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DOE OSTI2019

Deeply Integrated Vehicle Dynamic and Powertrain Operation for Efficient Plug-in Hybrid Electric Bus

The emerging connected and automated vehicle (CAV) technology has opened the door for developing innovative applications and systems to improve vehicle energy efficiency. While most of the recent research has been focused on optimizing vehicle dynamic (VD) and powertrain (PT) operation in isolation, there exists untapped potential to further improve vehicle fuel efficiency through a co-optimization of VD&PT control. In this paper, the authors develop an eco-operation solution for a plug-in hybrid electric bus (PHEB) which seamlessly integrates state-of-the-art CAV applications with advanced powertrain optimization strategies, aiming at improving vehicle energy efficiency and reducing tailpipe emissions. The proposed eco-operation system have 6 components, including traffic/signal timing information acquirement, information integration, scenario identification, powertrain, trajectory planning and a MATLAB/Simulink model for validation and fine-tuning. A deeply integrated vehicle dynamic and powertrain control algorithm is proposed in the paper to optimize the energy-efficiency. Based on the key logic of powertrain control strategy of PHEB, the authors develop a simplified PHEB powertrain model, and put it into their graph based optimization model as the edge cost to derive the optimal speed profile, which is further fine-tuned in the Simulink model. The proposed mode is validated in multiple numerical tests under Eco-Approach and Departure, Eco-Stop and Launch and Eco-Cruise scenarios, and shows significant performance (above 20%) in energy-saving.

Hao, Peng↗

NASA NTRSDate not supplied

The Flight Dynamics Risk Assessment of Artemis I

With launch vehicles and spacecraft, it is necessary to dynamically test the structure to validate structural models. These validated models are then used to determine a launch vehicle's control stability margin and the loads on the structure. While often a dedicated structural test article is used to correlate the integrated structure in preparation for the final analysis cycles, the Artemis I flight is using an approach where the components of the launch vehicle are dynamically tested and the component models validated. The fully integrated vehicle is not tested until a few months before launch, which limits the ability to fully correlate a model prior to launch. This paper introduces the Flight Dynamics Risk Assessment of the vehicle, which is the process being used to determine the adequacy of the vehicle structural model after the Integrated Modal Test. This work outlines the process of quickly tuning a model post-test then determining any control margin violations and increases in loads due to that tuned model.

Eric C Stewart↗

NASA NTRSDate not supplied

The Flight Dynamics Risk Assessment of Artemis I

Eric C Stewart↗

DOE OSTI2022

Tuning transport in graphene oxide membrane with single-site copper ($\mathrm{II}$) cations

Controlling the ion transport through graphene oxide (GO) membrane is challenging, particularly in the aqueous environment due to its strong swelling tendency. Fine-tuning the interlayer spacing and chemistry is critical to create highly selective membranes. We investigate the effect of single-site divalent cations in tuning GO membrane properties. Competitive ionic permeation test indicates that Cu 2+ cations dominate the transport through the 2D channels of GO membrane over other cations (Mg 2+ /Ca 2+ /Co 2+ ). Without/With the single-site M 2+ modifications, pristine GO, Mg-GO, Ca-GO, and Cu-GO membranes show interlayer spacings of ~13.6, 15.6, 14.5, and 12.3 Å in wet state, respectively. The Cu-GO membrane shows a two-fold decrease of NaCl (1 M) permeation rate comparing to pristine GO, Mg-GO, and Ca-GO membranes. In reverse osmosis tests using 1000 ppm NaCl and Na 2 SO 4 as feeds, Cu-GO membrane shows rejection of ~78% and ~94%, respectively, which are 5%–10% higher than its counterpart membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Understanding anisotropic growth of Au penta-twinned nanorods by liquid cell transmission electron microscopy

