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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Ultra-Fast 4H-SiC LGAD With Etched Termination and Field Plate

The design, fabrication, and demonstration of a novel Silicon Carbide Low Gain Avalanche Detector (4HSiC LGAD), exhibiting an ultra-fast time response and excellent time resolution, are reported. Here, the use of field plates is proposed to suppress the high electric field caused by the negative bevel-etched angle in 4H-SiC LGADs based on TCAD simulations. Experimental measurements confirm that the field plate significantly increases the breakdown voltage of the 4H-SiC LGADs. Gain and time resolution are measured by using the ultraviolet transient current technique (UV-TCT) showing that 4H-SiC LGADs possess excellent timing performance, with a time resolution better than 35 ps for the injected laser signal with single minimum ionizing particle (MIP) charges generation at room temperature. Additionally, the gain suppression effect in a 4H-SiC LGAD is observed for the first time.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Electrical breakdown dynamics in an argon bubble submerged in conductive liquid for nanosecond pulsed discharges

Abstract This study delves into the dynamics of cold atmospheric plasma and their interaction within conductive solutions under the unique conditions of nanosecond pulsed discharges (22 kV peak voltage, 10 ns FWHM, 4.5 kV ns −1 rate-of-rise). The research focuses on the electrical response, breakdown, and discharge propagation in an argon bubble, submerged in a NaCl solution of varying conductivity. Full or partial discharges were observed at conductivities of 1.5 µ S cm −1 (deionized water) to 1.6 mS cm −1 , but no breakdown was observed at 11.0 mS cm −1 when reducing the electrode gap. It is demonstrated that at higher conductivity electric breakdown is observed only when the gas bubble comes into direct contact with the electrode and multiple emission nodes were observed at different timescales. These nodes expanded in the central region of the bubble over timescales longer than the initial high-voltage pulse. This work offers a temporal resolution of 2 ns exposure times over the first 30 ns of the initial voltage pulse, and insight into plasma formation over decaying reflected voltage oscillations over 200 ns.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Evaluation of HPK n + - p planar pixel sensors for the CMS Phase-2 upgrade

To cope with the challenging environment of the planned high luminosity upgrade of the Large Hadron Collider (HL-LHC), scheduled to start operation in 2029, CMS will replace its entire tracking system. The requirements for the tracker are largely determined by the long operation time of 10 years with an instantaneous peak luminosity of up to 7.5 × 10 34 cm –2 s –1 in the ultimate performance scenario. Depending on the radial distance from the interaction point, the silicon sensors will receive a particle fluence corresponding to a non-ionizing energy loss of up to $\Phi_{\text {eq}}$ = 3.5 × 10 16 cm –2 . Here this paper focuses on planar pixel sensor design and qualification up to a fluence of $\Phi_{\text {eq}}$ = 1.4 × 10 16 cm –2 . For the development of appropriate planar pixel sensors an R&D program was initiated, which includes $n^+ -p$ sensors on 150 mm (6”) wafers with an active thickness of 150 μm with pixel sizes of 100 × 25 μm 2 and 50 × 50 μm 2 manufactured by Hamamatsu. Single chip modules with ROC4Sens and RD53A readout chips were made. Irradiation with protons and neutrons, as well was an extensive test beam campaign at DESY were carried out. This paper presents the investigation of various assemblies mainly with ROC4Sens readout chips. It demonstrates that multiple designs fulfill the requirements in terms of breakdown voltage, leakage current and efficiency. The single point resolution for 50 × 50 μm 2 pixels is measured as 4.0 μm for non-irradiated samples, and 6.3 μm after irradiation to $\Phi_{\text {eq}}$ = 7.2 × 10 15 cm –2 .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Layout and performance of HPK prototype LGAD sensors for the High-Granularity Timing Detector

