Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Performance Tuning”

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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
NASA NTRSDate not supplied

Development of a Sensorimotor Ground Analog from Astronaut Postflight Experience

Exploration class missions including Artemis, Gateway, and beyond will require a new level of autonomy around periods of gravitational transition, where sensorimotor disturbances are great. Because of this, there is a need to define sensorimotor assessment thresholds that indicate when performance in operational tasks might be impacted or unsafe. To define these thresholds, a Sensorimotor Adaptation Analog (SAA) was proposed that could induce varying levels of sensorimotor disorientation through combined vestibular, visual, and proprioceptive disruptions. The purpose of this study was to gather subjective feedback on the SAA from previously flown astronauts that would mimic their post-flight experience and functional performance immediately after landing (R+0-4hrs; high level) and post-landing (R+24-48hrs; low level). The SAA consisted of galvanic vestibular stimulation (GVS), visual disorientation goggles, and a weighted suit to alter proprioceptive feedback and replicate subjective heaviness. A random sum-of-sines profile between 0-1Hz was used for the GVS with peak amplitudes ranging from 1-4mA. The GVS was applied first at the low (2mA) and high (3mA) levels, followed by the weighted suit alone, then combined with the GVS at the low (20% body weight) and high levels (40% body weight). Last, the disorientation goggles were applied alongside both the GVS and weighted suit at the low (0.07-0.10+ blood alcohol content (BAC)) and high (0.12-0.15+ BAC) levels. Each element of the SAA could be increased or decreased depending on crew feedback to find the disorientation levels that best matched their experience. Five USOS astronauts (1 male, 4 female) who had previously flown (average time since flight: 377 days) participated. Crewmembers reported that GVS alone replicated ~80-90% of their post-flight performance with the weighted suit fine-tuning the experience to replicate an additional 5-10% of their experience. Crewmembers did not believe the disorientation goggles represented either the visual disruptions or illusory sensations that they experienced, nor did they impact performance in post-flight tasks similarly. The final SAA, resulting from crewmember feedback, includes the GVS at the levels described above and the weighted suit at 15% and 30% body weight. The disorientation goggles were removed from SAA. These results provided a more realistic SAA that can be used to define the sensorimotor assessment thresholds through ground subjects and potentially expanded for use in countermeasure testing and as a pre-flight training tool.

S. C. Moudy↗
DOE OSTI2020

Active analog tuning of the phase of light in the visible regime by bismuth-based metamaterials

The active and analog tuning of the phase of light by metamaterials is needed to boost the switching performance of photonic devices. However, demonstrations of this type of tuning in the pivotal visible spectral region are still scarce. Herein, we report the active analog tuning of the phase of visible light reflected by a bismuth (Bi)-based metamaterial, enabled by a reversible solid-liquid transition. This metamaterial, fabricated by following a lithography-free approach, consists of twodimensional assemblies of polydisperse plasmonic Bi nanostructures embedded in a refractory and transparent aluminum oxide matrix. The analog tuning of the phase is achieved by the controlled heating of the metamaterial to melt a fraction of the nanostructures. A maximum tuning of 320° (1.8 π) is observed upon the complete melting of the nanostructures at 230°C. This tuning is reversible by cooling to 25°C. In addition, it presents a wide hysteretic character due to liquid Bi undercooling. This enables the phase achieved by this analog approach to remain stable over a broad temperature range upon cooling and until resolidification occurs around 100°C. Therefore, Bi-based metamaterials are endowed with analog optical memory capabilities, which are appealing for a wide range of applications, including optical data storage with enhanced information density or bistable photonic switching with a tunable “on” state.

