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DOE OSTI2026

Origins of Enhanced Ion Transport in Nanostructured Anion-Conducting Polyelectrolytes

Ion-conducting polymer chemistry and microstructure profoundly impact membrane water uptake and ionic conductivity. Water uptake strongly impacts ionic conductivity; yet excess water uptake compromises ion-exchange membrane mechanical properties. Although nanophase separation has been proposed to overcome this trade-off, it is unclear how polymer backbone architecture governs ionic nanostructure and its subsequent impact on water uptake and conductivity. Here, we integrate experiments and molecular dynamics simulations to elucidate the role of backbone chemistry in governing ionic nanostructure, hydration behavior, and ion transport in anion-conducting polyelectrolytes (ACPs). We systematically investigate hydrocarbon polynorbornene (PNB)-based ACPs with three distinct backbone architectures: vinyl-addition polymerization (VAP), ring-opening metathesis polymerization (ROMP), and hydrogenated ROMP. While maintaining comparable ion exchange capacities (IECs) and identical side-chain chemistry, we isolate the effects of backbone structure. We show that nanophase-separated ionic nanostructures originate in the dry state and evolve upon hydration through heterogeneous water uptake, with water preferentially partitioning into ion-rich domains. This nanophase separation arises from a delicate interplay between ionic segregation propensity and the entropic barrier imposed by backbone stiffness. Specifically, flexible backbones intensify attractive ion–ion interactions by reducing the entropic penalty for backbone deformation, promoting nanophase separation, while rigid backbones suppress ionic nanostructure formation. Nanophase-separated ion domains locally concentrate water upon hydration, which in turn enables the connectivity required for fast transport at lower water concentration values. Furthermore, these findings demonstrate that backbone chemistry can be tuned as a design lever to promote nanophase separation and enhance ion transport without excessive water uptake.

Anions↗

DOE OSTI2023

Imaging Nanoscale Energy Transport and Conversion with Ultrafast Electron Microscopy (Final Technical Report)

Light-matter interactions are ubiquitous in nature and reside at the heart of innumerable technologies. The cascade of processes that occur when a material absorbs a photon of light are exceedingly complex and are interwoven in both space and time, rendering precise determination of the atomic-scale and ultrafast mechanisms immensely challenging. The advent of methods for generating short pulses of light several decades ago led to major advances in understanding the initial moments of light absorption and the resultant effects, though directly interrogating the response of the atoms within the material continued to prove challenging. More recently, methods for generating ultrashort pulses of X-rays and fast electrons have opened the way to probing photoinduced structural dynamics of a wide range of matter in multiple phases. An especially promising laboratory-scale method is ultrafast electron microscopy (UEM), wherein the modalities of conventional transmission electron microscopes (imaging, diffraction, spectroscopy) are extended into the femtosecond temporal regime. Here, the ultrafast imaging and diffraction modalities of UEM were used to study the transient structural aspects of photoexcitation of semiconducting materials (e.g., spatially-resolved electron-phonon coupling, excitation and emission of acoustic phonons, and discrete nanoscale scattering processes). The project had three main objectives: (1) determination of the excitation mechanisms of dense, hypersonic charge-carrier waves and the spatially mediated means by which they couple to the lattice via coherent phonon emission, especially with UEM imaging, wherein effects of nanoscale structural and morphological features on the coupling and relaxation dynamics are expected to dictate nucleation sites and preferred wave vectors, (2) elucidation of photoinduced acoustic-phonon seeding, emergence, propagation, and decay over nanoscale crystal regions and especially with respect to local strain fields and atomic-scale disruptions in lattice order, and (3) interwoven with the first two were efforts aimed at realizing combined angstrom-femtosecond spatiotemporal imaging with UEM. The outcomes and impacts of this project were the generation of new knowledge with respect to fundamental light-matter interactions and, especially, the spatially-mediated excitation and evolution of the structural response of materials following coherent photoexcitation. Importantly, the spatial and temporal resolutions of the UEM imaging modalities used are well-suited for such studies and enable spatially-resolved mechanisms to be determined as a function of atomic order, structural features, and morphology. In addition, ultrafast crystallographic measurements were used to correlate real- and reciprocal-space dynamics in order to determine atomic-scale preferential wave vectors and ultrafast scattering mechanisms, especially as dictated by specimen boundary conditions. The obtained results, as detailed in peer-reviewed publications and presentations, illustrate the importance of ultrafast, angstrom-scale real-space imaging for developing a comprehensive understanding of energy transport and conversion in materials.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Nontraditional Approaches To Enable High-Energy and Long-Life Lithium–Sulfur Batteries