Morphology control of anisotropic metal nanocrystals plays an important role in tuning shape-dependent physicochemical properties for various applications, but underlying understanding of their anisotropic growth mechanism remains a great challenge. Here, we investigate the formation of Au penta-twinned nanorod by in situ liquid cell transmission electron microscopy (LC-TEM). It is found that a truncated-decahedron forms in the absence of cetyl-trimethyl ammonium bromide (CTAB), whereas in the presence of CTAB a reentrant groove appears in decahedron to relieve strain during the nanorod formation, which induces the formation of {100} facets. The growth dynamics of penta-twinned nanorod implies that CTAB molecules can promote the nanorod growth by selectively inhibiting atom addition to {100} facets. Density functional theory (DFT) simulations confirm that the partial relieve of strain energy of decahedron nanoparticle is caused by the adsorption of Br- ions. Moreover, the selective adsorption of CTAB lowers the surface energy of {100} facets, resulting in the nanorod growth along the [110] direction. Based on the appearance of reentrant groove and growth dynamics unraveled by LC-TEM, the synergy of strain and surface energy tuning by additives is discovered. The study provides an in-depth insight into the anisotropic growth of nanorods and lays foundations for controlled synthesis of nano-materials.

Jin, Biao↗

NASA NTRS2002

Adaptive Identification and Control of Flow-Induced Cavity Oscillations

Progress towards an adaptive self-tuning regulator (STR) for the cavity tone problem is discussed in this paper. Adaptive system identification algorithms were applied to an experimental cavity-flow tested as a prerequisite to control. In addition, a simple digital controller and a piezoelectric bimorph actuator were used to demonstrate multiple tone suppression. The control tests at Mach numbers of 0.275, 0.40, and 0.60 indicated approx. = 7dB tone reductions at multiple frequencies. Several different adaptive system identification algorithms were applied at a single freestream Mach number of 0.275. Adaptive finite-impulse response (FIR) filters of orders up to N = 100 were found to be unsuitable for modeling the cavity flow dynamics. Adaptive infinite-impulse response (IIR) filters of comparable order better captured the system dynamics. Two recursive algorithms, the least-mean square (LMS) and the recursive-least square (RLS), were utilized to update the adaptive filter coefficients. Given the sample-time requirements imposed by the cavity flow dynamics, the computational simplicity of the least mean squares (LMS) algorithm is advantageous for real-time control.

Kegerise, M. A.↗

DOE OSTI2019

Strong Damping‐Like Spin‐Orbit Torque and Tunable Dzyaloshinskii–Moriya Interaction Generated by Low‐Resistivity Pd 1− x Pt x Alloys

Abstract Despite their great promise for providing a pathway for very efficient and fast manipulation of magnetization, spin‐orbit torque (SOT) operations are currently energy inefficient due to a low damping‐like SOT efficiency per unit current bias, and/or the very high resistivity of the spin Hall materials. This work reports an advantageous spin Hall material, Pd 1− x Pt x , which combines a low resistivity with a giant spin Hall effect as evidenced with three independent SOT ferromagnetic detectors. The optimal Pd 0.25 Pt 0.75 alloy has a giant internal spin Hall ratio of >0.60 (damping‐like SOT efficiency of ≈0.26 for all three ferromagnets) and a low resistivity of ≈57.5 µΩ cm at a 4 nm thickness. Moreover, it is found that the Dzyaloshinskii–Moriya interaction (DMI), the key ingredient for the manipulation of chiral spin arrangements (e.g., magnetic skyrmions and chiral domain walls), is considerably strong at the Pd 1− x Pt x /Fe 0.6 Co 0.2 B 0.2 interface when compared to that at Ta/Fe 0.6 Co 0.2 B 0.2 or W/Fe 0.6 Co 0.2 B 0.2 interfaces and can be tuned by a factor of 5 through control of the interfacial spin‐orbital coupling via the heavy metal composition. This work establishes a very effective spin current generator that combines a notably high energy efficiency with a very strong and tunable DMI for advanced chiral spintronics and spin torque applications.

