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DOE OSTI2023

Highly durable fuel cell electrocatalyst with low-loading Pt-Co nanoparticles dispersed over single-atom Pt-Co-N-Graphene nanofiber

The limited durability of Pt electrocatalysis toward cathodic oxygen reduction reaction remains challenging, yet crucial for the development of Proton Exchange Membrane Fuel Cell. Here, we present a rational design of a robust catalyst consisting of PtCo nanoparticles supported on Pt-Co-N-graphene nanofiber prepared through electrospun Cobalt-Metal-Organic-Framework. The catalyst delivers unprecedented mass activity of 2.48 A·mgPt -1 , and retains 80% of initial value after 60,000 Accelerated-Stress-Test cycles. Operando X-ray absorption spectroscopies show that the electronic configurations of Pt sites in PtCo and Co sites in Co-N4 in the hybrid catalyst are modified toward high catalytic activities. Density Functional Theory unveils that the enhanced curvature of the substrate induced by the morphology engineering lowers the reaction thermodynamic barrier on Co-N4 sites, favoring the formation of H2O and suppressing that of H2O2. This result along with the strong affinity of PtCo nanoparticles to the Pt-Co-N-graphene fiber endows the catalyst an exceptional durability.

acidic electrolyte↗

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 OSTI2020

Self-supported MoO 2 /MoS 2 nano-sheets embedded in a carbon cloth as a binder-free substrate for high-energy lithium–sulfur batteries

As one of the most prospective candidates for next-generation rechargeable batteries, lithium-sulfur (Li-S) batteries currently still encounter great challenges associated with the low conductivity, severe shuttle effects, and sluggish redox kinetics. Herein, a self-supported sulfur host is fabricated by an in-situ growth of MoO 2 /MoS 2 nano-sheets on a carbon cloth (CC). First, carbon cloth serves as a good template for the morphology-controlled synthesis of nanostructured materials, which not only alleviates the agglomeration of MoO2/MoS2, but also enhances the flexibility and mechanical strengthen of the hybrid architecture as a free-standing host. Second, the polysulfide-trapping ability can be greatly enhanced by both physical and chemical adsorption from the MoO 2 /MoS 2 -anchored carbon cloth. Moreover, the partially sulfurized MoO 2 /MoS 2 nano-sheets integrate the benefits of conductive MoO 2 and sulfiphilic MoS 2 , thus facilitating fast charge transfer and redox kinetics of polysulfide conversion. As a result, these attributes enable the host to hold a high sulfur loading (up to 7.6 mg cm -2 ), which exceeds most of the reported carbon cloth-related cathode work in the literature. Furthermore, the Li-S cells can achieve a high peak capacity of 1350 mA h g -1 , excellent rate capability (C/20 - 2C rate), impressive areal capacity (up to 6.3 mA h cm -2 ), and a high capacity retention of 85% after 100 cycles.

25 ENERGY STORAGE↗

DOE OSTI2022

Carbon-Binder Weight Loading Optimization for Improved Lithium-Ion Battery Rate Capability

Battery performance is strongly correlated with electrode microstructure and weight loading of the electrode components. Among them are the carbon-black and binder additives that enhance effective conductivity and provide mechanical integrity. However, these both reduce effective ionic transport in the electrolyte phase and reduce energy density. Therefore, an optimal additive loading is required to maximize performance, especially for fast charging where ionic transport is essential. Such optimization analysis is however challenging due to the nanoscale imaging limitations that prevent characterizing this additive phase and thus quantifying its impact on performance. Herein, an additive-phase generation algorithm has been developed to remedy this limitation and identify percolation threshold used to define a minimal additive loading. Improved ionic transport coefficients from reducing additive loading has been then quantified through homogenization calculation, macroscale model fitting, and experimental symmetric cell measurement, with good agreement between the methods. Rate capability test demonstrates capacity improvement at fast charge at the beginning of life, from 37% to 55%, respectively for high and low additive loading during 6C CC charging, in agreement with macroscale model, and attributed to a combination of lower cathode impedance, reduced electrode tortuosity and cathode thickness.