36 MATERIALS SCIENCE↗
DOE OSTI2022

High Temperature Steam Electrolysis Process Performance and Cost Estimates

Technology readiness levels (TRLs) of electrolysis systems have dramatically increased in recent years as the interest in clean hydrogen production and decarbonization of transportation, industrial and other sectors increases across the globe. This is especially true of high temperature steam electrolysis (HTSE) / solid oxide electrolysis cell (SOEC) systems which show promise of much higher system efficiencies than other more developed electrolysis technologies. This possibility of higher efficiencies of HTSE / SOEC systems has been previously assumed to be theoretically possible but in recent years it has become less theoretical and more realistic as an increasing amount of suppliers complete lab and pilot tests showing very promising results. Research in the areas of manufacturing techniques, material selection, electrode and electrolyte compositions, and balance of plant size and integration continues at a fast pace as an increasing number of suppliers both internationally and domestically become involved. The advantages of HTSE become more pronounced when HTSE is coupled with nuclear power plants (NPPs). This is because thermal energy produced by the nuclear reactor can be used in a series of heat transfer loops and heat exchangers to vaporize HTSE feedwater, which drastically improves the economics of the process. Idaho National Laboratory (INL) has been very involved in the research and modeling of HTSE systems for a number of years, in collaboration with other national laboratories, academia, and industry stakeholders both on the hydrogen production as well as the hydrogen demand side. The modeling completed over the years on a large variety of projects has led to a wealth of knowledge at INL including in the area of the technoeconomic assessment (TEA) of HTSE systems. TEAs include process modeling of the HTSE systems to calculate system energy requirements and equipment sizing, followed by estimation of capital and operating costs to enable calculation of the levelized cost of hydrogen (LCOH). The TEA work performed has produced incremental improvements and tuning of the methods, assumptions, models, and results of the analyses as well as providing some opportunities for validating these results. The purpose of this document is to record the current baseline HTSE analyses led by INL to show the current status of assumptions and costs of these systems. Given the rapid development of this technology, the variety of suppliers entering the space, and the increasing attention government and industry are giving to such systems, this document may be updated on a periodic basis with updated analysis and assumptions. This document compiles various analyses results and approaches completed over a period of years into a single document to be used as a baseline going forward. It represents what the INL HTSE analysis group assumes to be the internal best estimate of the current operation, costs, and landscape of the HTSE industry state of the art capability for current SOEC technology in an Nth-of-a-Kind (NOAK) plant, which in this study is defined as existence of the manufacturing capacity to support previous deployment of N = 100 count of 25 MWe modular HTSE blocks (with modular equipment component cost reductions specified as following a 95% learning curve). That said, This is a public document and as such so no proprietary data was used or included in this report. There may be HTSE suppliers that have performance specifications, and cost estimates, and test data that differ from the analysis presented in this document. This document is meant to be a best conservative estimate of the technology and not an absolute reference.

08 HYDROGEN↗
DOE OSTI2022

High Temperature Steam Electrolysis Process Performance and Cost Estimates - DOE Hydrogen Program AMR Presentation