Zhu, Lijun↗

DOE OSTI2026

Highly Anisotropic Quasi‐Direct Organic Metal Halide Hybrids: A Platform for Polarization‐Sensitive Optoelectronics

Low-dimensional organic–inorganic metal halide hybrids (OMHHs) exhibit remarkable optical properties and enhanced environmental stability. We investigate a 1D OMHH with formula C 4 N 2 H 14 PbBr 4 , consisting of Pb–Br chains separated by organic cations, which shows a large Stokes shift (0.83 eV) and broadband emission. Through first-principles calculations and polarized Raman spectroscopy, we characterize the material's vibrational properties and identify the specific phonon modes that drive exciton self-trapping. Our novel GW/Bethe-Salpeter equation force formalism reveals that low-frequency phonons (∼ 100 cm −1 , primarily involving Pb–Br motions) couple strongly with excitons, with a remarkably high Huang-Rhys factor of 137 ± 4, and gives a pathway for ultrafast structural analysis during the absorption process. This phonon-exciton coupling mechanism explains the material's broadband emission and provides a pathway for controlling optical properties through vibrations and for tuning vibrations through optical excitations. The material also exhibits highly anisotropic optical properties and electronic transport, with bands that are dispersive along the Pb–Br chains but nearly flat in perpendicular directions, resulting in direction-dependent electrical conductivity that is calculated to be an order of magnitude higher along the chain direction and consistent with measurements. These combined properties make this system an excellent platform for polarization-sensitive optoelectronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2025

PFSA-Ionomer Dispersions to Thin-Films: Interplay Between Sidechain Chemistry and Dispersion Solvent

In fuel-cell catalyst layers (CLs), ionomers exists as nanoscale thin-films binding catalyst particles, wherein ionic and gaseous species transport to catalyst sites. To improve film function, ionomers have been designed based on the prototypical perfluorosulfonic acid (PFSA). Since CLs are fabricated through solution-based processing of inks, understanding how ink/dispersion solvent impacts ionomer interactions and function is important to guide future ionomer design. Herein, PFSA and its chemical derivatives are characterized from dispersion (in solvent) to thin film (cast on support) to investigate the impact of solvent water content on ionomer dispersion (structure, acidity) and resulting film properties. Dispersion characterization reveals that secondary aggregate structure depends on the sidechain chemistry, but all PFSA-based ionomers evolve similarly as dispersion becomes water-rich. The differences in aggregation alter ionomer adsorption and thin film morphology. Further, hydrophilic domain spacing and orientation are affected primarily by sidechain chemistry, and modulated by solvent composition. Thin-film conductivity correlates with hydration and nanodomain alignment, signifying the role of morphology in properties. Overall, this work provides insights into how chemistry can be used to coarse-tune structure–property relationships, while processing solvent is for fine-tuning of dispersion-film interplay for controlling CL-ionomer function, which can be translated to other chemistries and ink formulations.

25 ENERGY STORAGE↗

DOE OSTI2024

Predicting the tensile and compressive modulus of electrospun fiber mat‐reinforced hydrogels using the Halpin–Tsai equations

Abstract The reinforcement of mechanically‐weak hydrogels to yield composites with increased stiffness, strength, or toughness is a well‐established approach. In particular, introducing electrospun nanofibers into hydrogels is a common strategy for biomedical applications, as the resulting hierarchical structure mimics biology and allows for control over fiber diameter and alignment and tuning of mechanical properties. However, further study of the link between the constituent materials and the mechanical properties of the composite is uncommon. One potential model to understand the mechanical properties of fiber‐reinforced hydrogels involves the Halpin–Tsai equations, which relate the modulus values of the fibers and hydrogel matrix and the fiber volume fraction, to the modulus of the composite. To assess the application of this model to fiber‐reinforced hydrogels, predicted values were compared with experimental values from mechanical testing of a poly(ethylene glycol) (PEG) matrix reinforced with an electrospun polycaprolactone (PCL) fiber mat. Although the equations described these systems well in tension, providing a facile approach to identify a fiber volume fraction that will achieve a desired modulus, the Halpin–Tsai approach was less successful under compression. This study motivates additional investigation of the role of structural features of hydrogel composites in determining mechanical properties to enable design of materials for specific applications.

