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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 307 records · Page 17

Pulsed Light Synthesis of High Entropy Nanocatalysts with Enhanced Catalytic Activity and Prolonged Stability for Oxygen Evolution Reaction

The ability to synthesize compositionally complex nanostructures rapidly is a key to high-throughput functional materials discovery. In addition to being time-consuming, a majority of conventional materials synthesis processes closely follow thermodynamics equilibria, which limit the discovery of new classes of metastable phases such as high entropy oxides (HEO). Herein, a photonic flash synthesis of HEO nanoparticles at timescales of milliseconds is demonstrated. By leveraging the abrupt heating and cooling cycles induced by a high-power-density xenon pulsed light, mixed transition metal salt precursors undergo rapid chemical transformations. Hence, nanoparticles form within milliseconds with a strong affinity to bind to the carbon substrate. Oxygen evolution reaction (OER) activity measurements of the synthesized nanoparticles demonstrate two orders of magnitude prolonged stability at high current densities, without noticeable decay in performance, compared to commercial IrO 2 catalyst. This superior catalytic activity originates from the synergistic effect of different alloying elements mixed at a high entropic state. It is found that Cr addition influences surface activity the most by promoting higher oxidation states, favoring optimal interaction with OER intermediates. The proposed high-throughput method opens new pathways toward developing next-generation functional materials for various electronics, sensing, and environmental applications, in addition to renewable energy conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

When Machine Learning Meets 2D Materials: A Review

The availability of an ever-expanding portfolio of 2D materials with rich internal degrees of freedom (spin, excitonic, valley, sublattice, and layer pseudospin) together with the unique ability to tailor heterostructures made layer by layer in a precisely chosen stacking sequence and relative crystallographic alignments, offers an unprecedented platform for realizing materials by design. However, the breadth of multi-dimensional parameter space and massive data sets involved is emblematic of complex, resource-intensive experimentation, which not only challenges the current state of the art but also renders exhaustive sampling untenable. To this end, machine learning, a very powerful data-driven approach and subset of artificial intelligence, is a potential game-changer, enabling a cheaper – yet more efficient – alternative to traditional computational strategies. It is also a new paradigm for autonomous experimentation for accelerated discovery and machine-assisted design of functional 2D materials and heterostructures. Here, the study reviews the recent progress and challenges of such endeavors, and highlight various emerging opportunities in this frontier research area.

2D materials↗

Thiol‐Functionalized Conjugated Metal–Organic Frameworks for Stable and Efficient Perovskite Photovoltaics

Abstract Metal–organic frameworks (MOFs) have been investigated recently in perovskite photovoltaics owing to their potential to boost optoelectronic performance and device stability. However, the impact of variations in the MOF side chain on perovskite characteristics and the mechanism of MOF/perovskite film formation remains unclear. In this study, three nanoscale thiol‐functionalized UiO‐66‐type Zr‐based MOFs (UiO‐66‐(SH) 2 , UiO‐66‐MSA, and UiO‐66‐DMSA) are systematically employed and examined in perovskite solar cells (PSCs). Among these MOFs, UiO‐66‐(SH) 2 , with its rigid organic ligands, exhibited a strong interaction with perovskite materials with more efficient suppression of perovskite vacancy defects. More importantly, A detailed and in‐depth discussion is provided on the formation mechanism of UiO‐66‐(SH) 2 ‐assisted perovskite film upon in situ GIWAXS performed during the annealing process. The incorporation of UiO‐66‐(SH) 2 additives substantially facilitates the conversion of PbI 2 into the perovskite phase, prolongs the duration of stage I, and induces a delayed phase transformation pathway. Consequently, the UiO‐66‐(SH) 2 ‐assisted device demonstrates reduced defect density and superior optoelectronic properties with optimized power conversion efficiency of 24.09% and enhanced long‐term stability under ambient environment and continuous light illumination conditions. This study acts as a helpful design guide for desired MOF/perovskite structures, enabling further advancements in MOF/perovskite optoelectronic devices.