Technology readiness levels (TRLs) of electrolysis systems have dramatically increased in recent years as the interest in clean hydrogen production and decarbonization of transportation, industrial and other sectors increases across the globe. This is especially true of high temperature steam electrolysis (HTSE) / solid oxide electrolysis cell (SOEC) systems which show promise of much higher system efficiencies than other more developed electrolysis technologies. This possibility of higher efficiencies of HTSE / SOEC systems has been previously assumed to be theoretically possible but in recent years it has become less theoretical and more realistic as an increasing amount of suppliers complete lab and pilot tests showing very promising results. Research in the areas of manufacturing techniques, material selection, electrode and electrolyte compositions, and balance of plant size and integration continues at a fast pace as an increasing number of suppliers both internationally and domestically become involved. The advantages of HTSE become more pronounced when HTSE is coupled with nuclear power plants (NPPs). This is because thermal energy produced by the nuclear reactor can be used in a series of heat transfer loops and heat exchangers to vaporize HTSE feedwater, which drastically improves the economics of the process. Idaho National Laboratory (INL) has been very involved in the research and modeling of HTSE systems for a number of years, in collaboration with other national laboratories, academia, and industry stakeholders both on the hydrogen production as well as the hydrogen demand side. The modeling completed over the years on a large variety of projects has led to a wealth of knowledge at INL including in the area of the technoeconomic assessment (TEA) of HTSE systems. TEAs include process modeling of the HTSE systems to calculate system energy requirements and equipment sizing, followed by estimation of capital and operating costs to enable calculation of the levelized cost of hydrogen (LCOH). The TEA work performed has produced incremental improvements and tuning of the methods, assumptions, models, and results of the analyses as well as providing some opportunities for validating these results. The purpose of this document is to record the current baseline HTSE analyses led by INL to show the current status of assumptions and costs of these systems. Given the rapid development of this technology, the variety of suppliers entering the space, and the increasing attention government and industry are giving to such systems, this document may be updated on a periodic basis with updated analysis and assumptions. This document compiles various analyses results and approaches completed over a period of years into a single document to be used as a baseline going forward. It represents what the INL HTSE analysis group assumes to be the internal best estimate of the current operation, costs, and landscape of the HTSE industry state of the art capability for current SOEC technology in an Nth-of-a-Kind (NOAK) plant, which in this study is defined as existence of the manufacturing capacity to support previous deployment of N = 100 count of 25 MWe modular HTSE blocks (with modular equipment component cost reductions specified as following a 95% learning curve). That said, this is a public document and as such so no proprietary data was used or included in this report. There may be HTSE suppliers that have performance specifications, and cost estimates, and test data that differ from the analysis presented in this document. This document is meant to be a best conservative estimate of the technology and not an absolute reference.

08 HYDROGEN↗
DOE OSTI2024

Metal–support interactions in metal oxide-supported atomic, cluster, and nanoparticle catalysis

Supported metal catalysts are essential to a plethora of processes in the chemical industry. The overall performance of these catalysts depends strongly on the interaction of adsorbates at the atomic level, which can be manipulated and controlled by the different constituents of the active material (i.e., support and active metal). The description of catalyst activity and the relationship between active constituent and the support, or metal–support interactions (MSI), in heterogeneous (thermo)catalysts is a complex phenomenon with multivariate (dependent and independent) contributions that are difficult to disentangle, both experimentally and theoretically. So-called “strong metal–support interactions” have been reported for several decades and summarized in excellent review articles. However, in recent years, there has been a proliferation of new findings related to atomically dispersed metal sites, metal oxide defects, and, for example, the generation and evolution of MSI under reaction conditions, which has led to the designation of (sub)classifications of MSI deserving to be critically and systematically evaluated. These include dynamic restructuring under alternating redox and reaction conditions, adsorbate-induced MSI, and evidence of strong interactions in oxide-supported metal oxide catalysts. Here, we review recent literature on MSI in oxide-supported metal particles to provide an up-to-date understanding of the underlying physicochemical principles that dominate the observed effects in supported metal atomic, cluster, and nanoparticle catalysts. Critical evaluation of different subclassifications of MSI is provided, along with discussions on the formation mechanisms, theoretical and characterization advances, and tuning strategies to manipulate catalytic reaction performance. We also provide a perspective on the future of the field, and we discuss the analysis of different MSI effects on catalysis quantitatively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRSDate not supplied

Implementation of A New Microwave Scattering Database and A Forward Model for Active Microwave Sensors in CRTM

