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DOE OSTI2023

Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

Abstract The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high‐energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as‐induced dual‐gradient solid‐electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm −2 . Moreover, X‐ray photoelectron spectroscopy and synchrotron X‐ray experiments revealed that N‐rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high‐energy cathode materials including LiNi 0.7 Mn 0.2 Co 0.1 O 2 , Li 1.2 Co 0.1 Mn 0.55 Ni 0.15 O 2 , and sulfur demonstrate significantly improved cycling stability with high cathode loading.

Xie, Chuyi↗

DOE OSTI2023

Suppressing Universal Cathode Crossover in High‐Energy Lithium Metal Batteries via a Versatile Interlayer Design**

25 ENERGY STORAGE↗

DOE OSTI2020

Dendrite Suppression by a Polymer Coating: A Coarse‐Grained Molecular Study

Abstract A major hurdle to the successful deployment of high‐energy‐density lithium metal based batteries is dendrite growth during battery cycling, which raises safety and cycle life concerns. Coating the Li metal anode with a soft polymer layer has been previously shown to be effective in suppressing dendrite growth, leading to uniform lithium deposition even at high current densities. A 3D coarse‐grained molecular model to study the mechanism of dendrite suppression is presented. It is found that the most effective coatings delay or even prevent dendrites from penetrating the polymer layer during deposition. The optimal deposition can be achieved by jointly tuning the polymer stiffness and relaxation time. Higher polymer dielectric permittivity and coating thickness are also effective, but the deposition rate and, therefore, the charging current density is reduced. These findings provide the basis for rational design of soft polymer coatings for stable lithium deposition.

Kong, Xian↗

NASA NTRS1987

Electric fields and double layers in plasmas

Various mechanisms for driving double layers in plasmas are briefly described, including applied potential drops, currents, contact potentials, and plasma expansions. Some dynamical features of the double layers are discussed. These features, as seen in simulations, laboratory experiments, and theory, indicate that double layers and the currents through them undergo slow oscillations which are determined by the ion transit time across an effective length of the system in which double layers form. It is shown that a localized potential dip forms at the low potential end of a double layer, which interrupts the electron current through it according to the Langmuir criterion, whenever the ion flux into the double is disrupted. The generation of electric fields perpendicular to the ambient magnetic field by contact potentials is also discussed. Two different situations were considered; in one, a low-density hot plasma is sandwiched between high-density cold plasmas, while in the other a high-density current sheet permeates a low-density background plasma. Perpendicular electric fields develop near the contact surfaces. In the case of the current sheet, the creation of parallel electric fields and the formation of double layers are also discussed when the current sheet thickness is varied. Finally, the generation of electric fields and double layers in an expanding plasma is discussed.

Singh, Nagendra↗

DOE OSTI2024

Pilot microbial electrolysis cell closes the hydrogen loop for hydrothermal wet waste conversion to jet fuel

The global shift toward net-zero emissions necessitates resource recovery from wet waste. In this study, we demonstrate the first feasibility of combining pilot-scale microbial electrolytic cells (MECs) with hydrothermal liquefaction (HTL) for simultaneous post-hydrothermal liquefaction wastewater (PHW) treatment and efficient hydrogen (H₂) production to meet biocrude upgrading requirements. Long-term single reactor operation revealed that fixed anode potential enabled rapid startup, and low catholyte pH and high salinity were effective in suppression of cathodic methanogenesis and acetogenesis – resulting in high current density of 16.6 A m –2 and 9.3 A m –2 when feeding synthetic wastewater and PHW respectively. Additionally, the anode biofilm exhibited spatial variations in response to local environmental conditions. In conclusion, onsite parallel or serial operations of multiple MECs showed good performance using actual PHW with a record-high H 2 production rate of 0.5 L L R day –1 for MEC over 10 liters scale, and the optimal chemical oxygen demand (COD)-to-H 2 yield reached 0.127 kg-H 2 per kg-COD, supporting a self-sufficient, closed-loop upgrade to jet fuel.

