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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Gated Molecular Diffusion at Liquid–Liquid Interfaces

The jamming of nanoparticle surfactants (NPSs) at liquid-liquid interface imparts attractive properties to the interfacial assemblies and enables the structuring of liquids. Herein, we report photoresponsive supramolecular microcapsules with jammed NPS assemblies at the oil-water interface, taking advantage of host-guest molecular recognition. The permeability of the colloidal membrane can be effectively manipulated by switching the NPSs from a jammed state to an unjammed state with a photo trigger, leading to a controlled molecular diffusion and release, affording a versatile platform for the construction of next generation smart microcapsule systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

MECHANICAL PERFORMANCE EVALUATION OF THE PRINTED CIRCUIT HEAT EXCHANGER CORE EXPERIMENTS UNDER TENSION AND PRESSURE LOADING

The printed circuit heat exchanger (PCHE) has small channels with high surface area, making them an efficient solution for next-generation nuclear plants (NGNPs). These PCHEs are fabricated through a diffusion bonding process. This fabrication step changes the microstructure of wrought metal plates. The current ASME design code does not support the PCHE design for NGNPs due to a lack of test data. Hence, there has been initiative towards elevated temperature mechanical property characterization of the diffusion bonded material. One of the most common channel shapes is a semicircular channel with sharp corners. These corners act as a stress riser at the diffusion bonding interface. Evaluating elevated temperature mechanical performance of diffusion bonded material in the presence of stress risers is an essential step towards the ASME code development of PCHE design. This study selected two specimen geometries: the first is a PCHE bar specimen for tensile loading with three rows and three columns of channels, and the second is a lab-scaled PCHE with six rows and eight columns of channels. A set of elevated temperature monotonic and cyclic tests were conducted on the PCHE bar specimen to evaluate the mechanical performance under axial tensile loadings to study the failure mechanism. The lab-scaled PCHE specimens were tested under overpressure loads at room temperature, and pressure creep and pressure creep-fatigue loadings to mimic the realistic loading conditions observed in typical NGNPs. The X-ray scans of channeled specimens show interesting observations. The test results and observations are presented in the paper.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stability Analysis of Coupled Advection-Diffusion Models with Bulk Interface Condition

Numerical stability is of critical importance in general circulation models because it affects the design of algorithms, time to solution, and computational costs associated with the simulations, which are very expensive in practice. In this paper we extend the stability analysis for ocean-atmosphere coupling proposed in [Zhang et al., J. Sci. Comput. 84, 44(2020)] to a more realistic model that includes horizontal advection. We analyze various time-stepping strategies. We find that advection has a stabilizing effect in scenarios common to climate models when bulk interface condition and explicit flux coupling are used. We also show that our method can be used to study the stability impact of advection for other interface conditions such as Dirichlet-Neumann conditions.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Enhanced diffusion bonding of alloy 617 using electric field-assisted sintering

The development of compact heat exchangers (CHXs) has gained increasing interest in many industries owing to their high thermal efficiency and reduced size. Diffusion bonding (DB) is an advantageous technique for fabricating CHXs. Alloy 617 is a candidate for manufacturing CHXs for high-temperature advanced nuclear reactors due to its elevated-temperature properties. Previous endeavors in DB of Alloy 617 were conducted by hot pressing (HP), which reported precipitates at the diffusion-bond interface, limited grain boundary (GB) migration, and significantly reduced high-temperature mechanical properties. To overcome these challenges, this study investigated DB of Alloy 617 using electric field-assisted sintering (EFAS). Stacks composed of three sheets were bonded with EFAS using different temperatures, pressures, and hold times. DB using HP as the zero-current analog of EFAS was also performed for comparison. The result shows that Cr- and Mo-rich precipitates were formed at the interface of the hot-pressed samples. The electric current and temperature in EFAS play a significant role in precipitation and GB migration. The electric current coupled with correct temperatures can effectively prevent precipitate formation at the interface and achieve excellent GB migration. Nanoscale Al-rich oxide was formed at the interface of the samples made by both HP and EFAS, but grain boundaries can ignore the nanoscale Al-oxide and migrate across the interface. The temperature, pressure, and hold time also affected diffusion. The temperature is a prerequisite for a successful GB migration, and GB migration can be enhanced by increasing pressure and hold time.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Coupled Interfacial and Bulk Kinetics Govern the Timescales of Multiphase Ozonolysis Reactions