In this study, lithium-sulfur (Li-S) batteries are promising for automotive applications due to their high theoretical energy density (2600 Wh/kg). In addition, the natural abundance of sulfur could mitigate the global raw material supply chain challenge of commercial lithium-ion batteries that use critical elements, such as nickel and cobalt. However, due to persistent polysulfide shuttling and uncontrolled lithium dendrite growth, Li-S batteries using nonencapsulated sulfur cathodes and conventional ether-based electrolytes suffer from rapid cell degradation upon cycling. Despite significant improvements in recent decades, there is still a big gap between lab research and commercialization of the technology. To date, the reported cell energy densities and cycling life of practical Li-S pouch cells remain largely unsatisfactory. Traditional approaches to improving Li-S performance are primarily focused on confining polysulfides using electronically conductive hosts. However, these micro- and mesoporous hosts suffer from limited pore volume to accommodate high sulfur loading and the associated volume change during cycling. Moreover, they fail to balance adsorption-conversion of polysulfides during charge-discharge, leading to the formation of massive dead sulfur. Such hosts are themselves electrochemically inactive, which decreases the practical energy density. In contrast, a series of nontraditional approaches, paired with advances in multiscale mechanistic understanding, have recently demonstrated exciting performance outcomes not only in conventional coin cells but also in practical pouch cells. In this Account, we first introduce our novel cathode design strategies to overcome polysulfide shuttling and sluggish redox kinetics in thick S cathodes via selenium-sulfur chemistry and cathode host engineering. Next, we gain a mechanistic understanding of Li-S batteries in various types of electrolytes via a series of spectroscopic, nuclear magnetic resonance, and electrochemical methods. Meanwhile, a novel cathode solid electrolyte interphase encapsulation strategy via nonviscous highly fluorinated ether-based electrolyte is introduced. The established selection rule by investigating how solvating power retards the shuttle effect and induces robust cathode/solid-electrolyte interphase formation is also included. We then discuss how the synergistic interactions between rational cathode structures and electrolytes can be exploited to tailor the reaction pathways and kinetics of S cathodes under high mass loading and lean electrolyte conditions. In addition, a novel interlayer design to simultaneously overcome degradation processes (polysulfide shuttling and lithium dendrite formation) and accelerate redox reaction kinetics is presented. Finally, this Account concludes with an overview of the challenges and strategies to develop Li-S pouch cells with high practical energy density, long cycle life, and fast-charging capability.

25 ENERGY STORAGE↗

DOE OSTI2024

Control, Fault Management, and Grid Support Functionality of an MV AC-DC Solid State Transformer based EV Extreme Fast Charging Station

Electric vehicles (EVs) have become increasingly popular in recent times while revolutionizing the consumer and commercial transportation market. The development of charging infrastructure has become one of the priorities for increasing the adoption of EVs. Extreme fast charging (XFC) technology can reduce the so-called ’range anxiety’ of consumers as they significantly reduce the charging time. With the advent of wide band-gap (WBG) power devices and improvement in power electronic converters, medium voltage (MV) solid state transformer (SST) based XFC system has the potential to replace the traditional XFC stations because of the lower footprint, ease of installation, enhanced control feature, and better system efficiency. The control system design is one of the critical aspects of the SST development process. Careful consideration and detailed analysis are required to find out suitable control method for the SST based on its topology among different centralized and decentralized control architectures. Also, the control parameters selection and potential improvement to the transient response of the controller ought to be investigated. Another major concern of the SST is different types of internal fault which reduces the overall reliability of the XFC system. As a result, designing a robust protection system is essential. Among different fault modes, open circuit switch faults have received significant attention as an active research area because of their likelihood and severe effects on converters. Therefore, the power stages used in the XFC system require functional and accurate open circuit switch fault management methods. An equally significant aspect of this SST based XFC is its compatibility in a microgrid where there is no synchronous generator present. When the grid is not available, the XFC SSTs can provide grid forming capability and continue supplying the critical loads in islanded mode. The transition between grid connected and islanded mode, especially the grid resynchronization process has to be carefully performed for the safety of the microgrid components. The challenges posed by the aforementioned issues have inspired the work done in this dissertation. Here, a 13.2 kV, 1 MVA, AC/DC SST for the XFC system is examined and a comparative analysis is conducted to select the control architecture based on feasibility of implementation and performance. A detailed control parameter design process is demonstrated considering the sensor dynamics and delay. The selected decentralized control method is augmented by introducing a novel sensor-less load current feedforward method to provide better voltage regulation at the DC bus during a change of load. Next, in the fault management section, a hierarchical failure mode effect analysis (FMEA) is proposed to enable a systematic design of the internal fault protection of the XFC SST as there are limited examples in the literature regarding the analysis of the safety and design of the protection of a power electronic converter system. Novel open circuit switch fault management methods for the converters in the system are presented. Finally, XFC SST based MV microgrid operations in grid connected mode and islanded mode are explored. A secondary control method for grid resynchronization is presented and a design process of control parameters is shown to ensure the stability of the secondary voltage and frequency regulation.