The High-Granularity Timing Detector is a detector proposed for the ATLAS Phase II upgrade. The detector, based on the Low-Gain Avalanche Detector (LGAD) technology, will cover the pseudo-rapidity region of 2.4 < |n| < 4.0 with two end caps on each side and a total area of 6.4 m 2 . The timing performance can be improved by implanting an internal gain layer that can produce signals with a fast rising edge. It significantly improves the signal-to-noise ratio. The required average timing resolution per track for a minimum ionizing particle is 30 ps at the start and 50 ps at the end of the HL-LHC operation. This is achieved with several layers of LGAD. The innermost region of the detector would accumulate a 1MeV neutron-equivalent fluence up to 2.5 10 15 n eq /cm 2 including a safety factor of 1.5 before being replaced during the scheduled shutdowns. The addition of this new detector is expected to play an important role in the mitigation of high pile-ups at the HL-LHC. The layout and performance of the various versions of LGAD prototypes produced by Hamamatsu (HPK) have been studied by the ATLAS Collaboration. The breakdown voltages, depletion voltages, inter-pad gaps, collected charge as well as the time resolution have been measured and the production yield of large size sensors has been evaluated.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Hygrothermal aging effects on polyimide and acrylate-based adhesive materials in high-performance flat-flex cable assemblies

Flat-flex assemblies are widely used across a diverse range of technologies, including consumer electronics, automotive systems, aerospace and defense applications, and medical devices, due to their compact form factor and flexibility. However, environmental stressors like temperature and humidity are known to degrade performance over time, though the main mechanisms for degradation remain unknown. Here, in this work, we examined the aging behavior of copper/polyimide/adhesive laminate systems under varying temperature and humidity conditions, focusing on material degradation and its effects on mechanical and dielectric properties. Results show that peel strength and breakdown voltage decrease with exposure time, temperature, and humidity; spectroscopic characterization revealed that the adhesive, and not the polyimide, is the weak link in the material stack-up. The adhesive, identified as a butyl acrylate-acrylonitrile (BA-AN) copolymer, exhibited age-related spectral changes that correlated with exposure severity and duration. Hydrolysis at BA ester and AN nitrile groups was identified as the primary degradation mechanism, producing amides, acids, and alcohols. We developed a mechanistic model that connects kinetic parameters for BA-AN spectral band decay to peel strength and breakdown voltage, and implicates hydrolysis at the AN moiety, not BA, in performance decrements. Modeling predictions at ambient conditions indicate faster decline in peel strength than dielectric strength at early times, followed by plateauing of both properties at longer times. These findings provide critical insights into laminate aging mechanisms and highlight the importance of addressing BA-AN degradation to improve the long-term reliability of these systems in high-humidity environments.

organic↗
DOE OSTI2022

Properties and device performance of BN thin films grown on GaN by pulsed laser deposition

Wide and ultrawide-bandgap semiconductors lie at the heart of next-generation high-power, high-frequency electronics. Here, in this paper, we report the growth of ultrawide-bandgap boron nitride (BN) thin films on wide-bandgap gallium nitride (GaN) by pulsed laser deposition. Comprehensive spectroscopic (core level and valence band x-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and Raman) and microscopic (atomic force microscopy and scanning transmission electron microscopy) characterizations confirm the growth of BN thin films on GaN. Optically, we observed that the BN/GaN heterostructure is second-harmonic generation active. Moreover, we fabricated the BN/GaN heterostructure-based Schottky diode that demonstrates rectifying characteristics, lower turn-on voltage, and an improved breakdown capability (~234 V) as compared to GaN (~168 V), owing to the higher breakdown electrical field of BN. Our approach is an early step toward bridging the gap between wide and ultrawide-bandgap materials for potential optoelectronics as well as next-generation high-power electronics.