Polymer Science↗

DOE OSTI2020

Toward controlled functional sequencing and hierarchical structuring in imidazolium ionenes

This focused mini-review highlights recent advances related to the design and applications of imidazolium ionenes and forward-looking perspectives. Creative strategies which employ established synthetic approaches and utilize the modularity of the imidazole moiety unlock great potential for tailoring both functional and structural features arising from precise spacing of ionic groups within the polymer backbone. Here, as imidazolium ionenes draw more interest, increased sophistication of chemical modifications and material processing is occurring, with a corresponding shift toward more demanding applications. Synthetic routes for placement and sequencing of ionic content are discussed, in addition to recent approaches to control structure and self-assembly or tune behaviors of imidazolium ionenes and composites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Microwave-assisted conversion of methane over H-(Fe)-ZSM-5: Evidence for formation of hot metal sites

We report microwave-assisted catalysis offers great promise as an “intensified” technology for chemical processing. The present study investigates microwave-assisted direct conversion of methane with focus on the design and evaluation of microwave-sensitive H-(Fe)ZSM-5 catalysts for the existence of hotspot formation. Isomorphous substituted H-(Fe)ZSM-5 catalysts are tuned to identify key design parameters that control their microwave sensitivity. Increasing the amount of Al and Fe substitution in the zeolite lattice is found to result in higher microwave sensitivity due to improved dielectric properties and hence facilitated microwave heating of the catalyst bed. Comparison between the performance of these catalysts in a conventional thermally-heated (CH) fixed-bed and a microwave (MW) reactor allows identification of the effect of microwave irradiation on the catalyst activity. Methane conversion is drastically enhanced at MW conditions (from 3% at CH conditions to 40% at MW conditions), indicating accelerated methane activation over the metal site and hence suggesting a hot metal site despite much lower catalyst bulk temperature measured in the microwave reactor. The existence of metal hotspot formation is further supported by the reaction product distribution and spent catalyst analysis. At MW conditions, C 2 (ethane and ethylene) and coke (mainly carbon nanotubes and nanofibers) selectivity are much higher at the cost of aromatics make compared to CH conditions. This can be explained by reduced aromatization activity at the Brønsted acid sites of the zeolite due to its lower relative temperature of the zeolite. The much-enhanced metal aggregation observed in the spent catalyst from the MW reactor along with the distribution of coke species further confirms the existence of selective heating (i.e. hotspot formation) occurring at the active metal site in the catalyst at MW conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

From suppressed void growth to significant void swelling in NiCoFeCr complex concentrated solid-solution alloy

Void swelling can result in dimensional instability and undermine the safe operation of nuclear reactors. Current strategies to inhibit void swelling mainly focus on enhancing defect absorption and recombination by introducing high-density defect sinks. Complex concentrated solid-solution alloys (CSAs), including high-entropy alloys, can withstand severe radiation damage due to their inherent chemical complexity without interfaces. However, the underlying mechanisms for void suppression in CSAs are far from clear. In this research, we studied the void evolution with respect to irradiation depths, doses, and temperatures in equiatomic NiCoFeCr under 3 MeV Ni ion irradiations. At relatively low doses (16 and 54 displacements per atom, dpa), voids form mainly outside of the ion-damaged region, and void formation in the peak damage region is suppressed, leading to negligible swelling. However, with further increase of dose (86 up to 250 dpa), significant void growth occurs in the peak damage region and extended dislocation lines dominate instead of short dislocation lines and loops formed at lower doses. From 500 to 700 °C, the dislocation density decreases while dislocations grow. Although the overall void swelling increases dramatically from 500 to 580 °C at 54 dpa, void growth in the peak damage region is still suppressed. The transition from suppressed void growth to significant void swelling is attributed to dislocation evolution and local chemical inhomogeneity (enrichment of Fe/Cr in the matrix) at higher doses. Our study shows that controlling element diffusion and defect evolution through tuning chemical complexity can further enhance the swelling resistance of CSAs.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Tuning domain size and crystallinity in isoindigo/PCBM organic solar cells via solution shearing

