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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 271 records · Page 15

Approaching the Radiative Efficiency Limit in Perovskite Solar Cells with Scalable Defect Passivation and Selective Contacts

This award aimed to enable perovskite solar cells to approach the radiative efficiency limit in scalable manufacturing environments by controlling recombination losses, especially surface recombination losses at electrodes and interfaces. The project combined organic molecular synthesis, perovskite film processing and characterization, and spectroscopic tool development for probing recombination centers. The project ultimately achieved record-low surface recombination velocity (SRV) in mixed cation methylammonium-free perovskite thin films, demonstrated photoluminescence as an effective process metrology tool to optimizing processing of device stacks, and showed that the aminopropyltrimethoxysilane (APTMS) is suitable for passivating the exposed perovskite interface in p-i-n stack devices. The project used combinations of phosphonic acids to modify the transparent conducting oxide and APTMS to passivate the perovskite/electron transport layer interface, thereby demonstrating reduction of SRVs in both partial and full device stacks. The project showed concomitant improvements in device performance, and demonstrated that APTMS passivation was compatible with large area coating of external stakeholder perovskite films using both scalable solution and vapor methods. Notably, the project also supplied surface passivating materials to a number of other US based and SETO-funded teams.

14 SOLAR ENERGY↗

Stacking Independence and Resonant Interlayer Excitation of Monolayer WSe 2 /MoSe 2 Heterostructures for Photocatalytic Energy Conversion

Here, we report a comparison of the photocatalytic performance of WSe 2 -on-MoSe 2 and MoSe 2 -on-WSe 2 heterostructures. While built-in electric fields exist in these heterostructures on the order of 100 kV/cm due to band offsets between these two materials, the photocatalytic performance (i.e., photocurrent) is independent of the stacking order of the two materials. Solving Poisson’s equation under these conditions, we find that the built-in electric field produced in the heterostructure is at least 1 order of magnitude smaller than that produced in the electrochemical double layer (i.e., Helmholtz layer). Mott–Schottky measurements indicate that transition metal dichalcogenides (TMDCs) on ITO electrodes have similar capacitance to that of bare ITO, providing further evidence that the interfacial electric fields produced in the solid state heterostructure are negligible compared to the fields generated by the ions in solution. The photocatalytic performance of these heterostructures provided the largest relative enhancement in the heterojunction region under 920 and 785 nm irradiation compared with 532 and 633 nm wavelength excitation. Here, the 920 nm (1.35 eV) photons lie below the band gaps and produce very little photocurrent in the constituent monolayer materials but resonantly excite the interlayer optical transition in the heterostructure, producing a 5-fold enhancement in the measured photocurrent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low Melting Temperature Gallium–Indium Liquid Metal Anode for Solid-State Li-Ion Batteries

Solid-state Li-ion batteries are attracting attention for their enhanced safety features, higher energy density, and broader operational temperature range compared to systems based on liquid electrolytes. However, current solid-state Li-ion batteries face performance challenges, such as suboptimal cycling and poor rate capabilities, often due to inadequate interfacial contact between the solid electrolyte and electrodes. To address this issue, we incorporated a gallium–indium (Ga–In) liquid metal as the anode in a solid-state Li-ion battery setup, employing Li 6 PS 5 Cl as the solid electrolyte. Operating at room temperature, this configuration achieved an initial capacity of 389 mAh g –1 and maintained 88% of this capacity after 30 cycles at a 0.05 C rate. It also demonstrated a capacity retention of 66% after 500 cycles at a 0.5 C rate. In comparison to solid anode materials, such as tin, the Ga–In liquid metal exhibited superior cycling stability and rate capacity, which is due to the self-healing and fluid properties of the alloy that ensure stable interfacial contact with solid electrolytes. In situ X-ray diffraction (XRD) and ex situ scanning electron microscope (SEM) analyses revealed that indium does not directly participate in the lithiation/delithiation process. Instead, it helps maintain the alloy’s low melting point, facilitating its return to a liquid state after delithiation. In a comparative analysis of stack pressure during cycling in cells utilizing Ga–In liquid metal and tin, the Ga–In liquid metal cell demonstrated an ability to buffer pressure increases associated with deformation. In conclusion, these findings suggest a promising approach for enhancing solid-state batteries by integrating liquid metal anodes, which improve interfacial contact and stability.