30 DIRECT ENERGY CONVERSION↗

NASA NTRSDate not supplied

Electric Sail Design Sensitivities

Electric Sails (E-Sails) are a promising propulsion technology that seek to enable high characteristic propellentless acceleration for spacecraft to reach distant and/or difficult to reach orbits such as rapid transit to heliopause. The E-Sail system exchanges momentum by using positively charged electrostatic tethers to repel solar wind photons to push it through space. This concept was first theorized by Pekka Janhunen in 2004 with further developments occurring including a NASA Innovative Advanced Concepts Phase 1 and Phase 2 hosted out of NASA’s Marshall Space Flight Center (MSFC). These developments led to further maturation of the overall system, and this paper is designed to help identify different design sensitivities of an integrated Electric Sail system. To approach this, a small team at MSFC took an in-house developed three degrees of freedom (3DoF) simulation tool and a trajectory modelling tool to look at different design parameters and to determine a potential ideal E-Sail configuration. An E-Sail system has different design architectures including a barbell design, hub and spoke design, and a potential hybrid solution. The barbell design features two equally massed satellites that spin around a central point in the tether system. The hub and spoke design features a large central spacecraft with small end spacecraft to aid in formation control of the overall E-Sail system. Leveraging elements from both the hub and spoke, and barbell design, a hybrid option exists where one could have a larger central mass and one or two tethers extended to a smaller end mass [2]. In summary, the hub and spoke design is the ideal configuration for E-Sail with tethers spanning kilometers to achieve the designed design characteristic acceleration of at least one mm/s2 with this architecture being the focus of this study. Different key design parameters were varied as part of this study. These parameters include the total number of tethers, the length of the tethers, spin rate, relative spacecraft mass, tether voltage, inertia per tether, and impact of slew rate changes. These results started from an internal MSFC technology demonstration mission design and then the parameters were varied with engineering judgement to ensure that the results were consistent with expected results. These were varied in the MSFC 3DoF tool and compared to baseline results to generate a candidate ideal E-Sail design system. These results were then used to help inform the mission analysis design for the system. The 3DoF trajectory optimization was performed in the Astrodynamics and Space Science Enabling Toolbox (ASSET) and utilized collocation optimization of control vector pointing with the objective function being transfer duration. A representative model of the E-Sail force was derived as a function of the Sun-pointing vector direction. This model was initialized with a zero Sun Incidence Angle (SIA) trajectory for the initial guess generation, then with a portion of the mission optimized SIA time history for fast outbound transfers. After the trajectory is hyperbolic relative to a heliocentric frame, the SIA is maintained at 0 degrees except for any needed trajectory correction maneuvers. This trajectory optimization looked at different characteristic acceleration values to analyze the impact it had on mission performance. As a result of this study, the team can best inform mission designers and technology development efforts to mature the E-Sail system. This study will allow mission designers to have defined rules-of-thumb to design an E-Sail system to meet desired mission needs as well as providing several sample mission profiles. These design drivers will inform maturation efforts on which design requirements to consider for an integrated E-Sail design.