Despite having achieved the long sought-after performance of 10% power conversion efficiency, high performance organic photovoltaics (OPVs) are still mostly constrained to lab scale devices fabricated by spin coating. Efforts to produce printed OPVs lag considerably behind, and the sensitivity to different fabrication methods highlights the need to develop a comprehensive understanding of the processing-morphology relationship in printing methods. Here we present a systematic experimental investigation of a model low bandgap polymer/fullerene system, poly-isoindigo thienothiophene/PC 61 BM, using a lab-scale analogue to roll-to-roll coating as the fabrication tool in order to understand the impact of processing parameters on morphological evolution. We report that domain size and polymer crystallinity can be tuned by a factor of two by controlling the temperature and coating speed. Lower fabrication temperature simultaneously decreased the phase separation domain size and increased the relative degree of crystallinity in those domains, leading to improved photocurrent. We conclude that domain size in isoindigo/PCBM is dictated by spontaneous phase separation rather than crystal nucleation and growth. Moreover we present a model to describe the temperature dependence of domain size formation in our system, which demonstrates that morphology is not necessarily strictly dependent on the evaporation rate, but rather on the interplay between evaporation and diffusion during the printing process.

14 SOLAR ENERGY↗

DOE OSTI2023

Chitosan as a Canvas for Studies of Macromolecular Controls on CaCO 3 Biological Crystallization

A mechanistic understanding of how macromolecules, typically as an organic matrix, nucleate and grow crystals to produce functional biomineral structures remains elusive. Advances in structural biology indicate that polysaccharides (e.g., chitin) and negatively charged proteoglycans (due to carboxyl, sulfate, and phosphate groups) are ubiquitous in biocrystallization settings and play greater roles than currently recognized. This review highlights studies of CaCO 3 crystallization onto chitinous materials and demonstrates that a broader understanding of macromolecular controls on mineralization has not emerged. With recent advances in biopolymer chemistry, it is now possible to prepare chitosan-based hydrogels with tailored functional group compositions. By deploying these characterized compounds in hypothesis-based studies of nucleation rate, quantitative relationships between energy barrier to crystallization, macromolecule composition, and solvent structuring can be determined. Finally, this foundational knowledge will help researchers understand composition-structure-function controls on mineralization in living systems and tune the designs of new materials for advanced applications.

15 GEOTHERMAL ENERGY↗

DOE OSTI2022

Titrating Controlled Defects into Si-LTA Zeolite Crystals Using Multiple Organic Structure-Directing Agents

Controlling defects in zeolites is crucial for tuning their adsorption and catalytic properties. In this work, we have performed an integrated zeolite synthesis, spectroscopy, and density functional theory study to test the limit of F– as a charge-balancing agent that mitigates defects in siliceous zeolites. We focused on the synthesis of siliceous zeolite LTA at 150 °C with 1,2-dimethyl-3-(4-methylbenzyl) imidazolium as the primary organic structure-directing agent (OSDA) and tetramethyl ammonium (TMA) as the secondary OSDA. By varying the amount of TMA in the synthesis gel, positive charges were titrated into the resulting as-made Si-LTA. Surprisingly, we found that greater TMA concentration does not induce more F– to enter into the zeolite. 29Si solid-state MAS NMR, Raman spectroscopy, and density functional theory suggest that this system has surpassed its capacity for F– to balance OSDA charge, and additional positive charge is balanced by Si–O– framework defects. The number of defects in the as-made Si-LTA can be precisely titrated by the amount of TMA in the zeolite structures. For the Si-LTA synthesized without TMA, framework defects formed in the early stage of crystal growth were found to heal during later crystallization, leading to defect-free Si-LTA. However, for the Si-LTA synthesized with TMA, the defects formed in early stages do not heal. A DFT thermodynamic analysis explains that crowding of Si-LTA pores by TMA impedes defect healing; this prediction is corroborated by synthesis experiments at an elevated temperature (170 °C). These results indicate that F– can have a limited capacity to balance OSDA charge in zeolite synthesis, opening up a third route to zeolite synthesis intermediate between the fluoride and hydroxide routes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Optical Effects of Divalent Functionalization of Carbon Nanotubes