Alloys↗

Scalable membrane-less microbial electrolysis cell with multiple compact electrode assemblies for high performance hydrogen production

Bioelectrochemical hydrogen production via microbial electrolysis cells (MECs) is a promising method for sustainable energy production and decarbonization of energy systems. However, the application of MECs is limited by the electrochemical performance, scalability, and the cost associated with expensive materials. Here, in this study, a scalable MEC (500 mL) with novel compact electrode assemblies and high electrode surface area to volume ratio (160 m 2 /m 3 ) was designed and constructed. The use of membranes, precious metal catalyst, and current collectors with high costs was avoided. A high current density at the steady state of 49.5 ± 5.3 A/m 2 was achieved using acetate as the substrate with phosphate buffer under the applied voltage of 1.01 V. The corresponding volumetric current density was 3948 ± 422 A/m 3 . The compact electrode assembly design limited methane production rate to 3.9 ± 0.2 L/L/D, while achieving a hydrogen production rate of 33.7 ± 1.7 L/L/D. With the suppression of microbial hydrogen consumption, the hydrogen production rate was 39.8 ± 1.9 L/L/D, higher by almost one order of magnitude than those of MECs with scaling up attempts. The compact electrode configuration reduced internal resistance to 88.5 ± 4.4 Ω cm 2 . The energy efficiency based on input electricity was 146 ± 7 % to 189 ± 9 % within the applied voltage range of 0.71 to 1.05 V. The results in this study demonstrated successful scaling up of high performance small MECs and offered a new possible approach of scaling up MECs by stacking high-performance subunits, with no trade-offs on electrochemical performance.

08 HYDROGEN↗

Prototyping of a Rotary Triboelectric Nanogenerator for Power at Sea

Increasing at-sea power generation by Triboelectric Nanogenerator (TENG) energy harvesters towards the order of 1-Watt will create significant opportunities to power ocean observation buoys and distributed sensor nodes by extending mission time and increasing sensor payload. Of the many possible configurations of harvesting wave energy with TENGs, we document the rationale for choosing and developing a rotary TENG that operates by the freestanding mode. The rotary TENG prototype consists of two plates, a rotor and a stator, to take advantage of the various mechanisms of converting wave action into rotational motion. We have constructed a testing apparatus that allows us to vary several key parameters of the device: distance between rotor and stator, triboelectric material, rotational speed, number of electrodes and output load impedance. Preliminary results show that when driven at a constant 500 rpm, we can achieve a power density of 0.7 W/m3. A variable speed motor drives the rotor, which can be driven using a velocity profile informed by the equivalent to the output from a wave energy converter (WEC). The optimized rotational TENG can be stacked and driven by a single shaft, increasing the energy density of the device. The output of such a TENG could be used to power devices in the ocean at a low cost and high durability.

electrostatic generator↗

Electrostatic Gating of Ionic Conductance through Heterogeneous van der Waals Nanopores

Nanofluidic ionic transistors typically require gate voltages above 1 V and operate only at submillimolar ionic strengths, limiting their biocompatible applications. We demonstrate ionic transistors consisting of single sub-10 nm nanopores drilled in van der Waals (vdW) heterostructures with internal gate electrodes made of few-layer graphene. These devices deliver up to 10-fold current modulation at gate voltages as low as 0.3 V in 10 mM KCl, and ∼2-fold modulation at near-physiological 100 mM KCl. Baseline conductance with no gate shows surface-charge-dominated transport below 100 mM KCl, consistent with negatively charged hBN walls and ∼5 nm opening of the pores. The surface charge and the electrochemical asymmetry introduced by the three-electrode configuration govern the device’s behavior: negative gate voltage (V G ) enriches ionic concentrations and enhances current, whereas positive V G induces a local depletion zone that suppresses transport. The current modulation by V G is dependent on the polarity of the transmembrane potential and leads to ion current rectification. Molecular dynamics simulations of a nanopore in a hBN–graphene–hBN stack reveal confinement and surface charge-dependent suppression of the relative permittivity of interfacial water. Continuum modeling with radially varying interfacial water permittivity reproduces the asymmetric I–V characteristics and explains how the embedded gate sculpts local potential and ion concentrations. By enabling sub-0.5 V control of ionic transport at up to 100 mM salt concentrations, these devices address a key need in nanofluidics to create low-power ionic circuits and biosensing.