42 ENGINEERING↗
DOE OSTI2023

Low RF loss conductive ceramic for high power input coupler windows for SRF cavities

High power RF couplers connect transmission lines to cavities, providing power used to accelerate particle beam • Coupler also provides vacuum barrier for beam vacuum via RF windows • RF windows experience breakdown at much lower voltages than comparable insulators in DC fields • For large voltages, electron emission from “triple junction” and multipacting lead to window failure due to arching and/or thermal runaway.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

Fast Growth of Ga2O3 on Highly Offcut (100)-Oriented Substrates

Beta-Ga2O3 has emerged as a leading candidate for next-generation power electronics, radio frequency (RF) switches, and extreme environment electronics due to a wide band gap (4.6 - 4.9 eV), high dopability (approximately 40 meV activation energy for an isolated silicon donor), and melt growth characteristics resulting in commercially available 4-inch substrates and commercial demonstrations of 6-inch substrates by multiple techniques. The (100) surface of Ga2O3 is highly desirable from a device and epitaxy standpoint - bulk growth of (100) material is more scalable than (010), the surface is nearly lattice-matched to p-type partner NiO, and Al2O3 incorporates at higher concentrations without phase separation. More importantly, the impact ionization coefficients along the [100] direction are low, leading to the highest possible critical fields. This is advantageous compared to the current state of the art, (001), due to reduced surface defects and increased possible breakdown voltage. However, the epitaxial growth rate on (100) surfaces is less than 10% of other faces due to weak bonding and favorable desorption, and on-axis (100) growth easily forms twin domains. Recent demonstrations have shown growth rate improvements from 0.4 nm/min to 1.5 nm/min by growing on (100) wafers that are offcut 6 degrees in the -c direction. These films show step-flow growth from (20-1) step-edges and high electron mobility due to suppressed twins. Despite these exciting results, offcuts greater than 6 degrees have not been explored due to the waste associated with grinding and polishing large offcuts. In this talk we will discuss the molecular beam epitaxy (MBE) growth and properties of Beta-Ga2O3 grown on (100) substrates offcut in the -c direction up to 13.4 degrees. These large offcuts are enabled by edge-fed film-defined growth (EFG) where the offcut is grown into the surface by pulling the crystal through the EFG die with the seed crystal rotated by the desired offcut angle. We will demonstrate that 13.4 degrees offcut substrates still exhibit a terraced (100) surface, and that a >10x increase (>5 nm/min) in growth rate is achieved. As previously reported on lower offcuts, we observe reversal of substrate twin domains around the (001) direction at the substrate-epilayer interface. We will discuss electrical properties including record-low (by MBE) unintentional doping densities of < 5E15 cm-3 and critical breakdown field in Schottky barrier diodes comparable with state-of-the-art (001) Ga2O3 without edge termination.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Interactions between atmospheric pressure plasmas and metallic catalyst particles in packed bed reactors

Atmospheric-pressure plasmas sustained in packed bed reactors (PBRs) are being investigated for chemical conversion of gases and pollution control. Metallic catalysts added to the surfaces of the dielectric beads of PBRs can increase the energy efficiency and selectivity of chemical processes by reducing operating temperature and providing additional reaction pathways. In this paper, results from a computational investigation of plasma surface interactions between micron-scale metallic catalysts and humid-air plasmas in PBRs are discussed. Here we found that high plasma density regions form in the proximity of the metallic catalysts. These higher-density plasma regions were confirmed experimentally using ICCD imaging. The intense plasmas result from geometrical electric field enhancement and redistribution of charges within the conductive particles, leading to further enhancement. The high electric field at the triple points of the catalysts can produce electric field emission of electrons, which provides a pre-ionization source or additional source of electrons. These regions of high electric field and sources of electrons guide discharges towards the catalysts and increases fluxes of excited species, ions, electrons and photons to their surfaces. These fluxes are focused primarily at the triple points between the metal, dielectric and gas. As a result, the catalyst is locally heated, which could lead to further increased rates of thermocatalytic reactions on the surface. Surface roughness of the metal inclusions can lead to additional electric field enhancement, which changes the character of the discharges in the vicinity of the catalysts while reducing breakdown voltage.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Electric Drive Technologies Consortium (EDTC)/ Cost competitive, high-Performance, highly Reliable (CPR) Power Devices on 4H-SiC (Final Report)

