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DOE OSTI2023

Physics and applications of dusty plasmas: The Perspectives 2023

Dusty plasmas are electrically quasi-neutral media that, along with electrons, ions, neutral gas, radiation, and electric and/or magnetic fields, also contain solid or liquid particles with sizes ranging from a few nanometers to a few micrometers. These media can be found in many natural environments as well as in various laboratory setups and industrial applications. As a separate branch of plasma physics, the field of dusty plasma physics was born in the beginning of 1990s at the intersection of the interests of the communities investigating astrophysical and technological plasmas. An additional boost to the development of the field was given by the discovery of plasma crystals leading to a series of microgravity experiments of which the purpose was to investigate generic phenomena in condensed matter physics using strongly coupled complex (dusty) plasmas as model systems. Finally, the field has gained an increasing amount of attention due to its inevitable connection to the development of novel applications ranging from the synthesis of functional nanoparticles to nuclear fusion and from particle sensing and diagnostics to nano-contamination control. The purpose of the present perspectives paper is to identify promising new developments and research directions for the field. As such, dusty plasmas are considered in their entire variety: from classical low-pressure noble-gas dusty discharges to atmospheric pressure plasmas with aerosols and from rarefied astrophysical plasmas to dense plasmas in nuclear fusion devices. Both fundamental and application aspects are covered.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Evidence of E × B staircase in HL-2A L-mode tokamak discharges

Theory and simulation suggest the existence of an E ×B staircase in the plasma core consisting of a series of nested m/n = 0/0 E×B shear layers that regulate turbulent transport across the layers together with mesoscale transport events occurring between them. Here, we show evidence for these phenomena in HL-2A L-mode discharges. Both high resolution electron cyclotron emission Te profiles and frequency modulated continuous wave reflectometer ne profiles show multiple gradient corrugations. The analysis of simultaneous poloidally and radially separated beam emission spectroscopy turbulent density fluctuation measurements over most of the minor radius of the plasma provides the evidence of eddy tilting and propagation direction reversals largely coincident with the profile corrugations, with long-range transport events occurring between these locations. The results provide significant additional evidence for the existence of an E × B staircase that influences particle and heat transport in L-mode discharges.

Liu, Wenbin (ORCID:0000000310424117)↗

DOE OSTI2023

Reducing ion diffusion at atmospheric pressure through intermingled positive and negative ions

Increasing ion molecule reaction times for ambient ionization techniques can increase sensitivity of detection. Longer reaction times result in an increase in analyte signal relative to the reactant ion signal, however with a subsequent decrease in the total ion intensity. This loss in the total number of ions reaching the detector limits the extent to which increased reaction time can improve detection in practical applications. In this study ion loss was measured using either electric fields or gas flow to control ion transit time. Ion transit times ranged from 40 ms to 8s, which resulted in ion densities ranging from 5 x 10 6 to 2 x 10 4 ions/cm 3 , respectively. These results provide insights into practical reaction time limitations or experimental boundaries when exploring sensitivity enhancements in ambient ionization. When exploring longer reaction times with an atmospheric flow tube coupled to a mass spectrometer (AFT-MS), an additional corona discharge ionization source of the same polarity was added in an attempt to increase total ion signal, but no improvement in signal was observed. This observation suggested that there was a maximum ion density being reached by the corona discharge that could not be increased by adding more of the same polarity ions. A hypothesis was that intermingling both polarities of ions would reduce ion loss and increase the measured ion signal. When two corona discharge sources—one each of positive and negative polarity—were used simultaneously in an AFT-MS, the total ion signal of either polarity measured by the MS was approximately double the current from a single corona discharge source. An increase in the negative ion signal was also observed when ~10 parts-per-trillion vapor levels of an explosive (RDX) were introduced. In this case both the nitrate reactant ions and the RDX signal more than doubled with the addition of a corona discharge source producing positive ions. When intermingling positive and negative ions, an increase in ion current was also observed when the AFT was coupled directly to a Faraday detector or to an ion mobility spectrometer. This was the first demonstration of interfacing the AFT to an IMS. The observations and developments from this work will help in creating more portable instruments with improved sensitivity for detection of chemicals.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