Materials science↗

Binder-free thin graphite fiber mat sandwich electrode architectures for energy-efficient vanadium redox flow batteries

Vanadium redox flow batteries (VRFB) are emerging as the preferred energy storage solution for long-duration energy storage (LDES) and grid-scale load levelling. In this study, we report a novel binder-free sandwich electrode architecture consisting of a thin layer (6–12 mg cm –2 ) of thermally activated graphite felt mat (TGFM) sandwiched between thin carbon papers (TCP-TGFM-TCP). This electrode architecture substantially reduced the polarization (I-V) resistance of the VRFB by 23 %, resulting in a current density increase from 340 mA cm –2 at 1 V for the thermally activated graphite felt (TGF) electrode to 470 mA cm –2 at 1 V, and an energy efficiency of 80 % at 100 mA cm –2 is realized.

25 ENERGY STORAGE↗

Increasing the Pressure‐Free Stripping Capacity of the Lithium Metal Anode in Solid‐State‐Batteries by Carbon Nanotubes

Abstract Lithium metal is the key anode material for solid‐state‐batteries as its successful implementation will drastically increase their energy and power densities. However, anode contact loss during stripping leads to dendrites upon plating and subsequent cell failure. Design strategies to mitigate these issues are crucial to enable the use of lithium metal anodes. This paper reports the dissolution kinetics of composite anodes made of lithium metal and carbon nanotubes (CNTs) with a garnet‐type solid electrolyte (SE). In addition to an enhancement of the effective diffusion within the anode, its dissolution is fundamentally changed from being 2D to 3D. By maintaining contact with the SE, the CNTs facilitate lithium transport to the interface, which yields more than 20 mAh cm −2 discharge capacity at 100 µ A cm −2 without the application of external stack pressure ( > 1 MPa). Conclusions drawn from electrochemical data on the anode microstructure are validated using cryo‐focused‐ion‐beam scanning electron microscopy and correlated with the mechanical properties. Micro‐indentation, acoustic analysis, and stress–strain testing show that mechanical properties of the anode, like yield strength and hardness, are adjustable. Overall, it is shown that the mechanical and electrochemical properties of Li–CNT composite electrodes can be tailored to suit the requirements of a practical cell.

Fuchs, Till↗

Fabricating Silver Nanowire–IZO Composite Transparent Conducting Electrodes at Roll-to-Roll Speed for Perovskite Solar Cells

This study addresses the challenges of efficient, large-scale production of flexible transparent conducting electrodes (TCEs). We fabricate TCEs on polyethylene terephthalate (PET) substrates using a high-speed roll-to-roll (R2R) compatible method that combines gravure printing and photonic curing. The hybrid TCEs consist of Ag metal bus lines (Ag MBLs) coated with silver nanowires (AgNWs) and indium zinc oxide (IZO) layers. All materials are solutions deposited at speeds exceeding 10 m/min using gravure printing. We conduct a systematic study to optimize coating parameters and tune solvent composition to achieve a uniform AgNW network. The entire stack undergoes photonic curing, a low-energy annealing method that can be completed at high speeds and will not damage the plastic substrates. The resulting hybrid TCEs exhibit a transmittance of 92% averaged from 400 nm to 1100 nm and a sheet resistance of 11 Ω/sq. Mechanical durability is tested by bending the hybrid TCEs to a strain of 1% for 2000 cycles. The results show a minimal increase (<5%) in resistance. The high-throughput potential is established by showing that each hybrid TCE fabrication step can be completed at 30 m/min. We further fabricate methylammonium lead iodide solar cells to demonstrate the practical use of these TCEs, achieving an average power conversion efficiency (PCE) of 13%. The high-performance hybrid TCEs produced using R2R-compatible processes show potential as a viable choice for replacing vacuum-deposited indium tin oxide films on PET.