Radiative transfer models are extensively used for the assimilation of satellite observations into NWP models as well as retrieving geophysical products from satellite measurements. CRTM is a community model developed by NOAA JCSDA and widely used for different purposes requiring RT calculations. CRTM requires bulk scattering lookup tables in order to perform all-sky RT calculations. However, the current CRTM lookup tables for microwave frequencies were generated based on the Mie theory by assuming spherical frozen particles. The scattering lookup tables generated using the DDA technique has shown to largely improve the RT scattering calculations in the MW region. This presentation targets (i) the implementation and validation of a DDA database that was originally developed for the ARTS RT model into CRTM, and (ii) developing the CRTM active sensor module that takes advantage of the backscattering coefficients computed using the DDA method. The DDA database only provides single scattering properties of different habits, while CRTM requires bulk scattering properties. The CRTM cloud coefficients were previously generated based on the effective radius for representing the size of the particles. However, effective radius is neither measurable nor provided by the NWP models, thus need to be estimated from other geophysical variables such as water content. Therefore, in addition to calculating the CRTM bulk scattering properties from the DDA single scattering database, the CRTM was also largely modified to use cloud water content (kg.m-3), instead of effective radius, for performing the interpolation over size/mass of the particles. CRTM already requires water content as input, thus no extra variables are required for performing scattering calculations using the new ARTS DDA database. The CRTM scattering modules search for effective radius in cloud coefficient files and will use the cloud water content if the effective radius dimension is not found in the cloud coefficient files. Figure 1 shows the CRTM simulated brightness temperatures computed using different cloud coefficients versus ATMS observed values over Hurricane Irma on September 7, 2017 at 18:00 UTC. We used all the cloud water content values included in ERA5 with default CRTM/DDA habits for water, rain, snow, ice, hail, and graupel. ERA5 does not provide separate water content values for ice, hail, and graupel, thus the ice water content values were divided between ice, hail, and graupel clouds similar to what was explained in the previous section. In channels with a frequency lower than 90 GHz, emission from water and rain clouds can compensate for cloud scattering so that cloud contaminated Tbs are larger than corresponding clear sky Tbs. The DDA simulations for channels 1-7 largely perform better than the Mie simulations. The DDA simulations show a mix of small negative and positive simulated minus observed values, while the Mie results show large negative biases. The weighting functions for some of the ATMS temperature sounding channels (channels 9-15) peak mostly above the clouds, therefore the measured Tbs become less sensitive to clouds so that the results of both Mie and DDA become very similar. The Mie lookup tables generate excessive scattering for channel 16, but not enough scattering for the water vapor channels. In the specific case of Hurricane Maria, the DDA lookup tables do not generate enough scattering for channel 16, but the DDA results are much more consistent with observations for water vapor channels than for channel 16. It should be noted that the results may vary if we use other habits to represent snow, hail, and graupel in the DDA simulations. Although these results clearly show the advantage of the DDA database over the Mie dataset, different error sources such as error in the observations, displacement of clouds in the ERA5 reanalysis, and also lack of convective clouds or in general errors in the input atmospheric and cloud profiles contribute to the differences between the simulated and observed values. Aside from the improvements in the simulations, a major advantage of the new dataset is a large number of habits that can be used to tune the data assimilation systems to perform well in different weather conditions.

Isaac Moradi↗
DOE OSTI2022

Automatic Generation of High-Performance Convolution Kernels on ARM CPUs for Deep Learning

In this work, we present FastConv, a template-based code auto-generation open source library that can automatically generate high-performance deep learning convolution kernels of arbitrary matrices/tensors shapes. FastConv is based on the Winograd algorithm, which is reportedly the highest performing algorithm for the time-consuming convolution layers of convolutional neural networks. ARM CPUs cover a wide range designs and specifications, from embedded devices to HPC-grade CPUs. The leads to the dilemma of how to consistently optimize Winograd-based convolution solvers for convolution layers of different shapes. FastConv addresses this problem by using templates to auto-generate multiple shapes of tuned kernels variants suitable for skinny tall matrices. As a performance portable library, FastConv transparently searches for the best combination of kernel shapes, cache tiles, scheduling of loop orders, packing strategies, access patterns, and online/offline computations. Auto-tuning is used to search the parameter configuration space for the best performance for a given target architecture and problem size. The experiments with layer-wise evaluation on the VGG--16 model confirms a 1.25x performance gains is got by tuning the Winograd library. Integrated comparison results shows 1.02x to 1.40x, 1.14x to 2.17x, and 1.22x and 2.48x speedup is achieved over NNPACK, Arm NN, and FeatherCNN on the Kunpeng 920 beside few cases. Furthermore, problem size performance portability experiments with various convolution shapes shows that FastConv achieves 1.2x to 1.7x speedup and 2x to 22x speedup over NNPACK and ARM NN inference engine using Winograd on Kunpeng 920 . CPU performance portability evaluation on the VGG--16 show an average speedup over NNPACK of 1.42x, 1.21x, 1.26x, 1.37x, 2.26x, and 11.02x is observed on Kunpeng 920, Snapdragon 835, 855, 888, Apple M1, and AWS Graviton2, respectively.