4H-Silicon carbide (4H-SiC) is a wide bandgap semiconductor that offers superior material properties over silicon, including higher critical electric field, thermal conductivity, and electron saturation velocity. These advantages make 4H-SiC highly attractive for high-voltage, high-efficiency power electronics. However, realizing the full potential of SiC requires device technologies that are not only high-performing but also manufacturable and reliable under real-world operating conditions. This report summarizes the outcomes of a five-year R&D effort funded by the U.S. Department of Energy (DOE) under the Electric Drive Technologies Consortium (EDTC), focused on developing cost-competitive, high-performance, and highly reliable (CPR) power devices on 4H-SiC substrates. The program targeted scalable and manufacturable 1.2 kV-class SiC MOSFETs optimized for next-generation electric vehicles, renewable energy systems, and industrial power conversion. The project delivered transformative advancements in SiC power device performance and ruggedness. Particularly, Specific on-resistance (R on,sp ) was reduced by up to 37%, from ~4.0 m$\Omega \cdot$cm 2 in earlier designs to an industry-leading 2.40 m$\Omega \cdot$cm 2 , driven by optimized doping, refined JFET widths, and layout engineering. Breakdown voltages (BV) exceeded 1600 V, marking improvement over legacy baselines, and demonstrating the robustness of newly implemented junction profiles and edge terminations. Short-circuit withstand time (SCWT) saw a remarkable 4$\times$ increase, from ~2 $\mu$s to over 8 $\mu$s, achieved through the successful deployment of deep P-well structures (~1.8–2.0 $\mu$m) via channeling implantation. This innovative process breakthrough enabled precise junction formation without MeV-class implantation tools, reduced leakage under high field stress, and allowed even the shortest-channel devices (down to 0.3 $\mu$m) to achieve both high BV and excellent ruggedness—breaking the traditional trade-off between conduction efficiency and blocking capability. Several novel architectures pushed the performance envelope further. JBSFETs—featuring embedded Schottky portions—eliminated bipolar degradation and drastically reduced third-quadrant leakage, while Ladder MOSFETs introduced a clever orthogonal conduction path that achieved a 15.4% reduction in R on,sp over standard linear designs. Switching performance reached new benchmarks: short-channel devices showed a 31% reduction in total switching energy compared to 0.5 $\mu$m counterparts, while maintaining manageable gate drive requirements. Layout-optimized structures not only improved transconductance but also accelerated switching transitions, pointing to real-world benefits in converter-level efficiency. The devices also passed rigorous reliability validation. Stress-tested across TDDB, HTGB, HTRB, HVP, and burn-in, the devices screened under 30 V/10 hr and 43 V/1 s protocols consistently exhibited tighter lifetime distributions and long-term oxide robustness. These screening techniques proved effective in identifying latent defects and ensuring deployment-grade reliability. Meanwhile, advanced 3D TCAD simulations revealed and resolved electric field hotspots—particularly in HEXFET corners—where fields exceeding 4.8 MV/cm were mitigated through geometry-aware layout corrections. Overall, the results of this project demonstrate a manufacturable and scalable SiC power device platform that addresses key DOE performance targets for efficient, robust, and reliable 1.2kV 4H-SiC Power Devices. The developed technologies represent a meaningful step forward in the commercial readiness of high-voltage SiC solutions and provide a strong foundation for continued advancement in wide bandgap power electronics.