08 HYDROGEN↗

DOE OSTI2022

New Approaches to Improved PEM Fuel Cell Catalyst Layers

Polymer-electrolyte membrane (PEM) fuel-cells are one of the most promising energy conversion technologies for renewable clean energy applications. A major challenge preventing the widespread use and commercialization of PEM fuel cells is achieving high performance with low-loadings of platinum group metal (PGM) catalysts. One of the factors driving performance limitations in the cell is the mass transport losses within the cathode catalyst layers (CCL) due to sluggish oxygen-reduction reactions occurring at the platinum-ionomer interface. Any resistance to transport of these ionic and gaseous species within the CCL results in mass-transport limitations and performance losses, especially at high current densities. It is known that mass-transport losses increase with reduced platinum loading, thereby creating a performance-cost tradeoff for fuel cells. A viable solution to reduce the transport resistances in the catalyst layers is to create new ionomers that can provide good ion and oxygen transport needed to accomplish high-performing fuel cell catalysts. Using this approach Tetramer Technologies and LBNL propose improved fuel-cell catalyst ionomers based on Tetramers proprietary polymer chemistry.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2022

Room-Temperature Pseudo-Solid-State Iron Fluoride Conversion Battery with High Ionic Conductivity

Li-metal batteries (LMBs) employing conversion cathode materials (e.g., FeF 3 ) are a promising way to prepare inexpensive, environmentally friendly batteries with high energy density. Pseudo-solid-state ionogel separators harness the energy density and safety advantages of solid-state LMBs, while alleviating key drawbacks (e.g., poor ionic conductivity and high interfacial resistance). In this work, a pseudo-solid-state conversion battery (Li-FeF 3 ) is presented that achieves stable, high rate (1.0 mA cm –2 ) cycling at room temperature. The batteries described herein contain gel-infiltrated FeF 3 cathodes prepared by exchanging the ionic liquid in a polymer ionogel with a localized high-concentration electrolyte (LHCE). The LHCE gel merges the benefits of a flexible separator (e.g., adaptation to conversion-related volume changes) with the excellent chemical stability and high ionic conductivity (~2 mS cm –1 at 25 °C) of an LHCE. The latter property is in contrast to previous solid-state iron fluoride batteries, where poor ionic conductivities necessitated elevated temperatures to realize practical power levels. Importantly, the stable, room-temperature Li-FeF 3 cycling performance obtained with the LHCE gel at high current densities paves the way for exploring a range of architectures including flexible, three-dimensional, and custom shape batteries.

25 ENERGY STORAGE↗

DOE OSTI2020

Operando Tailoring of Defects and Strains in Corrugated β-Ni(OH) 2 Nanosheets for Stable and High-Rate Energy Storage

Nickel hydroxide represents a technologically important material for energy storage, such as hybrid supercapacitors. It has two different crystallographic polymorphs, α- and β-Ni(OH) 2 , showing advantages in either theoretical capacity or cycling/rate performance, manifesting a trade-off trend that needs to be optimized for practical applications. In this work, the synergistic superiorities in both activity and stability of corrugated β-Ni(OH) 2 nanosheets are demonstrated through an electrochemical abuse approach. With ≈91% capacity retention after 10 000 cycles, the corrugated β-Ni(OH) 2 nanosheets can deliver a gravimetric capacity of 457 C g -1 at a high current density of 30 A g -1 , which is nearly two and four times that of the regular α- and β-Ni(OH) 2 , respectively. Operando spectroscopy and finite element analysis reveal that greatly enhanced chemical activity and structural robustness can be attributed to the in situ tailored lattice defects and the strain-induced highly curved micromorphology. This work demonstrates a multi-scale defect-and-strain co-design strategy, which is helpful for rational design and tuned fabrication of next-generation electrode materials for stable and high-rate energy storage.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Strong Coupling of Iridium and Boron–Carbon-Nitride Support for Enhanced Acidic Water Oxidation