14 SOLAR ENERGY↗

Unconventional Anomalous Hall Effect Driven by Self‐Intercalation in Covalent 2D Magnet Cr 2 Te 3

Covalent 2D magnets such as Cr 2 Te 3 , which feature self-intercalated magnetic cations located between monolayers of transition-metal dichalcogenide material, offer a unique platform for controlling magnetic order and spin texture, enabling new potential applications for spintronic devices. Here, it is demonstrated that the unconventional anomalous Hall effect (AHE) in Cr 2 Te 3 , characterized by additional humps and dips near the coercive field in AHE hysteresis, originates from an intrinsic mechanism dictated by the self-intercalation. This mechanism is distinctly different from previously proposed mechanisms such as topological Hall effect, or two-channel AHE arising from spatial inhomogeneities. Crucially, multiple Weyl-like nodes emerge in the electronic band structure due to strong spin-orbit coupling, whose positions relative to the Fermi level is sensitively modulated by the canting angles of the self-intercalated Cr cations. These nodes contribute strongly to the Berry curvature and AHE conductivity. This component competes with the contribution from bands that are less affected by the self-intercalation, resulting in a sign change in AHE with temperature and the emergence of additional humps and dips. The findings provide compelling evidence for the intrinsic origin of the unconventional AHE in Cr 2 Te 3 and further establish self-intercalation as a control knob for engineering AHE in complex magnets.

2D magnets↗

Reversible Ferroelectric Polarization Modulation of Chiral Molecular Ferroelectrics by Circularly Polarized Light

Abstract The optical modulation of ferroelectric polarization constitutes a transformative, non‐contact strategy for the precise manipulation of ferroelectric properties, heralding advancements in optically stimulated ferroelectric devices. Despite its potential, progress in this domain is constrained by material limitations and the intricate nature of the underlying mechanisms. Recent studies have achieved efficient regulation of ferroelectric polarization and thermal conductivity in chiral ferroelectric thin films through the application of left‐ and right‐handed circularly polarized light (LCP and RCP). Differential absorption of circularly polarized light (CPL) induces nonequilibrium carrier dynamics, generating distinctive interfacial electrostatic fields that enable precise control of ultrathin ferroelectric films. For (R)‐BINOL−DIPASi and (S)‐BINOL−DIPASi (C 26 H 26 O 2 Si), polarization changes surpass 23%, exhibiting opposite response under LCP and RCP excitation. In R chiral films, remnant polarization decreases from 1.05 µC cm − 2 under LCP to 0.85 µC cm − 2 under RCP, whereas in S chiral films, polarization increases from 0.85 µC cm − 2 under LCP to 0.98 µC cm − 2 under RCP. This reversible modulation facilitates reliable switching between ON and OFF states, presenting the potential of chiral ferroelectric materials for flexible, high‐speed integrated photonic sensor technologies.

Chemistry↗

Overcoming the Damping–Elasticity Paradox via 3D‐Printed NiTiSn Nanocomposite

Abstract Developing high damping alloys (HDAs) with large elastic strain has attracted growing attention due to the increasing demand for energy absorption with overload reliability and reusability. However, damping capacity inherently conflicts with elasticity, because the former requires a liable movement of crystal defects while the latter opposite. To deal with the damping‐elasticity paradox, the advantage of pseudobinary eutectic reaction and rapid cooling of laser powder bed fusion is taken to fabricate a bulk NiTiSn nanocomposite with a two‐level hierarchical structure. The first‐level architecture is composed of martensitic NiTi nanolamellae and reinforced Ti 3 Sn nanolamellae. In addition to lattice strain matching and lamellar boundary strengthening, a novel mechanism of martensite reorientation mediated by reversible stress‐induced detwinning‐twinning is activated to generate large elastic strain. A high density of nanotwins and nanodomains within NiTi nanolamellae constitute the second‐level architecture, which provides pronounced internal friction for high damping capacity. As a result, our NiTiSn nanocomposite exhibits a record‐high integration of damping capacity (tanδ > 0.10) and elastic strain (exceeding 4.5%), as well as superb stability under cyclic overload. This research not only represents a major breakthrough in achieving HDAs with outstanding damping and elastic strain but also offers a novel paradigm for high‐performance functional and structural materials.