97 MATHEMATICS AND COMPUTING↗
NASA NTRS1997

NAS Parallel Benchmark. Results 11-96: Performance Comparison of HPF and MPI Based NAS Parallel Benchmarks

High Performance Fortran (HPF), the high-level language for parallel Fortran programming, is based on Fortran 90. HALF was defined by an informal standards committee known as the High Performance Fortran Forum (HPFF) in 1993, and modeled on TMC's CM Fortran language. Several HPF features have since been incorporated into the draft ANSI/ISO Fortran 95, the next formal revision of the Fortran standard. HPF allows users to write a single parallel program that can execute on a serial machine, a shared-memory parallel machine, or a distributed-memory parallel machine. HPF eliminates the complex, error-prone task of explicitly specifying how, where, and when to pass messages between processors on distributed-memory machines, or when to synchronize processors on shared-memory machines. HPF is designed in a way that allows the programmer to code an application at a high level, and then selectively optimize portions of the code by dropping into message-passing or calling tuned library routines as 'extrinsics'. Compilers supporting High Performance Fortran features first appeared in late 1994 and early 1995 from Applied Parallel Research (APR) Digital Equipment Corporation, and The Portland Group (PGI). IBM introduced an HPF compiler for the IBM RS/6000 SP/2 in April of 1996. Over the past two years, these implementations have shown steady improvement in terms of both features and performance. The performance of various hardware/ programming model (HPF and MPI (message passing interface)) combinations will be compared, based on latest NAS (NASA Advanced Supercomputing) Parallel Benchmark (NPB) results, thus providing a cross-machine and cross-model comparison. Specifically, HPF based NPB results will be compared with MPI based NPB results to provide perspective on performance currently obtainable using HPF versus MPI or versus hand-tuned implementations such as those supplied by the hardware vendors. In addition we would also present NPB (Version 1.0) performance results for the following systems: DEC Alpha Server 8400 5/440, Fujitsu VPP Series (VX, VPP300, and VPP700), HP/Convex Exemplar SPP2000, IBM RS/6000 SP P2SC node (120 MHz) NEC SX-4/32, SGI/CRAY T3E, SGI Origin2000.

Saini, Subash↗
DOE OSTI2020

Performance Limits of an Alternating Current Electroluminescent Device

Abstract The use of an alternating current (AC) voltage is a simple, versatile method of producing electroluminescence from generic emissive materials without the need for contact engineering. Recently, it was shown that AC‐driven, capacitive electroluminescent devices with carbon nanotube network contacts can be used to generate and study electroluminescence from a variety of molecular materials emitting in the infrared‐to‐ultraviolet range. Here, performance trade‐offs in these devices are studied through comprehensive device simulations and illustrative experiments, enhancing understanding of the mechanism and capability of electroluminescent devices based on alternating as opposed to direct current (DC) schemes. AC‐driven electroluminescent devices can overcome several limitations of conventional DC‐driven electroluminescent devices, including the requirement for proper alignment of material energy levels and the need to process emitting materials into uniform thin films. By simultaneously optimizing device geometry, driving parameters, and material characteristics, the performance of these devices can be tuned. Importantly, the turn‐on voltage of AC‐driven electroluminescent devices approaches the bandgap of the emitting material as the gate oxide thickness is scaled, and internally efficient electroluminescence can be achieved using low‐mobility single‐layer emitter films with varying thicknesses and energy barrier heights relative to the contact.