SGD-OD: investigating the potential oxygen demand of submarine groundwater discharge in coastal systems

Submarine groundwater discharge (SGD) supplies nutrients, carbon, metals, and radionuclide tracers to estuarine and coastal waters. One aspect of SGD that is poorly recognized is its direct effect on dissolved oxygen (DO) demand in receiving waters, denoted here as SGD-OD. Sulfate-mediated oxidation of organic matter in salty coastal aquifers produces numerous reduced byproducts including sulfide, ammonia, dissolved organic carbon and nitrogen, methane, and reduced metals. When these byproducts are introduced to estuarine and coastal systems by SGD and are oxidized, they may substantially reduce the DO concentration in receiving waters and impact organisms living there. We consider six estuarine and coastal sites where SGD derived fluxes of reduced byproducts are well documented. Using data from these sites we present a semiquantitative model to estimate the effect of these byproducts on DO in the receiving waters. Without continued aeration with atmospheric oxygen, the study sites would have experienced periodic hypoxic conditions due to SGD-OD. The presence of H2S supplied by SGD could also impact organisms. This process is likely prevalent in other systems worldwide.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Performance Investigation of High-temperature Latent Heat Storage for Integration with Advanced Nuclear Reactors

Integrating thermal energy storage (TES) with advanced nuclear reactors enhances the flexible use of nuclear energy, facilitating its expansion beyond conventional electricity generation. High-temperature TES, capable of storing heat above 400 degree C, emerges as a vital carbon-free energy solution for decarbonizing industrial sector, especially when combined with low-emission energy sources like advanced nuclear reactors. Idaho National Laboratory (INL) has recently developed a novel design for high-temperature latent heat storage system, called Heat pipe Integrated Thermal Battery (HITB), and efforts are underway to experimentally demonstrate the concept. HITB employs liquid-metal heat pipes to establish thermal linkage between TES and nuclear systems without direct fluid exchange, minimizing the potential risk of the integrated systems such as cross-contamination. HITB is designed to achieve high charging and discharging efficiency as well as high energy storage density by employing metal alloys as Phase Change Material (PCM). Initial proof-of-concept experiments are being undertaken using an aluminum alloy (Al59%-Mg35%-Zn6%). This paper discusses current progress of the HITB project at INL, seeking to develop high-temperature TES for versatile integration with advanced nuclear reactors, and shares insights from the performance evaluations via numerical modeling and analysis.

25 ENERGY STORAGE↗

DOE OSTI2023

Long-Term Changes in Concentration and Yield of Riverine Dissolved Silicon From the Poles to the Tropics

Riverine exports of silicon (Si) influence global carbon cycling through the growth of marine diatoms, which account for ~25% of global primary production. Climate change will likely alter river Si exports in biome-specific ways due to interacting shifts in chemical weathering rates, hydrologic connectivity, and metabolic processes in aquatic and terrestrial systems. Nonetheless, factors driving long-term changes in Si exports remain unexplored at local, regional, and global scales. We evaluated how concentrations and yields of dissolved Si (DSi) changed over the last several decades of rapid climate warming using long-term data sets from 60 rivers and streams spanning the globe (e.g., Antarctic, tropical, temperate, boreal, alpine, Arctic systems). We show that widespread changes in river DSi concentration and yield have occurred, with the most substantial shifts occurring in alpine and polar regions. The magnitude and direction of trends varied within and among biomes, were most strongly associated with differences in land cover, and were often independent of changes in river discharge. These findings indicate that there are likely diverse mechanisms driving change in river Si biogeochemistry that span the land-water interface, which may include glacial melt, changes in terrestrial vegetation, and river productivity. Finally, trends were often stronger in months outside of the growing season, particularly in temperate and boreal systems, demonstrating a potentially important role of shifting seasonality for the flux of Si from rivers. Our results have implications for the timing and magnitude of silica processing in rivers and its delivery to global oceans.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen

Hydrogen cyanide (HCN) is synthesized from ammonia (NH 3 ) and methane (CH 4 ) at ~1200°C over a Pt catalyst. Ammonia synthesis entails several complex, highly emitting processes. Plasma-assisted HCN synthesis directly from CH 4 and nitrogen (N 2 ) could be pivotal for on-demand HCN production. Here, we evaluate the potential of dielectric barrier discharge (DBD) N 2 /CH 4 plasma for decentralized catalyst-free selective HCN production. We demonstrate a single-step conversion of methane and nitrogen to HCN with a 72% yield at <300°C. HCN is favored at low CH 4 concentrations with ethane (C 2 H 6 ) as the secondary product. We propose a first-principles microkinetic model with few electron impact reactions. The model accurately predicts primary product yields and elucidates that methyl radical (·CH 3 ) is a common intermediate in HCN and C 2 H 6 synthesis. Compared to current industrial processes, N 2 /CH 4 DBD plasma can achieve minimal CO 2 emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Final Scientific Report on: Magnetized Shock Physics and Convergent Flows

The objective of this project was to study magnetized shocks in plasmas using the Omega Laser Facility to drive a solid foil into a magnetized gas, which would be preionized by the x-rays from the laser-solid interaction. The MIFEDS (magneto-inertial fusion electrical discharge system) provided the magnetic field. Magnetized shocks are of interest in magneto-inertial fusion, such as MagLIF and magnetized spherical implosions with both direct and indirect drive, space physics, heliophysics, and astrophysics. In magneto-inertial fusion the shocks of interest are collisional and perpendicular to the magnetic field lines, since the magnetic field needs to be compressed. In space, the shocks of interest are typically collisionless, due to the low plasma density, and both perpendicular and parallel to the magnetic field. The marginally collisionless regime between these is also of interest in both laboratory, fusion, and space plasmas, but has barely been investigated.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Review of the gas breakdown physics and nanomaterial-based ionization gas sensors and their applications

Ionization gas sensors are ubiquitous tools that can monitor desired gases or detect abnormalities in real time to protect the environment of living organisms or to maintain clean and/or safe environment in industries. The sensors’ working principle is based on the fingerprinting of the breakdown voltage of one or more target gases using nanostructured materials. Fundamentally, nanomaterial-based ionization-gas sensors operate within a large framework of gas breakdown physics; signifying that an overall understanding of the gas breakdown mechanism is a crucial factor in the technological development of ionization gas sensors. Moreover, many studies have revealed that physical properties of nanomaterials play decisive roles in the gas breakdown physics and the performance of plasma-based gas sensors. Based on this insight, this review provides a comprehensive description of the foundation of both the gas breakdown physics and the nanomaterial-based ionization-gas-sensor technology, as well as introduces research trends on nanomaterial-based ionization gas sensors. The gas breakdown is reviewed, including the classical Townsend discharge theory and modified Paschen curves; and nanomaterial-based-electrodes proposed to improve the performance of ionization gas sensors are introduced. The secondary electron emission at the electrode surface is the key plasma–surface process that affects the performance of ionization gas sensors. Finally, we present our perspectives on possible future directions.

nanomaterial-based gas breakdown characteristics↗

DOE OSTI2024

Numerical thermalization in 2D PIC simulations: Practical estimates for low-temperature plasma simulations

The process of numerical thermalization in particle-in-cell (PIC) simulations has been studied extensively. It is analogous to Coulomb collisions in real plasmas, causing particle velocity distributions (VDFs) to evolve toward a Maxwellian as macroparticles experience polarization drag and resonantly interact with the fluctuation spectrum. This paper presents a practical tutorial on the effects of numerical thermalization in 2D PIC applications. Scenarios of interest include simulations, which must be run for many thousands of plasma periods and contain a population of cold electrons that leave the simulation space very slowly. This is particularly relevant to many low-temperature plasma discharges and materials processing applications. We present numerical drag and diffusion coefficients and their associated timescales for a variety of grid resolutions, discussing the circumstances under which the electron VDF is modified by numerical thermalization. Though the effects described here have been known for many decades, direct comparison of analytically derived, velocity-dependent numerical relaxation timescales to those of other relevant processes has not often been applied in practice due to complications that arise in calculating thermalization rates in 1D simulations. Using these comparisons, we estimate the impact of numerical thermalization in several examples of low-temperature plasma applications including capacitively coupled plasma discharges, inductively coupled plasma discharges, beam plasmas, and hollow cathode discharges. Finally, we discuss possible strategies for mitigating numerical relaxation effects in 2D PIC simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