Chemistry↗

Thermal Conductivity of BAs under Pressure

Abstract The thermal conductivity of boron arsenide (BAs) is believed to be influenced by phonon scattering selection rules due to its special phonon dispersion. Compression of BAs leads to significant changes in phonon dispersion, which allows for a test of first principles theories for how phonon dispersion affects three‐ and four‐phonon scattering rates. This study reports the thermal conductivity of BAs from 0 to 30 GPa. Thermal conductivity vs. pressure of BAs is measured by time‐domain thermoreflectance with a diamond anvil cell. In stark contrast to what is typical for nonmetallic crystals, BAs is observed to have a pressure independent thermal conductivity below 30 GPa. The thermal conductivity of nonmetallic crystals typically increases upon compression. The unusual pressure independence of BAs's thermal conductivity shows the important relationship between phonon dispersion properties and three‐ and four‐phonon scattering rates.

36 MATERIALS SCIENCE↗

Fundamental Insights from a Single-Crystal Sodium Iridate Battery

Electrochemically driven chemical transformations play the key role in controlling storage of energy in chemical bonds and subsequent conversion to power electric vehicles and consumer electronics. The promise of coupling anionic oxygen redox with cationic redox to achieve a substantial increase in capacities has inspired research in a wide range of electrode materials. A key challenge is that these studies have focused on polycrystalline materials, where it is hard to perform precise structural determinations, especially related to the location of light atoms. Here a different approach is utilized and a highly ordered single crystal, Na 2-x IrO 3 is harnessed, to explore the role of defects and structural transformations in layered transition metal oxide materials on redox-activity, capacity, reversibility, and stability. Within a combined experimental and theoretical framework, it is demonstrated that 1) it is possible to cycle Na 2-x IrO 3 , offering proof of principle for single-crystal based batteries 2) structural phase transitions coincide with Ir 4+ /Ir 5+ redox couple with no evident contribution from anionic redox 3) strong irreversibility and capacity fade observed during cycling correlates with the Na + migration resulting in progressive growth of an electrochemically inert O 3 -type NaIrO 3 phase.

25 ENERGY STORAGE↗

Understanding the Reactivity of a Thin Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 Solid–State Electrolyte toward Metallic Lithium Anode

The thickness of solid-state electrolytes (SSEs) significantly affects the energy density and safety performance of all-solid-state lithium batteries. However, a sufficient understanding of the reactivity toward lithium metal of ultrathin SSEs (<100 μm) based on NASICON remains lacking. Herein, for the first time, a self-standing and ultrathin (70 μm) NASICON-type Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) electrolyte via a scalable solution process is developed, and X-ray photoelectron spectroscopy reveals that changes in LAGP at the metastable Li-LAGP interface during battery operation is temperature dependent. Severe germanium reduction and decrease in LAGP particle size are detected at the Li-LAGP interface at elevated temperature. As a result, oriented plating of lithium metal on its preferred (110) face occurs during in situ X-ray diffraction cycling.