Supporting iridium (Ir)-based materials on stable and suitable substrates is an efficient strategy to improve their catalytic performance for the oxygen evolution reaction (OER) in harsh acidic environments. Herein, we report a series of Ir catalysts supported on boron–carbon-nitride (BCN), denoted as Ir/BCN. Detailed experiments combined with density functional theory calculations demonstrate strong interactions between Ir nanoparticles (NPs) and the BCN support, significantly contributing to the improved OER performance. Among the synthesized catalysts, the Ir/BCN-75 catalyst outperforms commercial Ir black and IrO 2 in both half-cell and proton exchange membrane water electrolysis (PEMWE) tests. Specially, the Ir/BCN-75 catalyst achieves a high current density of 2.94 A cm –2 at 1.9 V with a low Ir loading of 0.26 mg cm –2 in PEMWE measurements, exceeding most Ir-based catalysts reported to date. The BCN support interacts strongly with Ir, wherein Ir–N bonding directs the Ir NP growth and enhances electrocatalytic activity, while Ir–B bonding contributes to the stability of the Ir/BCN catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

In Situ Characterization of Interface Evolution in Argyrodite‐Based All‐Solid‐State Li Batteries

Interfacial stability is one of the critical challenges in all-solid-state Li metal batteries. Multiple processes such as solid electrolyte (SE) decomposition and lithium dendrite growth take place at the solid interfaces during cycling, leading to the overall cell failure. To deconvolute these complex processes, in situ characterization is of paramount importance to elucidate the interfacial evolution on the SE upon Li plating/stripping. Herein, an all-solid-state asymmetric in situ cell is developed that allows the direct visualization of the highly localized Li plating/stripping processes under the optical microscope. Moreover, this cell configuration enables reliable post-mortem chemical and morphological analysis of the intact SE/Li interface. Using combined scanning electron microscopy and energy-dispersive X-ray spectroscopy, the study reveals that the evolution of the Li argyrodite interface is strongly influenced by the current density, particularly in terms of chemical distribution and Li plating morphology. More specifically, the solid interface is LiCl-rich with the formation of Li cubes at low current densities, while high currents result in more uniform elemental distribution and filament morphology. These findings elucidate the dynamic evolution mechanism at solid interfaces and offer valuable guidance for developing stable solid interfaces in all-solid-state Li metal batteries.

Huang, Di↗

DOE OSTI2023

Numerical investigation and experimental validation of water condensation in the gas diffusion layer with different properties

Liquid water in porous media hinders the transport of reactant to catalyst layer, where the electrochemical reactions occur, which in turn, reduces performance and lifetime of a proton exchange membrane fuel cell (PEMFC). In this study, two types of gas diffusion layer (GDL) materials are used to study the two-phase saturation distribution in a PEMFC. The correlations between the effective and anisotropic transport properties and porosity of the two GDLs are solved by the pore scale model. In addition, the anisotropic liquid water permeability and the relationship between saturation pressure and capillary pressure is determined by using the Lattice-Boltzmann method. Fuel cell performance as well as liquid water distribution in the GDL using neutron radiography are obtained for validation. Under wet conditions, the cell with Freudenberg GDL performs better than that using Toray GDL, especially at high current densities. The results of the two-phase model simulation show that the peak water saturation for Toray GDL occurs in the catalyst layer and can reach 40%, while the peak water saturation for Freudenberg GDL occurs inside the GDL directly under the ribs and only reaches 25% saturation. The combined results provide key insights to enable high power density operation of a PEMFC through GDL material optimization.