25 ENERGY STORAGE↗

DOE OSTI2024

Shape Matters: Understanding the Effect of Electrode Geometry on Cell Resistance and Chemo-Mechanical Stress

Rechargeable batteries that incorporate shaped three-dimensional electrodes have been shown to have increased power and energy densities when compared to a conventional geometry, i.e. a planar cathode and anode that sandwich an electrolyte. Electrodes can be shaped to enable a higher active material loading, while keeping ion transport distances small. However, the relationship between electrical and mechanical performance of shaped electrodes remains poorly understood. Many electrode designs have been explored, where the electrodes are individually shaped or intertwined, and advances in manufacturing and shape/topology optimization have made such designs a reality. Here, we explore sinusoidal half cells and interdigitated full cells. First, we use a simple electrostatics model to understand the cell resistance as a function of shape. Here we focus on low-temperature conditions, where the electrolyte conductivity decreases relative to that of the electrode; here, LiPF 6 EC:DMC electrolyte and MnO 2 electrode are considered. Next, we use a chemo-mechanics model to examine the stress that arises due to intercalation-driven volume expansion. We show that shaped electrodes provide a significant reduction in resistance in low-temperature conditions, however, they exhibit unfavorable stress concentrations. Overall, we find that the fully interdigitated electrodes may provide the best balance with respect to this resistance-stress trade-off.

25 ENERGY STORAGE↗

DOE OSTI2024

Carbon-Binder Optimization for Lithium-Ion Battery Extreme Fast Charge

carbon-binder additives↗

DOE OSTI2023

Performance of Polymer Electrolyte Membrane Water Electrolysis Systems: Configuration, Stack Materials, Turndown and Efficiency

A cell model is developed and validated to analyze the performance of polymer electrolyte membrane water electrolysis (PEMWE) stacks and systems. It is used to characterize the oxygen evolution reaction (OER) activity on a TiO2-supported IrO2 catalyst and an unsupported IrO2 powder catalyst. Electrochemical, stack, and system thermoneutral potentials are defined and determined for isothermal and non-isothermal stack operation. Conditions are determined under which the system thermoneutral potential or flammability of H2 in the O2 anode stream limits the stack turndown and operating temperature. Performance is analyzed of a complete PEMWE system with an electrolyzer stack containing an IrO2/TiO2 anode catalyst (2 mg/cm2 Ir loading) and N117-like membrane mitigated for H2 crossover, anode balance-of-plant (BOP) components, cathode BOP system with temperature swing adsorption for H2 purification, and electrical BOP system with transformer and rectifier. At the rated power condition, defined as 2 A/cm2 at 1.9 V, 80 °C, and 30 bar H2 pressure, the stack/system efficiency is 65.3%/60.3% at beginning of life (BOL), decreasing to 59.3%/53.9% at end of life (EOL). The peak stack/system efficiency is 76.3%/70.2% at BOL, decreasing to 71.2%/65.6% at EOL. Improvements in catalyst activity and membrane are identified for a 50% increase in current to 3 A/cm2 at 1.8 V.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Contribution of the backstreaming ions to the self-magnetic pinch (SMP) diode current

The results presented here were obtained with a self-magnetic pinch (SMP) diode mounted at the front high voltage end of the RITS accelerator. RITS is a Self-Magnetically Insulated Transmission Line (MITL) voltage adder that adds the voltage pulse of six 1.3 MV inductively insulated cavities. The RITS driver together with the SMP diode has produced x-ray spots of the order of 1 mm in diameter and doses adequate for the radiographic imaging of high area density objects. Although, through the years, a number of different types of radiographic electron diodes have been utilized with SABER, HERMES III and RITS accelerators, the SMP diode appears to be the most successful and simplest diode for the radiographic investigation of various objects. Our experiments had two objectives: first to measure the contribution of the back-streaming ion currents emitted from the anode target and second to try to evaluate the energy of those ions and hence the Anode-Cathode (A-K) gap actual voltage. In any very high voltage inductive voltage adder utilizing MITLs to transmit the power to the diode load, the precise knowledge of the accelerating voltage applied on the A-K gap is problematic. This is even more difficult in an SMP diode where the A-K gap is very small (~1 cm) and the diode region very hostile. The accelerating voltage quoted in the literature is from estimates based on the measurements of the anode and cathode currents of the MITL far upstream from the diode and utilizing the para-potential flow theories and inductive corrections. Thus, it would be interesting to have another independent measurement to evaluate the A-K voltage. The diode's anode is made of a number of high-Z metals in order to produce copious and energetic flash x-rays. It was established experimentally that the back-streaming ion currents are a strong function of the anode materials and their stage of cleanness. We have measured the back-streaming ion currents emitted from the anode and propagating through a hollow cathode tip for various diode configurations and different techniques of target cleaning treatment: namely, heating at very high temperatures with DC and pulsed current, with RF plasma cleaning, and with both plasma cleaning and heating. In conclusion, we have also evaluated the A-K gap voltage by energy filtering technique. Experimental results in comparison with LSP simulations are presented.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Laser ablation of high-loading Li-ion battery electrodes improves accessible capacity and cycle life for Behind-the-Meter Storage