Wang, Vivian↗
DOE OSTI2022

Confinement‐Driven Inverse Domain Scaling in Polycrystalline ErMnO 3

Abstract The research on topological phenomena in ferroelectric materials has revolutionized the way people understand polar order. Intriguing examples are polar skyrmions, vortex/anti‐vortex structures, and ferroelectric incommensurabilties, which promote emergent physical properties ranging from electric‐field‐controllable chirality to negative capacitance effects. Here, the impact of topologically protected vortices on the domain formation in improper ferroelectric ErMnO 3 polycrystals is studied, demonstrating inverted domain scaling behavior compared to classical ferroelectrics. It is observed that as the grain size increases, smaller domains are formed. Phase field simulations reveal that elastic strain fields drive the annihilation of vortex/anti‐vortex pairs within the grains and individual vortices at the grain boundaries. The inversion of the domain scaling behavior has far‐reaching implications, providing fundamentally new opportunities for topology‐based domain engineering and the tuning of the electromechanical and dielectric performance of ferroelectrics in general.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Impact of Halogen Groups on the Properties of PEA–Based 2D Pb–Sn Halide Perovskites

Tuning broad emission in 2D Pb–Sn halide perovskites (HPs) is essential for advancing optoelectronic applications, particularly for color-tunable and white-light-emitting devices. This broad emission is linked to structural factors, such as defects and phase segregation of the Pb component within the Pb–Sn system, which are strongly influenced by the molecular structure and chemical properties of spacer cations. Atomic tuning of the spacers via halogenation opens up a new way to fine-tune the molecular properties, enabling further augmentations of HP functionalities. Nevertheless, the distinct broad emission's sensitivity to spacer chemistry remains underexplored. Here, halogenation's influence is systematically investigated on 2D HP emission characteristics using a high-throughput workflow. These findings reveal that the F-containing phenethylammonium (4F-PEA) spacer narrows the broadband PL, whereas Cl broadens it. Through a correlative study, it is found that 4F-PEA reduces not only the local phase segregation but also the defect levels and microstrains in 2D HPs. This is likely attributed to the manifestation of less lattice distortion via stronger surface coordination of the dipole-augmented 4F-PEA. Furthermore, these results highlight halogenation as a key factor in modulating phase segregation and defect density in 2D Pb–Sn HPs, offering a promising pathway to tune the emission for enhanced optoelectronic performance.

2D Pb-Sn halide perovskites↗
DOE OSTI2021

Atomistic Insights of Irreversible Li + Intercalation in MnO 2 Electrode

Tunnel-structured MnO 2 represents open-framed electrode materials for reversible energy storage. Its wide application is limited by its poor cycling stability, whose structural origin is unclear. We tracked the structure evolution of β-MnO 2 upon Li + ion insertion/extraction by combining advanced in situ diagnostic tools at both electrode level (synchrotron X-ray scattering) and single-particle level (transmission electron microscopy). The instability is found to originate from a partially reversible phase transition between β-MnO 2 and orthorhombic LiMnO 2 upon lithiation, causing cycling capacity decay. Moreover, the MnO 2 /LiMnO 2 interface exhibits multiple arrow-headed disordered regions, which severely chop into the host and undermine its structural integrity. Our findings could account for the cycling instability of tunnel-structured materials, based on which future strategies should focus on tuning the charge transport kinetics toward performance enhancement.