42 ENGINEERING↗

DOE OSTI2019

Reverse Heterojunction (Al)GaInP Solar Cells for Improved Efficiency at Concentration

Mitigating series resistance is crucial to the efficiency of concentrator solar cells at high current density. Conventional AlGaInP junction designs for the top junction of III-V multijunction cells present a challenging tradeoff between series resistance on the one hand and current collection and voltage on the other hand. In this article we discuss the physics of a reverse heterojunction solar cell that aims to improve on this tradeoff by combining a high bandgap Al 0.18 Ga 0.33 In 0.49 P base and a lower bandgap (Al)GaInP emitter. The high mobility of the emitter leads to a relatively low series resistance, compared with a high bandgap homojunction cell. Furthermore, the electroluminescence spectrum shows emission peaks from both the emitter and base, leading to an open-circuit voltage that is not strictly dominated by either layer. The reverse heterojunction design is increasingly beneficial as the one-sun voltage increases.

14 SOLAR ENERGY↗

NASA NTRS1984

Test bed ion engine development

A test bed ion (TBI) engine was developed to serve as a tool in exploring the limits of electrostatic ion thruster performance. A description of three key ion engine components, the decoupled extraction and amplified current (DE-AC) accelerator system, field enhanced refractory metal (FERM) hollow cathode and divergent line cusp (DLC) discharge chamber, whose designs and operating philosophies differ markedly from conventional thruster technology is given. Significant program achievements were: (1) high current density DE-AC accelerator system operation at low electric field stress with indicated feasibility of a 60 mA/sq cm argon ion beam; (2) reliable FERM cathode start up times of 1 to 2 secs. and demonstrated 35 ampere emission levels; (3) DLC discharge chamber plasma potentials negative of anode potential; and (4) identification of an efficient high plasma density engine operating mode. Using the performance projections of this program and reasonable estimates of other parameter values, a 1.0 Newton thrust ion engine is identified as a realizable technology goal. Calculations show that such an engine, comparable in beam area to a J series 30 cm thruster, could, operating on Xe or Hg, have thruster efficiencies as high as 0.76 and 0.78 respectively, with a 100 eV/ion discharge loss.

Aston, G.↗

DOE OSTI2023

High-performance Ruddlesden–Popper perovskite oxide with in situ exsolved nanoparticles for direct CO 2 electrolysis

Carbon dioxide (CO 2 ) is one of the principal greenhouse gases accountable for global warming and extreme climate changes. Electrochemically converting CO 2 into carbon monoxide (CO) is a promising approach for CO 2 utilization in achieving industrial decarbonization. High-temperature CO 2 electrolysis via solid oxide electrolysis cells (SOECs) has great potential, including high-energy efficiency, fast electrode kinetics, and competitive cost; however, this technology still has challenges associated with developing highly active, robust CO 2 electrodes for SOECs. We report novel Ruddlesden–Popper structured Pr 1.2 Sr 0.8 Mn 0.4 Fe 0.6 O 4–δ (RP-PSMF) with in situ exsolved Fe nanoparticles as the CO 2 electrode in SOECs for direct CO 2 conversion to CO. The mechanism of CO 2 electrolysis is studied by using the distribution of relaxation times method from electrochemical impedance spectroscopy. La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3–δ (LSGM)-electrolyte supported SOECs with the RP-PSMF cathode have achieved exceptionally high current densities of 2.90, 1.61, 0.91, and 0.48 A·cm –2 at an applied voltage of 1.5 V at 800, 750, 700, and 650 °C, respectively. Moreover, SOECs with the RP-PSMF cathode have exhibited a stable electrolysis performance for 100 h under a current cycling operation. Here, these results suggest that RP-PSMF with exsolved Fe nanoparticles is a highly promising cathode for high-temperature direct CO 2 electrolysis cells.