Adoption of Behind-the-Meter Storage (BTMS) requires design of batteries that enable high safety, long cycle life, and low cost at the system level. Pairing Li 4 Ti 5 O 12 (LTO) with LiMn 2 O 4 (LMO) achieves targets related to safety and cycle life, but these materials' low energy densities contribute to higher cost at the system scale. Increasing electrode loading is a simple approach to improve energy density, but comes with a trade-off in electrode utilization due to long, tortuous Li + diffusion pathways. Here, laser ablation is used to microstructure (pattern) high-loading electrodes to enhance electrode performance through improved Li + diffusion pathways. Four cell types, comprising combinations of standard or patterned anode and cathode, were prepared to evaluate the effects of laser ablation at each electrode. A rate test shows that patterning electrodes enhances active material utilization at ≳1C rates. Patterning the cathode yields the most benefit, as cells with a patterned cathode demonstrate a ~20% higher accessible capacity than those without at 1.4C. Additionally, 1C capacity retention of cells with patterned cathode (91% through 3000 cycles) is significantly improved over cells with only the anode patterned (64%) and non-patterned electrodes (50%). Characterization of post-mortem cells before and after refreshing their electrolyte suggests that 1C capacity retention is improved by mitigation of electrode "dry-out". We hypothesize that the microstructure acts as a reservoir of additional electrolyte, or a path for gas to escape, so that active material remains wetted throughout long-term cycling, and/or the microstructure may reduce localized, gas-forming overpotentials in the high-loading electrode.

25 ENERGY STORAGE↗

DOE OSTI2022

Multi-Scale Modeling of Hydrogen Transport in a Porous Fuel Cell Anode

Proton-exchange-membrane fuel cells (PEMFC) are a clean energy conversion alternative to traditional fossil-fuel combustion; however, transport resistances in the electrode pose a lower-limit to catalyst loading and commercialization of PEMFCs. PEMFCs consist of simultaneous hydrogen (H 2 ) oxidation and oxygen (O 2 ) reduction at the anode and cathode, respectively. Here, while oxygen transport resistances in PEMFCs have been widely studied both experimentally and analytically, hydrogen transport resistances are less understood. Herein, we present a physics-based model that encompasses multi-scale transport within the anode side of the PEMFC. The O 2 in the cathode here is omitted and replaced with H 2 to deconvolute O 2 transport resistance contributions, similar to that of a hydrogen pump. Replication of the hydrogen pump setup allows for comparison of the model against experimental analysis of H 2 gas-transport resistance in H 2 limiting-current experiments, which can also inform gas transport (including oxygen) in general. Herein, we present a multi-scale analytical model of the porous anode catalyst layers and individual catalyst agglomerates that enables determination of the effects of electrode morphology such as agglomerate size, catalyst loading, etc. on H 2 transport resistance through the porous electrode to complement and better understand H 2 limiting current experiments and deconvolute local H 2 transport resistances.

Zhang, Rosa↗

DOE OSTI2017

Enhanced Cycling Stability of Sulfur Electrodes through Effective Binding of Pyridine-Functionalized Polymer