14 SOLAR ENERGY↗

Developing Stable Critical Materials and Microstructure for High-Flux and Efficient Hydrogen Production through Reversible Solid Oxide Cells

Reversible Solid Oxide Cells (RSOCs), which operate as either Solid Oxide Fuel Cells (SOFCs) or Solid Oxide Electrolytic Cells (SOECs), hold great promise for clean, high-efficiency energy conversion and hydrogen production. However, their commercial potential is hindered by stability issues arising from temperature-induced materials degradation. While substantial progress has been made in developing durable, reduced-temperature SOFCs - bringing them closer to commercial deployment, SOECs still exhibit substantially higher degradation rates at both the cell and stack levels under practical operating conditions.

08 HYDROGEN↗

A multiscale model to understand the interface chemistry, contacts, and dynamics during lithium stripping

A reversible Li-metal electrode, paired with a solid electrolyte, is critical for attaining higher energy density and safer batteries beyond the current lithium-ion cells. A stable stripping process may be even harder to attain as the stripping process will remove Li-atoms from the surface, and naturally reduce surface contact area, if not self-corrected by other mechanisms, such as diffusion and plastic deformation under an applied external stack pressure. Here, we capture these mechanisms occurring at multiple length- and time- scales, i.e., interface interactions, vacancy hopping, and plastic deformation, by integrating density functional theory (DFT) simulations, kinetic Monte Carlo (KMC), and continuum finite element method (FEM). By assuming the self-affine nature of multiscale contacts, we predict the steady-state contact area as a function of stripping current density, interface wettability, and stack pressure. We further estimate the exponential increase of overpotential due to contact area loss to maintain the same stripping current density. We demonstrate that a lithiophilic interface requires less stack pressure to reach the same steady-state contact area fraction than a lithiophobic interface. A “tolerable steady-state” contact area loss for maintaining stable stripping is estimated at 20 %, corresponding to a 10 % increase in overpotential. To constrain contact loss within the tolerance, the required stack pressure is 0.1, 0.5, and 2 times the yield strength of lithium metal for three distinct interfaces, lithiophilic Li/lithium oxide(Li2O), Li/lithium lanthanum zirconium oxide(LLZO), and lithiophoblic Li/lithium fluoride(LiF), respectively. The modeling results agree with experiments on the impact of the stack pressure quantitatively, while the discrepancy in stripping rate sensitivity is attributed to the simplifying interface interaction in our simulations. Overall, this multiscale simulation framework demonstrates the importance of electrochemical-mechanical coupling in understanding the dynamics of the Li/SE interface during stripping.

Feng, Min↗

Long-life high performance fuel cell program

A multihundred kilowatt Regenerative Fuel Cell for use in a space station is envisioned. Three 0.508 sq ft (471.9 cm) active area multicell stacks were assembled and endurance tested. The long term performance stability of the platinum on carbon catalyst configuration suitability of the lightweight graphite electrolyte reservoir plate, the stability of the free standing butyl bonded potassium titanate matrix structure, and the long life potential of a hybrid polysulfone cell edge frame construction were demonstrated. A 18,000 hour demonstration test of multicell stack to a continuous cyclical load profile was conducted. A total of 12,000 cycles was completed, confirming the ability of the alkaline fuel cell to operate to a load profile simulating Regenerative Fuel Cell operation. An orbiter production hydrogen recirculation pump employed in support of the cyclical load profile test completed 13,000 hours of maintenance free operation. Laboratory endurance tests demonstrated the suitability of the butyl bonded potassium matrix, perforated nickel foil electrode substrates, and carbon ribbed substrate anode for use in the alkaline fuel cell. Corrosion testing of materials at 250 F (121.1 C) in 42% wgt. potassium identified ceria, zirconia, strontium titanate, strontium zirconate and lithium cobaltate as candidate matrix materials.