25 ENERGY STORAGE↗

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Abstract Anionic redox chemistry is emerging as a key concept in the development of high‐energy lithium‐ion batteries, as it enables a nearly doubled charge storage capacity, aiding the development of high‐capacity batteries. However, the anionic reactivity is frequently irreversible from charge to discharge, leading to rapid decay of the capacity and voltage of batteries over long‐term cycling. Although the possibility of controlling the anionic redox reactions by tuning the geometric and electronic structures has recently been proposed, the implementation of this strategy is still a critical challenge. Herein, a strategy is proposed to improve the anionic redox reversibility of a model anionic redox active cathode material, Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 , by tuning the surface ligand geometry via the growth of a lattice‐compatible spinel LiCoO 2 coating layer on the particle surface. Detailed local structure and first principles investigations reveal that the shape and orientation of the octahedral layer in the host lattice are modified. Accordingly, a two‐band oxygen redox behavior is triggered in the ligand‐orientation‐regulated Li‐rich cathode, leading to enhanced reversibility, and thus, remarkably improved capacity and voltage retention over cycling. This study highlights the importance of controllable ligand orientation, carving a new path for the development and design of Li‐rich cathodes in the future.

Liu, Yanchen↗

Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Abstract Understanding structure–function relationships enables the design of materials with tailored functionalities. The long‐standing challenge is to design materials with high active volume to improve efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. This study reports a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in 3D and creating a significantly higher active volume. Such a structure in anatase is obtained and tuned by phase transformation during the heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

Ren, Peng↗

Electrolytes Polymerization‐Induced Cathode‐Electrolyte‐Interphase for High Voltage Lithium‐Ion Batteries

Abstract Lithium‐ion batteries (LIBs) based on LiNi x Co y Mn 1‐x‐y O 2 (NCM) cathode materials have been widely commercialized, because of their high energy density, favorable rate performance, and relatively low cost. However, with increased Ni content to further increase their energy density, their cycling stability deteriorates dramatically and thus fails to meet the commercial application requirements. The artificial cathode‐electrolyte‐interphase (CEI) is a promising approach to solve this problem. Here, a robust CEI is fabricated through in situ polymerization of ethylene carbonate induced by aluminum isopropoxide (AIP). By adding 1 wt.% AIP in a commercial electrolyte, the capacity retention of LiNi 0.8 Co 0.1 Mn 0.1 O 2 ||Li cell at 1 C rate has been significantly increased from 80.8% to 97.8% with a highly reversible capacity of 176 mA h g −1 after 200 cycles. AIP can be also used as an additive during the slurry‐making process, enabling a reversible capacity of 170 mA h g −1 for LiCoO 2 after 200 cycles even at a high charge cut‐off voltage of 4.6 V. It is confirmed that the in situ formed CEI layer can prevent the cathodes from cracking and reduce the irreversible phase transformation.

Yang, Jixiang↗

Atomic Gradient Structures: Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Understanding structure–function relationships enables the design of materials with tailored functionalities. The long-standing challenge is to design materials with high active volume to improve the efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. In this work, we report a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in three-dimension and creating a significantly high active volume. Such a structure in anatase is obtained and tuned by phase transformation during heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

TiO2↗

Operating High-Energy Lithium-Metal Pouch Cells with Reduced Stack Pressure Through a Rational Lithium-Host Design

Transitioning from a liquid electrolyte to an inorganic solid electrolyte offers a potential pathway to enable highly reversible lithium-metal anodes. However, the solid-electrolyte-protected lithium-metal anode suffers from poor interfacial ionic contacts and requires an impractically high stack pressure (>1.0 MPa) to maintain the interfacial contacts. It is demonstrated here that combining a hollow silver/carbon fiber scaffold and an inorganic/organic composite electrolyte enables a highly reversible lithium-metal anode. Since the high surface area of the electrode provides intimate contact and the hollow structure of the electrode relieves the lithium plating-induced stress, the electrode/electrolyte interface remains stable during cycling even under mild stack pressure. This unconventional structural design is validated in practical pouch cells assembled with the 3D lithium host containing a onefold excess of lithium and a high-nickel cathode. At a mild stack pressure of 320 kPa, the pouch cell displays 83% capacity retention for 200 cycles. This work illustrates that combining a hollow electrode architecture and a robust solid electrolyte offers a practical pathway toward rechargeable lithium-metal anodes.