Porous carbons have previously been widely used as host materials for sulfur (S) electrodes because of their high conductivity and high surface area. However, they generally lack strong chemical affinity to stabilize polysulfide species. Therefore, conducting polymers have been employed to stabilize S electrodes. Integrating conducting polymers with high-surface-area carbons can create a new materials platform and synergize their functions. However, the previously used conducting polymers were often insoluble, and coating them uniformly from solution onto a nonpolar carbon substrate is a challenge. Here, we report that solution-processable isoindigo-based polymers incorporating polar substituents provide critical features: the conjugated backbone provides good conductivity; functional pyridine groups provide high affinity to polysulfide species; and they possess high solubility in organic solvents. Here, these lead to effective coating on various carbonaceous substrates to provide highly stable sulfur electrodes. Importantly, the electrodes exhibit good capacity retention (80% over 300 cycles) at sulfur mass loading of 3.2 mg/cm 2 , which significantly surpasses the performance of others reported in polymer-enabled sulfur cathodes.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Experimental study on magnetically insulated transmission line electrode surface evolution process under MA/cm current density

The design of high-current density magnetically insulated transmission line (MITL) is a difficult problem of current large-scale Z-pinch device. In particular, a thorough understanding of the MITL electrode surface evolution process under high current density is lacking. On the “QiangGuang-I” accelerator, the load area possesses a low inductance short-circuit structure with a diameter of 2.85 mm at the cathode, and three reflux columns with a diameter of 3 mm and uniformly distributed circumference at the anode. The length of the high density MITL area is 20 mm. A laser interferometer is used to assess and analyze the state of the MITL cathode and anode gap, and their evolution process under high current density. Experimental results indicate that evident current loss is not observed in the current density area at pulse leading edge, and peak when the surface current density reaches MA/cm. Analysis on electrode surface working conditions indicates that when the current leading edge is at 71.5% of the peak, the total evaporation of MITL cathode structure can be realized by energy deposition caused by ohmic heating. The electrode state changes, and diffusion conditions are reflected in the laser interferometer image. The MITL cathode area mainly exists in metal vapor form. The metal vapor density in the cathode central region is higher than the upper limit of laser penetration density (∼4 × 10{sup 21}/cm{sup 3}), with an expansion velocity of ∼0.96 km/s. The metal vapor density in the electrode outer area may lead to evident distortion of fringes, and its expansion velocity is faster than that in the center area (1.53 km/s).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2018

Seeding Iron Trifluoride Nanoparticles on Reduced Graphite Oxide for Lithium-Ion Batteries with Enhanced Loading and Stability

Development of electric vehicles and portable electronic devices during the past decade calls for lithium-ion batteries (LIBs) with enhanced energy density and higher stability. Integration of FeF 3 phases and carbon structures leads to promising cathode materials for LIBs with high voltage, capacity, and power. In this study, FeF 3 ·0.33H 2 O nanoparticles were synthesized on reduced graphite oxide (rGO) nanosheets using an in situ approach. By chemically tuning the interfacial bonding between FeF 3 ·0.33H 2 O and rGO, we successfully achieved high particle loading and enhanced cycling stability. Specifically, a discharge capacity of ~208.3 mAh g –1 was observed at a current density of 0.5 C. The FeF 3 ·0.33H 2 O/rGO nanocomposites also demonstrate great cycle capability with a reversible discharge capacity of 133.1 mAh g –1 after 100 cycles at 100 mA g –1 ; the capacity retention is about 97%. Furthermore, this study provides an alternative strategy to further improve the stability and performance of iron fluoride/carbon nanocomposite materials for LIB applications.

25 ENERGY STORAGE↗

DOE OSTI2020

A lithium-sulfur battery with a solution-mediated pathway operating under lean electrolyte conditions

Lithium-sulfur (Li-S) battery is one of the most promising candidates for the next generation energy storage systems. However, several barriers, including polysulfide shuttle effect, the slow solid-solid surface reaction pathway in the lower discharge plateau, and corrosion of Li anode still limit its practical applications, especially under the lean electrolyte condition required for high energy density applications. Here, we propose a solution-mediated sulfur reduction pathway to improve the capacity and reversibility of the sulfur cathode and suppress dendrite growth on the Li metal anode simultaneously. With this method, a high coulombic efficiency (99%) and stable cycle life over 100 cycles were achieved under application-relevant conditions (S loading: 6.2 mg cm-2; electrolyte to sulfur ratio: 3 mLE gs-1; sulfur weigh ratio: 72 wt%). This result is enabled by a specially designed Li2S4-rich electrolyte, in which Li2S is formed through a chemical disproportionation reaction instead of electrochemical routes. A diglyme solvent was used to obtain electrolytes with the optimum range of Li2S4 concentration. Operando X-ray absorption spectroscopy confirms the solution pathway in a practical Li-S cell. This solution pathway not only introduces a new electrolyte regime for practical Li-S batteries, but also provides a new perspective for bypassing the inefficient surface pathway for other electrochemical processes.