Covalent functionalization of single-walled carbon nanotubes (SWCNTs) enables tuning of their optical properties through the generation of sp3-hybridized defects with distinct localized morphology. Groups with strong electron-withdrawing abilities result in redshifted emission experimentally. Further redshifts can be generated by groups bound to more than one carbon atom in the SWCNT (“divalent functionalization”). Depending on the type of divalent functionalization, the spectral diversity is reduced compared to their monovalent counterparts. Here we study the effect of divalent functionalization on the exciton localization at the defect site and related redshifts in emission of (6,5) SWCNT through low-temperature spectroscopy measurements and time dependent density functional theory calculations. These effects are characterized for three classes of divalent compounds distinct in the number of atoms in the functional group and bonding pattern to the tube. The bond character of the two carbon atoms proximal to the defect site is found to have a notable impact on the system stability and spectral redshifts. Functionalized systems are stabilized when the hybridization at the SWCNT remains sp2-like due to its ability to form planar bonds to the remaining hexagonal network, while bond character in the functionalized regions affects the redshifts. This is only possible for certain bonding geometries in divalent species, justifying their decreased spectral diversity. We further show that functionalization at spatially separated sites on the tube can be accompanied by a second chemical adduct, and the configuration of the resulting defect is dictated by bond reactivity following the first addition. This behavior justifies the spectral trends of a class of divalent systems with linker chains or high defect concentration. These results further corroborate that adducts predominantly form chemical bonds only to the neighboring carbons on the SWCNT surface (ortho species) in experimental samples. Our analysis of bond character in the vicinity of the defect sites rationalizes appearance of many spectral features arising from monovalent and divalent defect states of functionalized SWCNTs. As a result, this emerging understanding enables tuning of the emission characteristics through careful control of the defect structure.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Investigating the Elusive Nature of Atomic O from CO 2 Dissociation on Pd(111): The Role of Surface Hydrogen

CO 2 dissociation is a key step in CO 2 conversion reactions to produce value-added chemicals typically through hydrogenation. In many cases, the atomic O produced from CO 2 dissociation can potentially block adsorption sites or change the oxidation state of the catalyst. Here, we used ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and density functional theory (DFT) calculations to investigate the presence of surface species from the dissociation of CO 2 on Pd(111). AP-XPS results show that CO 2 was dissociated to produce adsorbed CO, but dissociated atomic O was not observed at room temperature. We were only able to observe atomic O when CO 2 was introduced at 500 K. Further investigations of O-covered Pd(111) revealed that chemisorbed O could be easily removed by low pressures of CO and H 2 . Notably, the effect of H 2 is quite prominent since it could react with chemisorbed O at a pressure as low as 2 × 10 -9 Torr, and the presence of H2 at ambient pressure prevented CO 2 dissociation. DFT calculations showed that in the presence of background H 2 , facile CO 2 dissociation took place via the reverse water–gas shift (rWGS) reaction, which resulted in the formation of adsorbed CO and removal of O by H 2 . DFT also identified the possible variation of surface species on simultaneous exposure of CO 2 and H 2 over Pd(111) depending on temperature and pressure, which opens alternative opportunities to tune the CO 2 hydrogenation catalysis by controlling the reaction conditions.

36 MATERIALS SCIENCE↗