Chemical transformations in aerosols impact the lifetime of particle phase species, the fate of atmospheric pollutants, and both climate- and health-relevant aerosol properties. Timescales for multiphase reactions of ozone in atmospheric aqueous phases are governed by coupled kinetic processes between the gas phase, the particle interface, and its bulk, which respond dynamically to reactive consumption of O 3 . However, models of atmospheric aerosol reactivity often do not account for the coupled nature of multiphase processes. Herein, to examine these dynamics, we use new and prior experimental observations of aqueous droplet reaction kinetics, including three systems with a range of surface affinities and ozonolysis rate coefficients ( trans -aconitic acid (C 6 H 6 O 6 ), maleic acid (C 4 H 4 O 4 ), and sodium nitrite (NaNO 2 )). Using literature rate coefficients and thermodynamic properties, we constrain a simple two-compartment stochastic kinetic model which resolves the interface from the particle bulk and represents O 3 partitioning, diffusion, and reaction as a coupled kinetic system. Our kinetic model accurately predicts decay kinetics across all three systems, demonstrating that both the thermodynamic properties of O 3 and the coupled kinetic and diffusion processes are key to making accurate predictions. An enhanced concentration of adsorbed O 3 , compared to gas and bulk phases is rapidly maintained and remains constant even as O 3 is consumed by reaction. Multiphase systems dynamically seek to achieve equilibrium in response to reactive O 3 loss, but this is hampered at solute concentrations relevant to aqueous aerosol by the rate of O 3 arrival in the bulk by diffusion. As a result, bulk-phase O 3 becomes depleted from its Henry's law solubility. This bulk-phase O 3 depletion limits reaction timescales for relatively slow-reacting organic solutes with low interfacial affinity (i.e., trans-aconitic and maleic acids, with k rxn ≈ 10 3 -10 4 M -1 s -1 ), which is in contrast to fast-reacting solutes with higher surface affinity (i.e., nitrite, with k rxn ≈ 10 5 M -1 s -1 ) where surface reactions strongly impact the observed decay kinetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Non-Diffusive Volume Advection with A High Order Interface Reconstruction Method

We show that non-diffusive volume advection in two-dimensions is achieved with several benchmark problems using a newly developed high-order volume of fluids (VOF) interface reconstruction method. (1) A new VOF interface reconstruction method using circular/corner facets (linear facets are a degenerate case of arcs). We create a circular interface facet in each mixed zone by matching neighbor volume with a hybrid Newton’s-bisection method and the local solution is final. In the general case, the new VOF interface reconstruction has 3rd order accuracy and can be easily made seamless. The new method addresses intrinsic issues with Young’s method such as gaps between interface facets in the case of a curved interface, and inability to define curvature nor identify corners. (2) A non-diffusive volume advection scheme. In an ALE advection step, a well-defined interface can be carried over through a Lagrange step and used to compute volume distribution into a relaxed mesh. Then, an interface reconstruction step is performed to redefine the interface in the relaxed mesh. We must point out that the interface carried over is also a solution of interface reconstruction because all the volume fractions in the relaxed mesh are naturally matched. We provide an interface tracking method compatible with our reconstruction scheme, where it is granted to use the prior info as an initial guess to capture sub-mesh resolution features. As a result, we are able to treat multiple facets inside a single mixed cell and obtain highly accurate, non-diffusive solution for advection problems with rather coarse meshes. We show our solutions for two-dimensional incompressible flows with two materials with a) the X + O diagonal translation; b) the Zalesak rotational test; and c) the single vortex spiral test.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Mechanical rolling formation of interpenetrated lithium metal/lithium tin alloy foil for ultrahigh-rate battery anode