High-Peak-Power Long-Wave Infrared Lasers with CO2 Amplifiers

Long-wave infrared (LWIR) picosecond pulses with multi-terawatt peak power have recently become available for advanced high-energy physics and material research. Multi-joule pulse energy is achieved in an LWIR laser system via amplification of a microjoule seed pulse with high-pressure, mixed-isotope CO 2 amplifiers. A chirped-pulse amplification (CPA) scheme is employed in such a laser to reduce the nonlinear interaction between the optical field and the transmissive elements of the system. Presently, a research and development effort is underway towards an even higher LWIR peak power that is required, for instance, for promising particle acceleration schemes. The required boost of the peak power can be achieved by reducing the pulse duration to fractions of a picosecond. For this purpose, the possibility of reducing the gain narrowing in the laser amplifiers and post-compression techniques are being studied. Another direction in research is aimed at the increased throughput (i.e., repetition rate), efficiency, and reliability of LWIR laser systems. The transition from a traditional electric-discharge pumping to an optical pumping scheme for CO 2 amplifiers is expected to improve the robustness of high-peak-power LWIR lasers, making them suitable for broad implementation in scientific laboratory, industrial, and clinical environments.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

In this work, we introduce the oxidation of long aliphatic alkanes using non-thermal, atmospheric plasma processing as an eco-friendly route for organic synthesis. A pulsed dielectric barrier discharge in He/O 2 gas mixtures was employed to functionalize n-octadecane. C 18 secondary alcohols and ketones were the main products, with an optimal molar yield of ~29.2%. Prolonged treatment resulted in the formation of dialcohols, diketones, and higher molecular weight oxygenates. Lighter hydrocarbon products and decarboxylation to CO 2 were also observed at longer treatment times and higher power inputs. A maximum energy yield of 5.48 × 10 –8 mol/J was achieved at short treatment times and high powers, associated with higher selectivity to primary oxygenates. Direct hydroxylation of alkyl radicals, as well as disproportionation reactions, are proposed as the main pathways to alcohols and ketones. The results hold promise for functionalizing long hydrocarbon molecules at ambient conditions using catalyst-free plasma discharges.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Anomalous Retrograde Drifts in Obstructed Magnetron Microdischarges: a Consequence of a Field Reversal in the Anode Sheath?

The goal of this project was to carry out experiments at the Plasma Collaborative Research Facility (Princeton Plasma Physics Laboratory) aimed at confirming or refuting the hypothesis that an electric field reversal occurs in the near-anode region of a strongly obstructed planar magnetron microdischarges. Magnetron discharges are magnetized plasmas with E x B field topologies, and variants of such discharges are widely used in materials processing. The topologies are also similar to that of Hall thrusters used in space propulsion. Understanding the structure of these discharges will aid in developing reliable simulations that are intended to facilitate the further development of such technologies, as the field reversals, presumed to be due to strong axial-driven electron transport, provides further insight into transport properties. The possible existence of such a field reversal is hinted at because of the retrograde-propagating (i.e., negative E x B) spokes or gradient-driven drift instabilities seen in the high speed videos and segmented anode probing of the plasma. The presence of this field reversal should be reflected in the ion dynamics, particularly, in an ion drift towards the anode. The proposed experiments to be conducted at the PCRF are to characterize this anode-directed ion drift using state-of-the-art laser-induced fluorescence velocimetry. In particular, we seek to see if the near-anode ion velocity reverses direction when the external circuit is varied to alter the electron current demand imposed at the anode. Such an ion velocity reversal would confirm the mechanism, which is that the highly obstructed (small gapped) discharge produces strong axial gradients in plasma density, driving more electrons towards the anode then that demanded by the external circuit.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Non-premixed counterflow methane flames in DC/AC/NS electric fields

