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At least 73 records · Page 4

Semi-solid alkali metal electrodes enabling high critical current densities in solid electrolyte batteries

The need for higher energy density rechargeable batteries has generated interest in alkali metal electrodes paired with solid electrolytes. However, metal penetration and electrolyte fracture at low current densities have emerged as fundamental barriers. Here, we show that for pure metals in the Li-Na-K system, the critical current densities scale inversely to mechanical deformation resistance. Furthermore, we demonstrate two electrode architectures in which the presence of a liquid phase enables high current densities while preserving the shape retention and packaging advantages of solid electrodes. First, biphasic Na-K alloys show K + critical current densities (with K-β*-Al 2 O 3 electrolyte) that exceed 15 mA∙cm -2 . Second, introducing a wetting interfacial film of Na-K liquid between Li metal and Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) solid electrolyte doubles the critical current density and permits cycling at areal capacities exceeding 3.5 mAh∙cm -2 . These design approaches hold promise for overcoming electro-chemo-mechanical stability issues that have heretofore limited performance of solid-state metal batteries.

25 ENERGY STORAGE↗

Cooperative Research and Development Agreement between National Energy Technology Laboratory and The Pennsylvania State University (Final Report)

This project will use bipolar membranes to produce efficient vapor-phase electrolysis cells for splitting CO 2 to CO and oxygen. CO is a valuable chemical feedstock that can be combined catalytically with hydrogen in the Fischer-Tropsch process to make liquid fuels. CO is arguably the best target for CO 2 reduction since, as a gaseous product, it is easily collected and is relatively immune to membrane crossover losses. The keys to success in this project are to design and synthesize hydrophilic, low resistance bipolar membranes and to create optimized electrode/catalyst/electrolyte architectures based on these new membranes and advanced catalysts in order to achieve high current density at low overpotentials for CO 2 conversion. High current density is key to achieving industrially relevant throughput for the process and low overpotentials maintain high overall efficiency for the process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simultaneous access to high normalized density, current, pressure, and confinement in strongly-shaped diverted negative triangularity plasmas

Strongly-shaped diverted negative triangularity (NT) plasmas in the DIII-D tokamak demonstrate simultaneous access to high normalized density, current, pressure, and confinement. NT plasmas are shown to exist across an expansive parameter space compatible with high fusion power production, revealing surprisingly good core stability properties that compare favorably to conventional positive triangularity plasmas in DIII-D. Non-dimensionalizing the key parameters, expanded operating spaces featuring edge safety factors below 3, normalized betas above 3, Greenwald density fractions above 1, and high-confinement mode (H-mode) confinement qualities above 1 are observed, even simultaneously, and all with a robustly stable edge free from deleterious edge-localized mode instabilities. Scaling of the confinement time with engineering parameters reveals at least a linear dependence on plasma current although with significant power degradation, both in excess of expected H-mode scalings. These results increase confidence that NT plasmas are a viable approach to realize fusion power and open directions for future detailed study.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Design, construction, and testing of no-insulation small subscale solenoids for compact tokamaks

Fusion energy systems studies (FESS) for next-step devices based on the most promising magnetic configurations indicate that high magnetic fields and high current density for magnet coil systems may reduce device size and lower the cost. High current density and radiation resistant fusion magnets are particularly beneficial for low cost, low aspect ratio compact reactor designs such as Fusion Nuclear Science Facility (FNSF), Fusion Pilot Plant (FPP) of low-aspect ratio spherical tokamak (ST) or compact stellarators. Unlike typical high field magnets for nuclear magnetic resonance (NMR), magnetic resonance imaging (MRI), or high energy physics research applications, neutron irradiation damage to organic insulations in the coil winding pack is a critical issue for next generation fusion reactors where orders of magnitude higher neutron fluence than those in present experimental reactors such as ITER are expected. Moreover, a high coil winding pack current density is needed for high field magnets in low cost, compact radial build next step fusion reactors. The slow current charging time, however, is an issue in fully non-insulated coils. In this work, we present the design, construction and testing of subscale Nb3Sn solenoids, up to half the diameter of the central solenoid (CS) for National Spherical Torus Experiment (NSTX), with and without inter-layer insulation for enhancing radiation resistance while improving the winding pack current density and coil performance. The major radius for the NSTX/NSTX-Upgrade (reference for compact ST) is 0.854/0.934 meter, and 4.8 meters for FNSF. The magnetic field for NSTX/NSTX-U at the plasma center is 0.6/1 Tesla and 9 Tesla for FNSF. The inner diameter of the central solenoid coil is 0.2/0.4 meter for NSTX/NSTX-U and 1.2 meters for FNSF. The current charging and discharging behavior of the prototype solenoids was investigated to quantify performance advantages of a simplified coil fabrication without error-prone vacuum pressure impregnation (VPI) for the removal of epoxy organic insulation. Scalability of the no insulation concept for fusion can be addressed via engineered coating for novel insulation on contact resistance or intra-layer no insulations. Radiation resistance and coil winding efficiency were significantly improved in the no insulation coils for next step compact fusion reactors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enabling bifacial thin film devices by developing a back surface field using Cu x AlO y