Wang, Hui↗

DOE OSTI2023

Predictive Engineering of Interfaces and Cathodes for High-Performance All Solid-State Lithium-Sulfur Batteries

The primary goal of this project is to leverage data-driven methods and machine learning strategies to develop accurate multi-physics models for all-solid-state Li-S battery (ASLSB) materials that can capture electrochemical and transport phenomena over atomic to mesoscopic length/timescales. These models will be rigorously validated by synthesis and advanced characterization experiments. The team will leverage the predictive power of these models, alongside synthesis/characterization experiments and battery fabrication to address longstanding issues at the electrode/electrolyte interfaces in ASLSBs. The project’s proposed technology involves the following: (1) halide-doped solid sulfide electrolytes that can concurrently provide high Li + ion conductivity and suppress dendrite growth; (2) novel mesoporous cathode composed of super-P and carbon nanotubes co-infiltrated with sulfur and sulfide electrolyte, which hold potential to allow high sulfur loading and optimal ion/electron pathways; and (3) functionalization of sulfide electrolyte with ionic liquids to improve physical contact and minimize impedance at the cathode/electrolyte interface. Successful development of proposed predictive models (at multiple scales) will bridge this knowledge gap and will advance fundamental understanding of reaction chemistry, kinetics, charge transfer, and dendrite growth at electrified SSIs. This will enable predictive design of effective strategies to mitigate interfacial problems in ASSLSBs, including poor interfacial contact, interfacial impedance to Li + ion transport, and poor electron/ion conduction within cathodes. Ultimately, the fundamental knowledge gained will lead to development of high-performance ASSLSBs.

25 ENERGY STORAGE↗

DOE OSTI2021

Investigation of Membrane Chemical Degradation as a Function of Catalyst Platinum Loading

Membrane chemical degradation is one of many factors that can impact fuel cell durability. Additionally, the fuel cell’s lifetime heavily depends on the membrane and its ability to maintain chemical and mechanical integrity. Previous studies indicate that chemical degradation is due to the formation of hydroxyl radicals that attack the polymer structure resulting in membrane thinning, pinhole formation, and the release of fluoride and sulfate ions. Membrane durability was investigated using ultra-low Pt electrode loadings (≤ 0.1 mg Pt cm -2 ). Accelerated stress testing (US-DOE protocols) demonstrated that the degradation rate was found to increase with higher Pt loadings. This is most likely due to more heterogeneous sites for radical formation due to hydrogen crossover to the cathode. We also explored membrane degradation rates while varying catalyst layer thickness, ionomer to carbon ratio, and types of carbon support. All of the aforementioned variables impact the membrane degradation rates.

25 ENERGY STORAGE↗

DOE OSTI2023

Oxygen Reduction at PtNi Alloys in Direct Methanol Fuel Cells—Electrode Development and Characterization

Catalyst layers made from novel catalysts must be fabricated in a way that the catalyst can function to its full potential. To characterize a PtNi alloy catalyst for use in the cathode of Direct Methanol Fuel Cells (DMFCs), the effects of the manufacturing technique, ink composition, layer composition, and catalyst loading were here studied in order to reach the maximum performance potential of the catalyst. For a more detailed understanding, beyond the DMFCs performance measurements, we look at the electrochemically active surface area of the catalyst and charge-transfer resistance, as well as the layer quality and ink properties, and relate them to the aspects stated above. As a result, we make catalyst layers with optimized parameters by ultrasonic spray coating that shows the high performance of the catalyst even when containing less Pt than commercial products. Using this approach, we can adjust the catalyst layers to the requirements of DMFCs, hydrogen fuel cells, or polymer electrolyte membrane electrolysis cells.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2021

Porous Fe3O4/S composites for Li/S batteries

Provided are porous Fe3O4/sulfur composites. The composites are composed of porous Fe 3 O 4 nanoparticles and sulfur, where the sulfur loading is 70-85% by weight based on the total weight of the composite. Also provided are batteries having cathodes containing porous FE 3 O 4 composites of the present disclosure.

Abruna, Hector D.↗