To achieve good rate capability of lithium metal anodes for high-energy-density batteries, one fundamental challenge is the slow lithium diffusion at the interface. Here we report an interpenetrated, three-dimensional lithium metal/lithium tin alloy nanocomposite foil realized by a simple calendering and folding process of lithium and tin foils, and spontaneous alloying reactions. The strong affinity between the metallic lithium and lithium tin alloy as mixed electronic and ionic conducting networks, and their abundant interfaces enable ultrafast charger diffusion across the entire electrode. Furthermore, we demonstrate that a lithium/lithium tin alloy foil electrode sustains stable lithium stripping/plating under 30 mA cm -2 and 5 mAh cm -2 with a very low overpotential of 20 mV for 200 cycles in a commercial carbonate electrolyte. Cycled under 6 C (6.6 mA cm -2 ), a 1.0 mAh cm -2 LiNi 0.6 Co 0.2 Mn 0.2 O 2 electrode maintains a substantial 74% of its capacity by pairing with such anode.

25 ENERGY STORAGE↗
DOE OSTI2020

Modeling Interfaces to Support Low-Level Waste Disposal System Performance Assessments - 20366

In low-level waste (LLW) disposal sites, interfaces between cementitious materials, used as waste forms and/or engineered barriers, and the surrounding soil or backfill material are often encountered. Reactions across these interfaces may lead to chemical and structural alteration of the cementitious and backfill materials that may ultimately affect long-term performance. For example, the ingress of carbon dioxide from soil gas into a waste tank concrete shell at the Hanford Site or Savannah River Site (SRS) or a low-level waste disposal vault at SRS leads to carbonation of cement hydration products (e.g. portlandite, calcium-silicate hydrate or C-S-H, and ettringite). The result of carbonation is a decrease in pH in the cement paste portion of the tank wall or vault concrete structure that could ultimately lead to de-passivation of the embedded structural steel and, eventually, to cracking. Cracking can lead to increased ingress of water into the structure, corresponding increased release of constituents of concern, and to subsequent increased transport of these constituents to the surrounding environment. The mobility of trace constituents (e.g., radionuclides of concern) in waste forms may increase in response to changes in pH, pore structure, and mineralogical gradients. Depletion of portlandite results in subsequent decalcification of C-S-H that leads to changes in the cement strength and may lead to structural failure. At the boundary between waste forms and concrete vaults, the migration of sulfate ions from the salt waste form (e.g., the saltstone waste form used for LLW disposal at the Savannah River Site in Saltstone Disposal Units, or SDUs) into the barrier or vault concrete has been predicted to result in expansive mineral phase formation (or 'sulfate attack'). Expansive mineral formation could result in cracking and potential loss of structural integrity in the vault concrete. In the performance assessment (PA) for the SRS SDUs, prediction of both the carbonation and sulfate attack fronts are critical to assessing the long-term performance of these LLW disposal vaults. A general purpose geochemical reactive transport model has been developed in LeachXS/ORCHESTRA to evaluate typical interfaces for LLW disposal environments, including SDUs at SRS. The model may be used to predict the long-term performance of interfaces between cementitious materials and saltstone or backfill materials with respect to primary phases by considering mass transport, cement chemistry, geochemical speciation, and multi-ionic diffusion over interfaces between different materials. The present study compares the performance and interactions between vault concrete and saltstone waste form for a representative SDU scenario. The materials were characterized using pH-dependence leaching test (EPA 1313) and semi-dynamic transport tests (EPA 1315) with test results used to parameterize the interface model. The development of a credible inter model provides an important basis for supporting future PAs where carbonation and sulfate attack are important aging and degradation mechanisms. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Synthesis, microstructure and micro-mechanical characterization of metal (Nb, Ti) – MAX phase (Ti 2 AlC) nanolaminates