Bifacial solar cells have the potential to increase the energy yield per unit area over traditional monofacial devices without significant added cost, driving $/kWh costs lower and accelerating the adoption of solar photovoltaics. However, the performance of bifacial thin film solar cells significantly lags that achieved by crystalline silicon cells. Here we incorporate wide bandgap Cu x AlO y as a back buffer layer for CdTe devices and achieve a backside illuminated device with high current density and high fill factor. Moreover, these values remain nearly constant even as the absorber layer thickness changes, indicating that a fully-depleted device is not required for efficient charge collection. We show that this response is indicative of a back surface field, albeit with a persistent high back surface recombination velocity. By managing electron reflection, we achieved a backside illumination conversion efficiency of 7.1% and bifaciality of 0.55 for a 3.3 µm CdTe device and 8.0% and 0.62 for a 2 µm device. Future improvements can be made by identifying and incorporating a passivation material that reduces the back surface recombination velocity.

36 MATERIALS SCIENCE↗

Visualizing degradation mechanisms in a gas-fed CO 2 reduction cell via operando X-ray tomography

We utilize operando X-ray computed tomography, coupled with real-time electrochemical analysis, to reveal the underlying failure mechanisms of membrane electrode assemblies (MEAs) for electrochemical CO 2 reduction (eCO 2 R). Through operando imaging, we can obtain unprecedented insights into the dynamic behavior of the MEA under different operating conditions, revealing critical changes in interface interactions, phase distribution, and structural integrity over time. Our findings identify phenomena giving rise to the transition from CO 2 R to the hydrogen evolution reaction (HER), as evidenced by shifts in cathode potential and CO 2 R selectivity. The formation of inhomogeneous precipitates at the gas diffusion electrode disrupts the CO 2 supply and reduces the active sites for eCO 2 R, resulting in a shift toward H2 production during low current density operation. Additionally, under high current density conditions, rapid water crossover up to the microporous layer/gas diffusion layer promotes the transition from CO 2 R to HER, further shifting cell potential toward anodic direction. Oscillating voltage conditions reveal the dissolution and regrowth of precipitates, providing direct visualization of the competing selectivity of CO 2 R and HER. This work offers new insight into the degradation mechanisms of MEAs, with implications for the design of more durable CO 2 R systems.

Lee, Sol A [California Institute of Technology (Ca↗

Failure Process During Fast Charging of Lithium Metal Batteries with Weakly Solvating Fluoroether Electrolytes

While improving the lithium metal (Li) Coulombic efficiency has been a focus for electrolyte design, the performance under high current densities is less studied yet highly relevant for practical applications. Here, we evaluate the charge-rate-dependent cycling stability using three types of weakly solvating fluoroether electrolytes. Although good cycle life was achieved in all three electrolytes under low current densities, they all exhibited a soft shorting behavior above various threshold current densities (between 2 and 5.2 mA cm –2 ). In this study, we attributed the current-dependent electrode morphology to both Li growth and residual solid electrolyte interface (rSEI) growth processes. In early cycles, Li morphology guided the formation of rSEI structures. In later cycles, the rSEI structure partially impacted Li growth. Under low current densities, the rSEI was inhomogeneous with large voids for subsequent bulky lithium growth. Under high current densities, the rSEI became more dense, which aggravated the high-surface/volume-ratio Li growth through and on the top of the rSEI. Among the three weakly solvating fluoroether electrolytes, the ones with lower ionic conductivity were observed to short within fewer cycles and at lower charge current densities. Our work suggests that fast ion transport in electrolytes may be a desirable feature for the stable operation at >1C charging in high-energy-density lithium metal batteries.

25 ENERGY STORAGE↗

High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of "dead" Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, we report a facile protection strategy for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer which is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer which prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li 2 O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi 0.6 Mn 0.2 Co 0.2 O 2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm -2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm -2 (1.5C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.

