as methyl/bromide and hydroxyl on the solvent molecules with the POC surface. Therefore, the location rather than the number of functional groups on the solvent molecule controls the POC-solvent interactions. Additionally, the POC pore window contracted or expanded up to 8% during solvation, which correlates with the experimental solubility and static solvent-POC binding, where solvents that caused less contraction of the POC pore window increased POC solubility. Finally, these results allow for the design of optimized POC-based PL compositions based on solvent-nanoporous host binding and variation in the pore window during solvation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