25 ENERGY STORAGE↗
DOE OSTI2024

Rational optimization of substituted α–MnO 2 cathode for aqueous zinc–ion battery

Density functional theory (DFT) is utilized to explore the effects of increasing concentrations of vanadium (V) and chromium (Cr) substitution on the discharge of α-MnO 2 cathode in hydrated zinc-ion batteries (ZIBs). During H + -intercalation and Zn 2+ -intercalation, Cr-substitution proves to be more effective than V-substitution in promoting discharge behaviors. Transitioning from Mn 0.875 Cr 0.125 O 2 , Mn 0.75 Cr 0.25 O 2 to Mn 0.625 Cr 0.375 O 2 is found to consistently enhance the discharge voltage, along with improved tunnel structure retention and volume expansion suppression. In comparison, the promoting effect of increasing V-substitution is relatively small at initial discharge stages and leads to degradation at later stages, primarily due to an increased concentration of unstable Mn 2+ ion. The superior effect of Cr-substitution is attributed to the unique atomic and electronic structures of substituted Cr 4+ and reduced Cr 3+ ions during discharge. These ions serve as active electron acceptors to limit the formation of Mn 3+ and Mn 2+ ions, and as anchors to stabilize the α-MnO 2 framework and intercalated H + /Zn 2+ ions, respectively. Finally, our study highlights fine-tuning through substitution to enhance the performance of α-MnO 2 -based cathode materials in ZIBs.

25 ENERGY STORAGE↗
DOE OSTI2025

Lewis Acid Site Engineering in Chromite Spinels Orchestrated Surface Reconstruction and Surpasses RuO 2 in Oxygen Evolution

Atomic-scale engineering of chromite spinels featuring redox-active tetrahedral A-sites and strong Cr–O covalency offers a promising route to superior platinum-group-metal-free oxygen evolution reaction (OER) catalysts. However, comprehensive studies addressing how cation substitution influences surface chemistry and governs OER activity and durability in chromite spinels remain limited. Here, in this work, a systematic investigation of the multicationic chromite series Ni x Fe y Cr 3−x−y O 4 is presented, identifying composition-dependent Lewis acidity as a descriptor of superior OER performance. It is further demonstrated that tuning surface acidity directly controls dynamic reconstruction processes and lattice-oxygen participation during spinel-based electrocatalysis. Following activation, the optimized Ni 0.8 Fe 0.3 Cr 1.9 O 4 catalyst delivers a current density of 10 mA cm −2 at an overpotential of 235 mV, surpassing RuO 2 , with excellent long-term stability. Integrating microscopic and spectroscopic analysis with operando impedance spectroscopy, it shows that activation generates an oxyhydroxide overlayer and reveals a previously unrecognized link between surface Lewis acidity and the growth kinetics and activity of these shells. Density functional theory calculations indicate that Fe incorporation at octahedral sites raises the O 2p-band center and lowers oxygen-vacancy formation energy, promoting lattice-oxygen activation and triggering reconstruction, yielding enhanced OER. This work integrates cation-driven surface-acidity modulation, acidity-governed reconstruction, and OER activity enhancement into a unified predictive framework for designing earth-abundant spinel-based catalysts.

operando impedance spectroscopy↗
DOE OSTI2022

The impact of neutrino-nucleus interaction modeling on new physics searches

Accurate neutrino-nucleus interaction modeling is an essential requirement for the success of the accelerator-based neutrino program. As no satisfactory description of cross sections exists, experiments tune neutrino-nucleus interactions to data to mitigate mis-modeling. In this work, we study how the interplay between near detector tuning and cross section mis-modeling affects new physics searches. We perform a realistic simulation of neutrino events and closely follow NOvA’s tuning, the first published of such procedures in a neutrino experiment. We analyze two illustrative new physics scenarios, sterile neutrinos and light neutrinophilic scalars, presenting the relevant experimental signatures and the sensitivity regions with and without tuning. While the tuning does not wash out sterile neutrino oscillation patterns, cross section mis-modeling can bias the experimental sensitivity. In the case of light neutrinophilic scalars, variations in cross section models completely dominate the sensitivity regardless of any tuning. Our findings reveal the critical need to improve our theoretical understanding of neutrino-nucleus interactions, and to estimate the impact of tuning on new physics searches. We urge neutrino experiments to follow NOvA’s example and publish the details of their tuning procedure, and to develop strategies to more robustly account for cross section uncertainties, which will expand the scope of their physics program.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Examining Metal Identity and Proximity Effects on Acetylene Hydrogenation with Azolate-Based MOFs