42 ENGINEERING↗
DOE OSTI2025

Electrical and structural characterization of in situ MOCVD Al2O3/β-Ga2O3 and Al2O3/β-(AlxGa1−x)2O3 MOSCAPs

This study investigates the electrical and structural properties of metal–oxide–semiconductor capacitors (MOSCAPs) with in situ metal-organic chemical vapor deposition-grown Al2O3 dielectrics deposited at varying temperatures on (010) β-Ga2O3 and β-(AlxGa1−x)2O3 films with different Al compositions. The Al2O3/β-Ga2O3 MOSCAPs exhibited a strong dependence of electrical properties on Al2O3 deposition temperature. At 900 °C, reduced voltage hysteresis (∼0.3 V) with improved reverse breakdown voltage (74.5 V) was observed, corresponding to breakdown fields of 5.01 MV/cm in Al2O3 and 4.11 MV/cm in β-Ga2O3 under reverse bias. In contrast, 650 °C deposition temperature resulted in higher voltage hysteresis (∼3.44 V) and lower reverse breakdown voltage (38.8 V) with breakdown fields of 3.69 and 2.87 MV/cm in Al2O3 and β-Ga2O3, respectively, but exhibited impressive forward breakdown field, increasing from 5.62 MV/cm at 900 °C to 7.25 MV/cm at 650 °C. High-resolution scanning transmission electron microscopy (STEM) revealed improved crystallinity and sharper interfaces at 900 °C, contributing to enhanced reverse breakdown performance. For Al2O3/β-(AlxGa1−x)2O3 MOSCAPs, increasing Al composition (x) from 5.5% to 9.2% reduced net carrier concentration and improved reverse breakdown field contributions from 2.55 to 2.90 MV/cm in β-(AlxGa1−x)2O3 and 2.41 to 3.13 MV/cm in Al2O3. The electric field in Al2O3 dielectric under forward bias breakdown also improved from 5.0 to 5.4 MV/cm as Al composition increased from 5.5% to 9.2%. The STEM imaging confirmed the compositional homogeneity and excellent stoichiometry of both Al2O3 and β-(AlxGa1−x)2O3 layers. These findings demonstrate the robust electrical performance, high breakdown fields, and excellent structural quality of Al2O3/β-Ga2O3 and Al2O3/β-(AlxGa1−x)2O3 MOSCAPs, highlighting their potential for high-power electronic applications.

Bhuiyan, A. F. M. Anhar Uddin (ORCID:0000000334212↗
DOE OSTI2023

Investigation of SF6 Alternatives in Spark Gap Switches for GWP Reduction

This primary purpose of this project was to evaluate alternative gas mixtures to sulfur hexafluoride (SF6) developed for high voltage power delivery applications for use in high voltage spark gap switches. These SF6 alternatives lower global warming potential emissions and enable improvements to the pressure-voltage design space. A combined experimental, computational, and theoretical study was used to quantify the impact of persistent breakdown products on the breakdown distribution of SF6-replacement gas mixtures. Viable SF6 replacements suitable for use in spark gap switches were studied to enable performance and agility improvements for next-generation pulsed power research relevant to national security missions. Experimental campaign included establishing parameters of switch gases as function of concentration. Various concentrations and pressures were tested for trends in breakdown voltage, repeatability, and durability, and breakdown constituents. A zero-dimensional plasma global model was used to simulate the plasma arc decay and recombination process in spark-gap switches relevant to the Z machine. Finally, a complete and consistent set of electron-neutral collision cross-sections for the novel insulating gas C4F7N is reported.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Vacuum Insulator Flashover Physics LDRD Report

Large, pulsed power and high voltage systems often employ a stack of insulators to separate a vacuum section away from water or oil sections. The size of this insulator stack often drives overall costs and feasibility of these systems. An electric breakdown along the insulator surface is a primary failure mechanism and is especially impactful if it occurs while power is still being delivered downstream. This report describes a set of experimental and modeling investigations into the cause of these breakdowns, especially focusing on the much less well-understood anode-initiated breakdowns that occur during early parts of power delivery. Additionally, new diagnostics for assessing relevant material properties and behavior of insulators are described. These results describe breakdown behavior and evolution at new temporal and spatial fidelities and provide hypotheses and some answers as to how these breakdowns can occur. This new understanding of the roles of different physics phenomena guide modifications and trade-offs in generating newer insulator stack designs that are smaller and/or have higher electrical stress thresholds.