E-Sail↗

NASA NTRS2018

Development of the Electrostatic Precipitator (ESP) for Mars and Electrodynamic Dust Shield (EDS)

Kennedy Space Center's Swamp Works is a fast-paced and diverse technology development laboratory that aims to advance commercial and government capabilities to colonize extraterrestrial environments. As a part of Swamp Works, the Electrostatic and Surface Physics Laboratory (ESPL) is currently developing new technologies that will further NASA's capabilities to colonize lunar and Martian environments. At the ESPL, the objective of the overall project is to aid in the dust mitigation of robotic and human exploration missions to the moon and Mars. The moon and Mars are covered with layers of dust, which can make long-term exploration missions very difficult. The team at the ESPL is developing an electrostatic precipitator (ESP) to aid in the reduction of interference from airborne Martian dust on equipment. The ESP is designed to mitigate the dust in an intake of CO2-rich dusty gas (i.e., the Martian atmosphere). The ESP is essentially a cylindrical tube with a coaxial wire electrode. Applying a high voltage through this electrode induces a corona discharge (a glowing plasma that envelops the electrode), which is used to charge the inflowing dust. The electric field caused by the corona pushes the charged dust to the walls of the precipitator, preventing the dust to flow out of the tube. Environmental dust can make long-term exploration missions very difficult, and settled dust is no exception. Settled lunar or Martian dust can hinder the performance and lifetime of equipment. For example, dust can settle on the solar panels of a lunar or Martian rover, decreasing its performance while increasing its charging time. To address this, the team at the ESPL is also developing an electrodynamic dust shield (EDS), which is designed to remove lunar or Martian dust from the surfaces of equipment. The EDS uses a non-uniform electric field to generate a dielectrophoretic force, which pushes the particles away from the surface of the shield. A number of dust shields will be tested on the exterior of the International Space Station (ISS) via MISSE-11, a flight payload to the ISS that will test the effects of long-term exposure to space on materials. During my internship at the ESPL, I aided in the development of these technologies. For the ESP, I helped characterize the electrical properties of various geometries and helped redesign the hardware of the testbed (the precipitator used to test this technology in the lab). To characterize the electrical properties of the ESP, I ran various tests of the precipitator, which consisted of varying the environmental conditions and geometry of the testbed. Analyzing the electrical properties of the ESP in various environmental conditions is necessary to characterize its collection efficiency, since it will be used in the dusty Martian environment. For the EDS, I helped analyze the dielectric strength of the surface of the shield via high-voltage testing. A dielectrically strong surface will help the shield survive the harsh environment of space, which will enable it to have both lunar and Martian applications.

Corona Discharge↗

DOE OSTI2026

An Atom-Precise Approach to Damp First-Order Phase Transitions and Its Implications for Neuromorphic Signal Processing

Neuromorphic computing inspired by mammalian intelligence aims to emulate the nonlinear dynamics of biological neurons and synapses to achieve fast, low-energy, and highly efficient information processing. Brain-inspired computing relies on the design and discovery of materials exhibiting nonlinear current–voltage profiles, frequently underpinned by electronic state transitions, to achieve spiking neurons and dynamically tunable synapses. A signature challenge in the design of artificial neurons is controlling the steepness of first-order transitions in active elements, as abrupt transitions are at risk of driving unstable voltage and temperature oscillations, which result in catastrophic device failure. A critical knowledge gap is the lack of structure–function correlations mapping the composition and atomistic structure of crystalline solids to nonlinear dynamical response characteristics. Here, we address the key question of how modification of atomistic structure correlates with alteration of neuron-like functionality. Constructing oscillator circuits from millimeter-scale single crystals enables high-resolution atomic structure solutions, which we use to demonstrate that the selective positioning of Pb cations modifies charge ordering along a one-dimensional CuxV2O5 framework even at low insertion stoichiometries, thereby providing an atom-precise design parameter for damping first-order transitions. We use temperature-variant X-ray diffraction and X-ray spectroscopy to elucidate the suppression of Cu-ion shuttling based on the precise positioning of Pb ions in seven-coordinated tunnel interstitial sites as the mechanistic basis for transition broadening, thus bridging a critical gap between statistical mechanics and quantum chemical descriptions of phase transitions. Such mechanistic understanding thus paves the way to site-selective modification strategies for modulating the sharpness of first-order transitions, with an exemplary demonstration here in tuning neuronal signal processing.

Crystal structure↗