Martin, R. E.↗

Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking

Multiferroic tunnel junctions (MFTJs) represent a class of multistate, non-volatile spintronic devices, in which electron tunnelling can be manipulated by switching long-range lattice and spin orders. In contrast to conventional oxide-based MFTJs, MFTJs constructed from two-dimensional van der Waals (vdW) crystals promise minimal defect concentration in the constituents and at interfaces, which may allow for probing intrinsic tunnelling physics and the development of high-performance devices. Here, in this study, we construct Fe 3 GeTe 2 /CuInP 2 S 6 /Fe 3 GeTe 2 all-vdW MFTJs by assembling multilayer flakes of ferromagnetic Fe 3 GeTe 2 electrodes and a ferroelectric CuInP 2 S 6 spacer. These MFTJs exhibit four non-volatile resistance states featuring sizable tunnelling magnetoresistance of ∼10 2 % and tunnelling electroresistance of ∼10 4 %. To tune the properties of the vdW MFTJ, we make use of the flexibility in material choice offered by vdW heterostructure devices; we use Fe 3 GeTe 2 /Fe 5 GeTe 2 asymmetric electrodes to boost the tunnelling electroresistance by 10 3 %, we integrate In 2 Se 3 as a ferroelectric with a smaller bandgap to enhance the ON-state current density by 10 4 % to 10 4 A cm −2 and we use Fe 3 GaTe 2 electrodes to demonstrate room temperature operation. Furthermore, when we combine the asymmetric ferromagnetic electrodes with the small-bandgap ferroelectric spacer to construct Fe 3 GeTe 2 /In 2 Se 3 /Fe 5 GeTe 2 MFTJs, we simultaneously realized tunnelling electroresistance of 10 6 % and an ON-state current density of 10 4 A cm −2 , both two orders of magnitude higher than the highest values achieved with conventional oxide-based MFTJs. In the future, our all-vdW MFTJs with the tailorability of all functional layers may make it possible to investigate fundamental aspects of interlayer tunnelling and enable the design of functional magnetoelectric nanodevices.

Xie, Ti [University of Maryland, College Park, MD ↗

Origin of the lithium metal anode instability in solid-state batteries during discharge

Enabling the lithium metal anode (LMA) in solid-state batteries (SSBs) would increase energy density and specific energy compared with lithium-ion batteries. However, pore formation in LMAs with irregular morphology, even at low current density, during discharge results in an unstable, high-impedance interface. Understanding and addressing this inherent anode instability is essential for increasing the power densities in SSBs. Herein, we suggest that the morphology of the stripped electrode is related to dislocations in the LMA. To investigate the influence of dislocations, symmetric cells, Li|Li 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO)|X-Li, are studied, where X-Li represents the microstructurally controlled LMA obtained via suitable thermomechanical processing. Operando impedance measurements are corroborated with SEM, confocal microscopy, and AFM data. Based on the experimental observations, a mechanism for pore formation is proposed. Here we show that the stack pressure required to maintain a stable interface is governed by the lithium microstructure and its thermomechanical processing history.

25 ENERGY STORAGE↗

A scalable membrane electrode assembly architecture for efficient electrochemical conversion of CO2 to formic acid

Abstract The electrochemical reduction of carbon dioxide to formic acid is a promising pathway to improve CO 2 utilization and has potential applications as a hydrogen storage medium. In this work, a zero-gap membrane electrode assembly architecture is developed for the direct electrochemical synthesis of formic acid from carbon dioxide. The key technological advancement is a perforated cation exchange membrane, which, when utilized in a forward bias bipolar membrane configuration, allows formic acid generated at the membrane interface to exit through the anode flow field at concentrations up to 0.25 M. Having no additional interlayer components between the anode and cathode this concept is positioned to leverage currently available materials and stack designs ubiquitous in fuel cell and H 2 electrolysis, enabling a more rapid transition to scale and commercialization. The perforated cation exchange membrane configuration can achieve >75% Faradaic efficiency to formic acid at <2 V and 300 mA/cm 2 in a 25 cm 2 cell. More critically, a 55-hour stability test at 200 mA/cm 2 shows stable Faradaic efficiency and cell voltage. Technoeconomic analysis is utilized to illustrate a path towards achieving cost parity with current formic acid production methods.