Liquid organic hydrogen carriers (LOHCs) are an attractive fuel source due to their compatibility with existing transportation methods and ease of use. However, they suffer from sluggish (de)hydrogenation kinetics. One promising platform for developing next-generation catalysts is metal–organic frameworks (MOFs), which can enable systematic interrogation into the influence of metal identity and spatial arrangement. In this study, the effect of the coordination environment was investigated using Ni- and Co-based azolate MOFs: MFU-4l-OH (M x Zn 5–x (OH) 4 (BTDD) 3 ; x = 4 for M = Co and x = 3 for M = Ni, H 2 BTDD = bis(1H-1,2,3-triazolo[4,5-b][4′,5′-i])dibenzo[1,4]dioxin), composed of single-site nodes, and M(OH) 2 BBTA (M = Ni, Co; H 2 BBTA = 1H,5H-benzo(1,2-d:4,5-d’)bistriazole), composed of extended chain-type nodes. The catalysts were characterized by isotherms, powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), inductively coupled plasma-optical emission spectroscopy (ICP-OES), and X-ray photoelectron spectroscopy (XPS) analysis. Acetylene hydrogenation activity under steady state conditions (150 °C, 1:1 C 2 H 2 :H 2 ) revealed higher turnover frequencies (TOFs) up 1.17 × 10 –2 mol C 2 H 2 mol −1 Ni min −1 and 1.98 × 10 –3 mol C 2 H 2 mol −1 Co min −1 for Ni-MFU-4l-OH and Co-MFU-4l-OH, respectively, compared to their BBTA analogues. However, the Co-based MOFs, particularly Co 2 (OH) 2 -BBTA, exhibited greater selectivity (up to 19%) for the fully hydrogenated ethane product. Isosteric heat of adsorption (Q st ) measurements for ethylene and ethane revealed that the BBTA framework had stronger binding to the products than MFU-4l. Furthermore, these findings demonstrate that metal identity and coordination environment may modulate acetylene hydrogenation performance, leading to design principles for tuning LOHC hydrogenation catalysts.

catalysts↗
DOE OSTI2021

Compositional heterogeneity in Cs y FA 1- y Pb(Br x I 1- x ) 3 perovskite films and its impact on phase behavior

Hybrid organic inorganic lead halide perovskite semiconductors of the form Cs y FA 1-y Pb(Br x I 1-x ) 3 are promising candidate materials for high-efficiency photovoltaics. Notably, cation and anion substitution can be used to tune the band gaps to optimize performance and improve stability. However, multi-component materials can be prone to compositional and structural inhomogeneity and the extent, length scale and impact of this heterogeneity on lead halide perovskite properties are not well understood. Here we use synchrotron X-ray diffraction to probe the evolution of crystal structure across the tetragonal-to-cubic phase transition for a series of Cs y FA 1-y Pb(Br x I 1-x ) 3 thin films with x = 0.05 to 0.3 and y = 0.17 to 0.40. We find that the transition occurs across a broad temperature range of approximately 40 °C, much larger than for pure compounds such as MAPbI 3 and MAPbBr 3 . Finally, we hypothesize that this smearing of the phase transition is due to compositional inhomogeneities that give rise to a distribution of local transition temperatures and we estimate the composition varies by about 10% to 15% with likely greater heterogeneity for the halide anion than the cation. This approach of mapping the transition is a simple and effective method of assessing heterogeneity, enabling evaluation of its impact.

36 MATERIALS SCIENCE↗