03 NATURAL GAS↗

DOE OSTI2020

Electrocatalytic CO 2 Reduction to Fuels: Progress and Opportunities

The electrochemical reduction of CO 2 continues to be an appealing option for storing renewable energy in a chemical form. In this review, we assess progress in designing catalysts that convert CO 2 to high energy density products. We explain how reaction data can be reported to reflect the intrinsic properties of the catalyst. This analysis shows that limited advances have been made in improving the performance of Cu. We suggest that opportunities remain using bimetallic catalysts that are resistant to dealloying. While aqueous systems are instrumental to developing our understanding of this chemistry, gas-fed systems that operate at high current densities must be developed. Although obstacles remain for practical application of CO 2 reduction, advances in fundamental understanding made over the years give reason for optimism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Ultrafast Preparation of Nonequilibrium FeNi Spinels by Magnetic Induction Heating for Unprecedented Oxygen Evolution Electrocatalysis

Carbon-supported nanocomposites are attracting particular attention as high-performance, low-cost electrocatalysts for electrochemical water splitting. These are mostly prepared by pyrolysis and hydrothermal procedures that are time-consuming (from hours to days) and typically difficult to produce a nonequilibrium phase. Herein, for the first time ever, we exploit magnetic induction heating-quenching for ultrafast production of carbon-FeNi spinel oxide nanocomposites (within seconds), which exhibit an unprecedentedly high performance towards oxygen evolution reaction (OER), with an ultralow overpotential of only +260 mV to reach the high current density of 100 mA cm -2 . Experimental and theoretical studies show that the rapid heating and quenching process (ca. 10 3 K s -1 ) impedes the Ni and Fe phase segregation and produces a Cl-rich surface, both contributing to the remarkable catalytic activity. Results from this study highlight the unique advantage of ultrafast heating/quenching in the structural engineering of functional nanocomposites to achieve high electrocatalytic performance towards important electrochemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1990

Magnetic heating of stellar chromospheres and coronae

The theoretical discussion of magnetic heating focuses on heating by dissipation of field-aligned electric currents. Several mechanisms are set forth to account for the very high current densities needed to generate the heat, but observed radiative losses do not justify the resultant Ohmic heating rate. Tearing modes, 'turbulent resistivity', and 'hyper-resistivity' are considered to resolve the implied inefficiency of coronal heating. Because the mechanisms are not readily applicable to the sun, transverse magnetic energy flows and magnetic flare release are considered to account for the magnitude of observed radiative loss. High-resolution observations of the sun are concluded to be an efficient way to examine the issues of magnetic heating in spite of the very small spatial scales of the heating processes.

Van Ballegooijen, A. A.↗

DOE OSTI2024

Design and Synthesis of PtPdNiCoMn High‐Entropy Alloy Electrocatalyst for Enhanced Alkaline Hydrogen Evolution Reaction: A Theoretically Supported Predictive Design Approach

Electrocatalytic hydrogen generation requires a multifunctional electrocatalyst with abundant active sites to drive multielectron transfer reactions. High entropy alloys (HEA) are five or more-elements with high configurational entropy are considered unique materials for next-generation electrocatalysts. Here, in this work, based on new screening guidelines for catalyst selections that combine density-functional theory calculated Gibbs formation-enthalpy with bond length and electronegativity variance, a novel HEA electrocatalyst consisting of five elements, namely, Pt, Pd, Ni, Co, and Mn has been designed. By simple room temperature electrodeposition, the designed catalyst is prepared and its hydrogen evolution reaction (HER) is explored and validated through experimental and theoretical approaches. The HEA demonstrated a superior HER activity with an overpotential of 22.6 mV at -10 mA cm -2 which outperforms Pt/C commercial catalyst. No evident degradation of the material is detected even after 100 hours of continuous operation under high current density. Moreover, the HEA has shown exceptional performance in harsh electrolyte conditions such as in simulated seawater and actual seawater. Remarkably, the density-functional theory calculated Gibbs formation-enthalpy is small (≈0 eV) compared to Pt/C placing the new HEA near the apex of Trasatti's model of Volcano plot, which is also suggestive of superior HER activity.

36 MATERIALS SCIENCE↗