25 ENERGY STORAGE↗

Interpenetrating 3D Electrodes for High-Rate Alkaline Water Splitting

Mass transfer is critical for the reaction kinetics and efficiency of alkaline water splitting (AWS). For AWS to operate at high current densities (hundreds of mA/cm 2 ), the device architecture must ensure a large catalytic surface area, rapid ion diffusion, and minimal solution and charge transfer resistances. Effective electrodes should also facilitate gas bubble detachment and release. 3D-printed electrodes have shown promise, but stacking them increases the ion diffusion length and solution resistance. Here we demonstrate a new device architecture with interpenetrating gyroid electrodes, providing a large ion-accessible surface area and gas diffusion channels. This design significantly reduces the interelectrode distance, lowering ion diffusion length and solution resistance. Simulations show faster ion diffusion and higher current density in the interpenetrating configuration compared with separate electrodes. This improved performance, especially at low temperatures and high current densities, highlights a promising strategy for enhancing AWS and other electrochemical systems limited by slow ion diffusion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface-Treated Composite Polymer as a Stable Artificial Solid Electrolyte Interphase Layer for Lithium Metal Anodes

Lithium (Li) metal batteries (LMBs) are one of the most promising high energy density batteries to meet the demands of electric transportation. However, the practical applications of LMBs are hindered by short cycle life and safety concern, mainly associated with side reactions between Li metal anode and liquid electrolyte and the growth of Li dendrites during cycling. In this study, we develop a stable artificial solid electrolyte interphase (aSEI), which consists of a surface-treated (S T ) PEO–Li 6.4 Ga 0.2 La 3 Zr 2 O 12 composite polymer coating layer (CPL) on Li metal anode. The developed aSEI is stable against selected electrolyte and enables a uniform electrodeposition of Li. Therefore, S T CPL@Li||LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cells exhibit improved cycling stability compared with bare Li||NMC811 cells at moderate to high current densities. Notably, using a 50 µm thick Li and a practical NMC811 cathode (~4.8 mAh cm -2 ), a capacity retention of 85% is obtained for S T CPL@Li||NMC811 cells at a current density of 2.4 mAcm -2 after 300 cycles compared with 24% for bare Li||NMC811 cells. Furthermore, S T CPL@Li||NMC811 cells demonstrate higher capacities at charge current densities of 2.4, 4.8 and 7.2 mAcm -2 compared with bare Li||NMC811 cells. Further, these findings suggest that S T CPL is promising for high current density practical LMBs.

25 ENERGY STORAGE↗

High-Power Lithium Metal Batteries Enabled by High-Concentration Acetonitrile-Based Electrolytes with Vinylene Carbonate Additive

To enable next-generation high power, high-energy-density lithium (Li) metal batteries (LMBs), an electrolyte possessing both high Li Coulombic efficiency (CE) at high-rate and good anodic stability on cathodes is critical. Acetonitrile (AN) is a well-known organic solvent for high anodic stability and high ionic conductivity, yet its application in LMBs is limited due to its poor compatibility with Li metal anode even at high salt concentration conditions. Here, we developed a highly concentrated AN-based electrolyte with vinylene carbonate (VC) additive to suppress Li+ depletion at high current densities. Addition of VC in the AN-based electrolyte leads to the formation of a polycarbonate-based solid electrolyte interphase which minimizes Li corrosion and leads to very high Li CE of up to 99.1% at a current density of 0.2 mA cm-2. Using such an electrolyte, fast charging of Li||NMC333 cells has been realized at a high current density of 3.6 mA cm-2, and stable cycling of Li||NMC622 cells with a high cathode loading of 4 mAh cm-2 has also been demonstrated.

Peng, Zhe↗

Theoretical Analysis of Critical Conditions for Crack Formation and Propagation, and Optimal Operation of SOECs

A theoretical analysis on crack formation and propagation was performed based on the coupling between the electrochemical process, classical elasticity, and fracture mechanics. The chemical potential of oxygen, thus oxygen partial pressure, at the oxygen electrode-electrolyte interface ( μ O 2 OE∣El ) was investigated as a function of transport properties, electrolyte thickness and operating conditions (e.g., steam concentration, constant current, and constant voltage). Our analysis shows that: a lower ionic area specific resistance (ASR), r i O E , and a higher electronic ASR ( r e O E ) of the oxygen electrode/electrolyte interface are in favor of suppressing crack formation. The μ O 2 O E ∣ E l , thus local pO 2 , are sensitive towards the operating parameters under galvanostatic or potentiostatic electrolysis. Constant current density electrolysis provides better robustness, especially at a high current density with a high steam content. While constant voltage electrolysis leads to greater variations of μ O 2 O E ∣ E l . Constant current electrolysis, however, is not suitable for an unstable oxygen electrode because μ O 2 O E ∣ E l can reach a very high value with a gradually increased r i O E . A crack may only occur under certain conditions when p O 2 T P B > p c r .