The response of counterflow diffusion flames to sub-breakdown DC and AC electric fields, as well as their superposition with ns pulse discharge waveforms, is studied in the plane-to-plane electrode geometry. Sub-breakdown DC and low-frequency AC electric fields cause the flame displacement toward the grounded electrode, in the direction of the applied field, indicating that the body force on the positive ions exceeds that on the electrons and negative ions. As the AC frequency increases, the flame response becomes less pronounced, due to the reduction of the electrohydrodynamic (EHD) body force impulse over the AC half-period. The electric field in the electrode gap is determined by ps Electric Field Induced Second Harmonic (E-FISH) generation, with absolute calibration using sub-breakdown ns pulses overlapped with the measured electric field waveform. The results show that the electric field distribution across the flame in the current saturation regime follows the Laplacian field. This indicates that the space charge density in the gap is too low to distort the applied DC or AC field, consistent with the kinetic modeling predictions. Combining a nanosecond pulse discharge with a sub-breakdown DC field generates a diffuse plasma across the entire gap. Time-resolved and spatially resolved measurements of the electric field in the discharge indicate the ionization wave propagation between the electrodes. The present results do not exhibit a detectable flame displacement enhancement by ns discharge pulses combined with a sub-breakdown field, observed previously. Kinetic modeling calculations show that the absence of this effect in the plane-to-plane geometry is due to the rapid plasma self-shielding. This indicates that alternative electrode geometries limiting the self-shielding would be more effective for the plasma / electric field enhanced flameholding and flame stabilization applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Transition from retrograde to prograde drift instabilities in a magnetron microdischarge

Rotating plasma structures, or “spokes,” in magnetized discharges characterized by perpendicular electric and magnetic fields have been seen in a growing number of studies and are believed to be the result of gradient-driven drift instabilities. Under certain conditions, we have shown the spoke’s rotation to be opposite to the E B direction, i.e., retrograde in its expected direction. Recently, we have linked such counter-intuitive rotation to a local inversion of the electric field. Here, we give further experimental evidence for this inversion and attempt to provide an explanation for a relatively distinct transition seen between retrograde and positive (prograde) drift. In the experiments, a partially magnetized plasma forms inside a magnetron device of mm radius operated with argon. Discharge current–voltage measurements are acquired for a range of argon fill pressure and inter-electrode spacing. We find two branches of operation—a low current branch of negative resistance, coinciding with the retrograde spoke rotation, and a higher current branch of positive resistance, coincident with prograde spoke rotation. We postulate that at low discharge currents, high magnetic field confinement leads to a large density gradient, causing more electron transport to the anode than that demanded by the external circuit. At higher currents, anomalous axial electron transport (across the magnetic field lines) becomes dominant, eliminating the conditions for field inversion. Here, the current thresholds for the field inversion are found to be sensitive to the argon pressure and inter-electrode spacing.

42 ENGINEERING↗

DOE OSTI2023

Degradation and Modeling of Large-Format Commercial Lithium-Ion Cells as a Function of Chemistry, Design, and Aging Conditions