08 HYDROGEN↗

Probing the Effects of the First Atomic Layer on the Dynamic Behavior of Sub-2 nm MgO/Al 2 O 3 Memristors

As electronic devices continue to scale down from the current sub-5 nm range, atomic-scale control of defects becomes increasingly crucial to suppressing their impact on the physical properties of the devices. Memristors present an excellent example as a nonlinear and dynamic device with high speed and endurance required for electronic applications ranging from neuromorphic computing to nonvolatile memories. Herein we investigate the impact of atomic defects in sub-2 nm thick MgO/Al 2 O 3 atomic layer stack (ALS) memristors that use an M1 (switching layer)/M2 (oxygen vacancy reservoir layer) bilayer structure grown using in vacuo atomic layer deposition (iALD). Intriguingly, we revealed a direct correlation of the atomic defects in the M2 layer with the memristor dynamic behavior using a combined analysis of in situ scanning tunneling spectroscopy (iSTS) on the M2 layer and ex situ characterization on the memristors. Specifically, incomplete coverage of the 1st ALD atomic layer of M2 on the electrode yields defects at the M2/electrode interface. Despite the monotonic increase of ALD coverage, by almost three-fold from ~30% to >90%, at completion of the M2 layer of ~ 0.7 nm in thickness, the impact of the defects on the M2/electrode interface has been found detrimental to both memristor switching speed and endurance. Guided by atomistic simulation, we addressed the issue of interface defects via tuning of the Al surface hydroxylation to increase the first atomic layer ALD coverage to ~75%, leading to improved memristor switching speed and endurance by several orders of magnitude. In conclusion, these findings shed light on the correlation between the atomic defects and the dynamic behavior of sub-2 nm memristors and the importance of minimizing the atomic defects in memristors for future electronic applications.

Atomic Layer Deposition↗

Modeling Framework to Analyze Performance and Structural Reliability of Solid Oxide Electrolysis Cells

Solid oxide electrolysis cells (SOEC) have been receiving significant attention recently because of their high energy efficiency and fast hydrogen production. In this study a multi-physics model to simulate the SOEC performance and structural reliability of a state-of-the-art planar SOEC design was developed. The electrochemical reactions, fluid dynamics, species transport, electron transfer, and heat transfer were modeled in the commercial computational fluid dynamics (CFD) software STAR-CCM+. The thermomechanical analysis and the associated structural reliability evaluations were conducted using the commercial finite element analysis software ANSYS. The electrochemistry model was validated by using the experimentally obtained current-voltage (I-V) characteristics of the electrode-supported SOECs. The reliability analysis using a risk-of-rupture approach showed low failure probabilities under standard operating conditions considered in this study. For cells operated at voltages well above a thermoneutral voltage, the reliability evaluations indicated a potential risk of cell failure, but the damage was concentrated locally in specific areas of the cell which typically do not lead to total loss of cell function. The presented approach provides insights for evaluating representative cell and stack performances and structural reliability without intensive testing and for developing optimally performing and structurally reliable SOECs for efficient hydrogen generation.

25 ENERGY STORAGE↗

Creating and Probing Large Gap 2D Topological Insulators for Quantum Computing (Final Report)

Research under this award focused on experimental and theoretical efforts in developing and characterizing 2D topological insulators (TIs). Key areas of investigation included materials synthesis, device fabrication and characterization, and theoretical advancements. The team synthesized ZrTe 5 , a material with potential for TI phases. Additionally, the team pursued the synthesis of elemental thin films like Indene and Bismuthene, known for their large TI gaps. Indene was successfully stabilized on SiC. Another approach involved stacking and twisting transition metal dichalcogenides (TMDs) to engineer desired TI band structures. On the theoretical front, advancements made under this award predicted remarkable topological properties in twisted WSe2 bilayers, motivating experimental efforts to realize these states. Regarding device fabrication and characterization, significant progress was made in reducing contact resistance, crucial for reliable transport measurements. Contactless Pulsed Tunneling Spectroscopy (CPTS) was employed to study the electronic properties of WTe 2 and WSe 2 . However, challenges in device fabrication and electrode material selection hampered efforts to obtain desired spectra. Ancillary work, utilizing pulsed electrical methods, on the study of sliding ferroelectrics yielded impactful results demonstrating high speed operation and lack of degradation of devices after many billions of cycles.

77 NANOSCIENCE AND NANOTECHNOLOGY↗