42 ENGINEERING↗

Effect of Electro-Sprayed Porous Electrodes on the Performance and Stability of Water Electrolysis

The efficiency of proton exchange membrane water electrolysis (PEMWE) is a critical issue in realizing the production of green hydrogen. Here, the coexistence of three phases in the catalyst layer of PEMWE causes the mass transport limitation at the interfaces between them. In particular, the vigorous production of gaseous hydrogen and oxygen derived from liquid water is generated in the form of bubbles that seriously deactivate the membrane-electrode assembly (MEA). In this study, we investigated the effect of porous structure in the electrode on the efficiency of hydrogen production at high current density, which is highly related to the mass transport limitation. A widely used commercial catalyst (IrO 2 ) were directly coated on the membrane by the electro-spray method. The porous electrodes on the membrane were formed by the charged catalyst particles that repulsed each other due to the electrostatic forces of the particles. Our membrane electrode assembly (MEA) exhibited outstanding electrolysis performances such as 5.3 A cm -2 and 3.2 A cm -2 at 2.0 V and 1.8 V, respectively, which are the highest values compared with the results published in the current studies. In addition to the porosity, it was confirmed that optimum binder contents positively affect the hydrophobicity and contact resistance of MEA. Through a simple porosity-controlled technique, the performance of PEMWE, in which three phases coexist, can be improved by more than 60 %. Accordingly, we expect that our systematic study on the role of porosity in the electrodes opens a new era to efficiently produce green hydrogen.

catalysts↗

A Flexible, Redox-Active, Aqueous Electrolyte-Based Asymmetric Supercapacitor with High Energy Density Based on Keratin-Derived Renewable Carbon

This work exploits the advantage of asymmetric configuration over symmetric supercapacitor in designing high energy density flexible devices from two active electrode materials–keratin-based renewable-resource hierarchically porous carbon and hydrous ruthenium oxide (RuO 2 ). Here, the asymmetric device exhibits significantly high capacitance. Conventional estimation of energy storage parameters, however, cannot be applied for devices with a Faradaic energy storage contribution via redox charge transfer mechanism. Therefore, this work applies a precise measurement of pseudocapacitance contribution at various scan rates to correct the device data that reveals effective capacitance of 120 F g –1 with the energy density of 37 W h kg –1 at 776 W kg –1 . It also retains excellent rate capability, >74% at high current density 25 A g –1 . The charge storage activity and device stability can be further enhanced by introducing redox-active electrolytes that improve specific capacitance, but the rate capabilities deteriorate at high current densities. Further, the principle of asymmetric electrode design is applied to fabricate a bending-tolerant, flexible device by depositing active electrode material on wire-shaped current collector followed by coupling those separated with polyvinyl alcohol gel containing redox electrolyte; it yields 36.8 mF cm –1 specific capacitance at a 0.2 mA cm –1 current density.

36 MATERIALS SCIENCE↗

A New Class of Proton Conductors with Dramatically Enhanced Stability and High Conductivity for Reversible Solid Oxide Cells

Reversible solid oxide cells based on proton conductors (P-ReSOCs) have potential to be the most efficient and low-cost option for large-scale energy storage and power generation, holding promise as an enabler for the implementation of intermittent renewable energy technologies and the widespread utilization of hydrogen. Here, the rational design of a new class of hexavalent Mo/W-doped proton-conducting electrolytes with excellent durability while maintaining high conductivity is reported. Specifically, BaMo(W) 0.03 Ce 0.71 Yb 0.26 O 3-δ exhibits dramatically enhanced chemical stability against high concentrations of steam and carbon dioxide than the state-of-the-art electrolyte materials while retaining similar ionic conductivity. In addition, P-ReSOCs based on BaW 0.03 Ce 0.71 Yb 0.26 O 3-δ demonstrate high peak power densities of 1.54, 1.03, 0.72, and 0.48 W cm –2 at 650, 600, 550, and 500 °C, respectively, in the fuel cell mode. During steam electrolysis, a high current density of 2.28 A cm –2 is achieved at a cell voltage of 1.3 V at 600 °C, and the electrolysis cell can operate stably with no noticeable degradation when exposed to high humidity of 30% H 2 O at –0.5 A cm –2 and 600 °C for over 300 h. Altogether, this work demonstrates the promise of donor doping for obtaining proton conductors with both high conductivity and chemical stability for P-ReSOCs.