42 ENGINEERING↗
DOE OSTI2024

Triboplasma assisted chemical conversion in granular systems: a semi-analytic model

We present a semi-analytic model for a novel plasma-assisted chemical conversion pathway using triboplasmas generated in granular flows. Triboelectric charge relaxation is a well known phenomena where the potential generated from contact charging of particles exceeds the breakdown voltage of the background gas. In this work, we extend the triboelectric charge relaxation theory to include non equilibrium plasma energy and particle balance equations to predict the formation of dissociated and excited species that act as precursors to chemical conversion, for example in plasma-assisted ammonia synthesis. Our example case study with nitrogen background gas and teflon/aluminum tribomaterial system yielded high excited nitrogen species densities per collision that are comparable to current plasma-assisted conversion pathways. We also present a regime diagram for various gases where Paschen breakdown parameters are used to determine whether triboplasmas can be formed for a given effective work-function difference between two materials. Our sensitivity studies indicate particle velocity, particle radius, solids fraction and space charge effects play a critical role in overall plasma densities and excited species production.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Effect of Coaxial Electrode Geometry on the Electric Field Enhancement Factor for a High Voltage Vacuum Gap

We present an experimental analysis of the change in the electric field enhancement factor with varying gap size and penetration depth (P.D) of cathode into anode for a coaxial vacuum gap, diagnosed using Fowler–Nordheim analysis and optical imaging via scanning electron microscope (SEM) and time integrated Digital single lens reflex camera (DSLR). Data were collected on the Coaxial Gap Breakdown Machine (240 A, 25 kV, 150 ns, 0.1 Hz). Experiments using five different gap sizes at nine different P.Ds are compared over runs comprising 50 shots for each case. The results show a strong link between enhancement factor and gap size, with P.D and surface topology. For large gap sizes, 150, 330, and 700 μm, the average enhancement factor value increases with increasing P.D. For smaller gap sizes, 50 and 100 μm, the average enhancement factor decreases with P.D. SEM imaging before and after plasma formation for each gap size allows for quantifying surface finish, microprotrusion growth, average blast diameter, and an estimation of the surface area breakdowns occupy. Time integrated DSLR imaging analysis of the gap at each shot allows for a determination of the distribution of breakdowns about the circumference of the gap for each case tested. Here, the Fowler–Nordheim analysis allows for a quantitative analysis of the surface roughness of all gap sizes tested. Results show that for large gap sizes, the gap geometry and increasing area of breakdown is the main cause for increasing average enhancement factor. For small gap sizes, the dominant driving factor for small average enhancement factors—that subsequently decrease with P.D—is significant changes in surface topology due to an increased number of breakdowns.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Exploring the Basic Physical Mechanisms of Cathode- and Anode-Initiated High-Voltage Surface Flashover

Surface flashover in vacuum imposes a substantial physical limit on modern, large-scale pulsed power. One of the ramifications is a minimum size requirement for new machines, which in itself becomes a hard barrier to the modernization and improvement of existing infrastructure. Pulsed power topologies require the physical mechanisms of both anode- and cathode-initiated flashover to be considered. Originally, the geometrical implications of field emission at the cathode triple junction (CTJ) motivated the usage of configurations that avoid electrons impinging on the insulating material. This will largely suppress the cathode-initiated flashover, which is best described by the secondary electron avalanche mechanism, gas desorption, and final breakdown in the desorbed gas. It depends on the cascade growth of a conducting plasma along the length of the insulator from the cathode. Mitigating the cathode-initiated flashover typically comes at the cost of a significant field enhancement at the anode triple junction (ATJ). In a typical implementation, the anode field may be three times higher than the cathode field for a given voltage, making the corresponding anode-initiated flashover much more common than otherwise. In the case of pulsed, anode-initiated flashover, experimental evidence suggests that charge is directly extracted from the insulator resulting in the insulator taking on a net positive charge advancing the anode potential. Furthermore, along with accompanying gas desorption from the surface, the potential will then propagate from the anode toward the cathode until the effective length of the gap is sufficiently reduced to support flashover. The underlying physical mechanisms of cathode- and anode-directed flashover are discussed in light of previously gathered experimental data and recent experiments with pulsed, high-gradient, anode-initiated flashover.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