Demand for large-format (>10 Ah) lithium-ion batteries has increased substantially in recent years, due to the growth of both electric vehicle and stationary energy storage markets. The economics of these applications is sensitive to the lifetime of the batteries, and end-of-life can either be due to energy or power limitations. Despite this, there is little information from cell manufacturers on the sensitivity of cell degradation to environmental conditions or battery use. This work reports accelerated aging test data from four commercial large-format lithium-ion batteries from three manufacturers, with varying design (thickness, casings, ...), chemistry (lithium-iron-phosphate (LFP) or lithium-nickel-manganese-cobalt-oxide positive electrodes (NMC), with graphite (Gr) negative electrodes), and capacity (50 to 250 Amp hours). The tested LFP|Gr cell is found to be relatively insensitive to cycling conditions like temperature or voltage window, while NMC|Gr cells have varying sensitivity. Degradation trends are further investigated by training predictive models: simple polynomial trend lines, a semi-empirical reduced-order model, and an empirical reduced-order model identified using machine-learning based on symbolic regression. Calendar and cycle life are simulated over a variety of conditions to directly compare the various batteries. Cell size and thickness are found to substantially impact sensitivity to temperature during cycle aging, while electrode chemistry impacts depth-of-discharge sensitivity. Real-world battery lifetime is evaluated by simulating residential energy storage and commercial frequency containment reserve systems in several U.S. climate regions. Predicted lifetime across cell types varies from 7 years to 20+ years, though all cells are predicted to have at least 10 year life in certain conditions.

battery lifetime↗

DOE OSTI2022

All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating

Li 7 La 3 Zr 2 O 12 (LLZO) garnet-type lithium-ion conductors are being investigated as a promising solid electrolyte for solid-state lithium batteries. To enable a functional all-solid-state configuration intensive investigations are needed to reduce the cathode/electrolyte interfacial resistance which contributes the most to cell performance loss. Among the commercial cathode materials investigated so far, LiCoO 2 (LCO) is one of the most stable with garnet electrolytes as only a superficial reaction has been detected between the two materials. However, even this minor reaction would block the Li-ion transport through the interface, resulting in deteriorated cell performance. In this work, we demonstrate that a thin aluminum oxide layer (5 nm) can be an effective interlayer to impede the formation of a harmful interphase and enable facile Li-ion transfer between LCO and the LLZO garnet. Room-temperature-sputtered LCO thin films were employed to form an interface with the garnet electrolyte and annealed at 800 °C to reveal the effect of the interfacial reaction on the Li-ion transfer across the interface. An aluminum oxide layer was then introduced between LCO and the garnet electrolyte by sputtering a metallic aluminum layer which is then annealed together with the upper LCO layer in oxygen, or by direct atomic layer deposition of the oxide. Compared to the LCO/LLZO/Li cells without an aluminum oxide interlayer, those with the interlayer exhibited improved performance, i.e., a stable discharge capacity of up to 90 mAh/(g LCO) at a C/10 rate, a rate capability up to 1.68C and a stable galvanostatic cycling at 0.1C for over 100 cycles with a discharge capacity fade rate of 0.15% per cycle. It was determined that aluminum diffused into the LCO layer after preventing the initial detrimental reaction between LCO and the LLZO garnet from happening during high temperature annealing, suggesting that the coating does not have to remain a physically blocking layer during cycling to function.

Electrochemistry↗

DOE OSTI2021

Performance of a Hybrid HVAC-Integrated Thermal Storage Device

Thermal equipment in buildings is a primary contributor to peak loads on the electrical grid. Thermal energy storage is a cost-effective strategy to decouple electric use from thermal loads, thus reducing grid peak costs for building owners. One method for storing thermal energy in a building is to integrate a phase change material (PCM) directly into the heating, ventilation, and air conditioning system. These systems often require additional glycol loops, pumps, valves, and heat exchangers to couple the storage to the cooling system and building space, which increases the complexity and cost. This work will discuss an alternate approach where the storage is added directly into the heat pump evaporator. A detailed two-dimensional finite difference heat transfer model of a PCM-refrigerant-glycol heat exchanger was developed to simulate the performance of this component. The fluid stream was discretized along the flow direction to capture changes in the fluid properties and local heat transfer rates, and the phase change material was discretized in both the x and y directions to capture the movement of the melt front. The model was used to understand the impact of different material and geometric properties on the charge and discharge characteristics of the device. Finally, a Ragone framework analogous to that used for electrochemical batteries was used to maximize the energy density and round-trip efficiency of the device while supplying loads appropriate for space cooling in buildings.

buildings↗