25 ENERGY STORAGE↗

Design and Prototyping of a Novel Toroidal Magnet System for MOLLER Experiment at Jefferson Lab

The Thomas Jefferson National Accelerator Facility (JLab) has designed a unique spectrometer system to measure the weak interaction between electrons. The experiment— Measurement of Lepton-Lepton Electroweak Reaction (MOLLER)—requires leveraging the recent 12 GeV electron beam upgrade and will run in JLab for three years. Focusing the signal for the MOLLER experiment requires five water-cooled toroidal magnets, each with unique geometry and with 7-fold symmetry. The five magnets operate in a vacuum and provide the magnetic field required to separate the incident beam electrons scattered from the target electrons (Møller scattering) and protons (elastic e-p scattering) in a liquid hydrogen target. The conceptual design was developed by the MOLLER Collaboration and was given to JLab in the form of amp turns and physical location, with additional physics requirements. This article presents prototyping of the coils and magnet support system and discusses the lessons learned during the process along with the plans for full magnet testing and installation. The JLab Magnet Group along with the MOLLER Collaboration developed the specification document that includes keep out zones to design the set of magnets. JLab contracted the design of the first toroid magnet (TM0) of the magnet system to Massachusetts Institute of Technology. The other four toroid magnets (TM1 through TM4) have been designed by JLab and are in the process of fabrication and assembly. Prototype coils of TM1-TM4 were fabricated by Everson-Tesla Incorporated, PA (USA). Finally, this article presents the unique challenges of the design, alignment, high current density, operating range, high radiation dose, and vacuum environment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Design and Prototyping of a Novel Toroid Magnet System for the MOLLER Experiment at Jefferson Lab

The Thomas Jefferson National Accelerator Facility (JLab) has designed a unique spectrometer system to measure the weak interaction between electrons. The experiment ?Measurement of Lepton-Lepton Electroweak Reaction? (MOLLER) requires leveraging the recent 12 GeV electron beam upgrade and will run in JLab for 3 years. Focusing the signal for the MOLLER experiment requires five water-cooled toroidal magnets, each with unique geometry and with 7-fold symmetry. This system of magnets provides the magnetic field required to separate the incident beam electrons scattered from the target electrons (Møller scattering) and protons (elastic e-p scattering) in a liquid hydrogen target. The conceptual design was developed by the MOLLER collaboration and was given to JLab in the form of amp turns and physical location, with additional physics requirements. This paper presents prototyping of the coils and magnet support system and discusses the lessons learned during the process along with the plans for full magnet testing and installation. The JLab Magnet Group along with the MOLLER collaboration developed the specification document that includes keep out zones to design the set of magnets. JLab contracted the design of the first toroid magnet in the magnet (TM0) to Massachusetts Institute of Technology. The other four toroid magnets (TM1 through TM4) have been designed by JLab and are in the process of fabrication and assembly. Prototype coils of TM1-TM4 have been fabricated by Everson-Tesla Incorporated, PA (USA). The manuscript presents the unique challenges of the design, alignment, high current density, operating range, high radiation dose, and vacuum environment.

Kashy, David↗

Conceptual Design of High Field Central Solenoid for Fusion Nuclear Science Facility

Fusion Nuclear Science Facility (FNSF) is a critical fusion nuclear step in the US beyond ITER before proceeding to a larger and electricity producing fusion power plant. Although FNSF is a steady state machine to be operated at high duty cycle, a high field and high current density central solenoid magnet is needed for plasma startups. Due to space constraints in the FNSF in-board radial build, the magnetic field and coil current density required exceed conventional low temperature superconductor (LTS) performance limits and the design can only be achieved by high temperature superconductors (HTS). The design for the central solenoid, also called the ohmic heating (OH) magnet for FNSF shall meet the 100 Weber double flux swing requirement for plasma startups. Finally, the stresses at such a high field and high current density coil may require a bucked and wedged TF-OH design to accommodate space for coil winding support structures in in-board system radial build for high field FNSF operations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