36 MATERIALS SCIENCE↗

Oxide‐Based Solid‐State Batteries: A Perspective on Composite Cathode Architecture

Abstract The garnet‐type phase Li 7 La 3 Zr 2 O 12 (LLZO) attracts significant attention as an oxide solid electrolyte to enable safe and robust solid‐state batteries (SSBs) with potentially high energy density. However, while significant progress has been made in demonstrating compatibility with Li metal, integrating LLZO into composite cathodes remains a challenge. The current perspective focuses on the critical issues that need to be addressed to achieve the ultimate goal of an all‐solid‐state LLZO‐based battery that delivers safety, durability, and pack‐level performance characteristics that are unobtainable with state‐of‐the‐art Li‐ion batteries. This perspective complements existing reviews of solid/solid interfaces with more emphasis on understanding numerous homo‐ and heteroionic interfaces in a pure oxide‐based SSB and the various phenomena that accompany the evolution of the chemical, electrochemical, structural, morphological, and mechanical properties of those interfaces during processing and operation. Finally, the insights gained from a comprehensive literature survey of LLZO–cathode interfaces are used to guide efforts for the development of LLZO‐based SSBs.

25 ENERGY STORAGE↗

A Dual–Phase Electrolyte for High–Energy Lithium–Sulfur Batteries

Dissolution of lithium polysulfides (LiPSs) is essential for fast cathode kinetics, but detrimental for anode stability, especially under lean electrolyte conditions. Here in this work, the phase separation phenomenon between solvents with different polarities (tetramethyl sulfone [TMS] and dibutyl ether [DBE]) is utilized to enable the design of a dual-phase electrolyte. High-polarity, high-density TMS–lithium bis(trifluoromethanesulfonyl)imide–ammonium trifluoroacetate as the cathode electrolyte strongly solvates LiPSs, which propel the sulfur redox reaction. Moreover, the composite of DBE and a polymeric ion conductor serves as the anode electrolyte. The addition of DBE in the anode side effectively prevents the crossover of corrosive species (LiPSs and ammonia trifluoroacetate), enabling a significant improvement in Li-metal anode stability. The electrode-specific dual-phase electrolyte design provides electrochemical performance superior to conventional electrolytes. Without additional electrode engineering, pouch cells assemble with the dual-phase electrolyte cycle under a lean electrolyte (4 µL mg –1 ) and low-Li-excess condition (N/P = 3) for 120 cycles.

25 ENERGY STORAGE↗

Enabling Extreme Fast-Charging: Challenges at the Cathode and Mitigation Strategies

We report charging lithium-ion batteries (LiBs) in 10 to 15 min via extreme fast-charging (XFC) is important for the widespread adoption of electric vehicles (EVs). Lately, the battery research community has focused on identifying XFC bottlenecks and determining novel design solutions. Like other LiB components, cathodes can present XFC bottlenecks, especially when considering long-term battery life. Therefore, it is necessary to develop a comprehensive understanding of how XFC conditions degrade LiB cathodes. The present article reviews relevant cathode-focused studies and summarizes the current understanding regarding cathode performance and aging issues under XFC conditions. Dominant aging modes and mechanisms are identified at different length-scales with electrochemical correlations for LiNi x Mn y Co z O 2 (NMC)-based cathodes. A range of electrochemical techniques and models provide key insights into cathode performance and life issues. A suite of multimodal and multiscale microscopy and X-ray techniques is surveyed to quantify chemical, structural, and crystallographic NMC-cathode degradation. Cathode cycle-life is scaled to equivalent EV miles to illustrate how cathode degradation translates to real-world scenarios and quantifies cathode-related bottlenecks that hinder XFC adoption. Finally, the article discusses several cathode cycle-life aging mitigation strategies with example case studies and identifies remaining challenges.

25 ENERGY STORAGE↗