High power actively Q-switched downhole LIBS analysis systems

An actively Q-switched laser induced breakdown spectroscopy (LIBS) probe, utilizing an optical fiber, a pump beam transmitted through the optical fiber, a coupler, and a lens for collimating the pump beam. The actively Q-switched laser, coupled to a sensor which provides information to a computer that controls a high voltage pulser providing a pulse to a Pockels cell located within the laser which can selectively cause the laser to pulse, resulting in high energy pulses and a second lens for focusing the output pulse such that it creates a plasma or spark. The light from the spark is captured and directed back through an optical system to remote equipment for elemental and/or molecular analysis.

McIntyre, Dustin Langdon↗
DOE OSTI2020

Mathematical Modeling of Hydroxide-Exchange-Membrane Water Electrolyzer

Water electrolyzers can transform intermittent renewable energy like solar energy and wind energy into the chemical energy of hydrogen with zero greenhouse-gas emissions. The hydroxide-exchange membrane electrolyzer (HEME) combines the capability to produce pressurized hydrogen with the advantage of being able to use low or non-platinum group metal (PGM) electrocatalysts in the alkaline environment.1 Hydroxide salts, for example, KOH, are added to the HEME water feed on both anode and cathode to improve its performance. However, the specific mechanism of performance improvement still needs to be further understood. In addition, at high current densities, bubble evolution can result in mass-transport limitations, a less well studied phenomena. Mathematical modeling is ideal to explore these issues as it is cost and time efficient and can deconvolute the physics, processes, and observed phenomena and study the applied-voltage breakdown. In this work, we extend our previously developed 1D two-phase continuum model2 to study the varies processes in the HEME and provide insights on performance optimizations. First, the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) kinetics at different hydroxide concentrations have been studied by rotating disk electrodes (RDE) and implemented in the model. Then, the model is calibrated and validated against experimental HEME polarization curves for different KOH concentrations as a liquid electrolyte. The model clearly shows a performance increase with increasing KOH concentrations, which is consistent with the experimental results. The reduced ohmic resistance and increased electrochemical active surface area (ECSA) are the two main reasons for performance increase. The large amount of hydroxide in the liquid electrolyte not only helps to distribute the reactant hydroxide throughout the catalyst layer (CL), which reduces ohmic loss, but also enables reaction at the interface between the liquid electrolyte and electrocatalyst, which increases the ECSA. Applied-voltage breakdown demonstrates that the electrolyzer performance is dominated by anode kinetics and ohmic loss. A comparison with the DI water feed shows a more uniform current distribution in the anode CL when KOH is added, which indicates a higher utilization of the CL. Second, we present modeling on the effects of bubble coverage. As gas evolves, part of the ECSA is minimized due to bubble coverage. To account for this effect, an empirical relationship between the fractional bubble coverage and the current density is implemented in the model.3 The model shows this bubble coverage effect is more pronounced at large current densities with DI water feed. Acknowledgements This work was funded under the HydroGEN Consortium by the Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231. References R. Abbasi, B. P. Setzler, S. Lin, J. Wang, Y. Zhao, H. Xu, B. Pivovar, B. Tian, X. Chen, G. Wu and Y. Yan, 31, 1805876 (2019). L. N. Stanislaw, M. R. Gerhardt and A. Z. Weber, ECS Transactions, 92, 767 (2019). H. Vogt and R. J. Balzer, Electrochimica Acta, 50, 2073 (2005).

Liu, Jiangjin↗