We utilize elevated temperature physical vapor deposition (PVD) techniques to design metal/MAX multilayered nanocomposite thin films with alternating nanoscale metallic (Nb, Ti) and MAX phase (Ti 2 AlC) layer thicknesses. These metal/MAX nanolaminate architectures attempt to exploit a unique hierarchical topology – as interfaces between the layers are expected to be in direct competition with the internal interfaces within the MAX layers, to drive their tunable macroscopic mechanical behavior. Two metal/MAX nanolaminates – Nb/Ti 2 AlC and Ti/Ti 2 AlC – were deposited. The Nb/Ti 2 AlC metal/MAX system showed highly diffused layer interfaces with distinct Ti – rich and Nb–Al – rich layers, with the presence of MAX phase alongside TiC and other Ti–Al and Nb–Al intermetallic phases. The Nb/Ti 2 AlC system possessed a layered architecture, though the MAX phases were not found to be continuously present in each alternating layer. The second Ti/Ti 2 AlC system showed a non-lamellar nanocomposite microstructure and the formation of mixed Ti n+1 AlC n phases (a mix of n = 1, 2), and no indication of layering. Diffusion occurring between the metal/MAX layers in both cases, likely due to the elevated temperatures during the deposition process, is speculated as the likely cause of these resultant microstructures. The mechanical properties of both systems were evaluated using micromechanical (nanoindentation and micro-pillar compression) techniques, which demonstrated high strengths for both systems (Nb system: yield and instability strengths of 4.88 ± 0.1 GPa and 5.57 ± 0.03 GPa, Ti system: yield and instability strength of 5.61 ± 0.28 GPa and 6.21 ± 0.25 GPa). In conclusion, this work highlights the promising mechanical properties of metal/MAX multilayered depositions and summarizes the challenges in PVD synthesis of metal/MAX multilayered nanolaminates.

MAX phase↗
DOE OSTI2023

The Impact of Circumsolar Diffuse Radiation on the Numerical Computation and Forecasting of DNI

Weather Research and Forecasting model with solar extensions (WRF-Solar) uses the Fast All-sky Radiation Model for Solar applications (FARMS) to predict solar radiation from the forecasted atmospheric gases, aerosols, and clouds. The Beer-Bouguer-Lambert law utilized by FARMS as well as other radiative transfer models assumes Direct Normal Irradiance (DNI) is a narrow beam only covering the sun disk. This assumption is interpreted differently in solar observations by pyrheliometers where the circumsolar diffuse radiation is accounted. This study precisely computes circumsolar diffuse radiation in all-sky conditions using a radiative transfer model based on a parameterization of precomputed cloud transmittance and reflectance. The model is implemented in WRF-Solar to provide day-ahead DNI forecast in the north America. The computation and forecasting of DNI is compared with the Beer-Bouguer-Lambert law to understand the impact of circumsolar diffuse radiation.

aerosols↗
DOE OSTI2024

Morphology selection in dealloying: A phase field study of the coupling among kinetic mechanisms

A phase field model is used to investigate how the corrosion rate and morphology of a dealloying metal is controlled by the kinetic rates of bulk solid diffusion, interfacial diffusivity, and interface dissolution. A specific focus is investigating the manner by which variations in these kinetic parameters synergistically influence the onset of a morphological instability at the solid-liquid interface, which is known to precede rapid dealloying corrosion towards highly topologically complex structures such as bicontinuous porous solids. This work demonstrates that this instability can be suppressed by either an increase of interdiffusion in the solid alloy, or by a decreasing rate of dissolution at the solid-liquid interface. When the instability is suppressed, the result is a relatively planar, passivated dealloying front. Importantly, however, coupled changes in kinetic parameters can also promote the morphological instability and sustain fine-scale ligament and pore formation. Finally, the relevance of the solid-liquid interfacial diffusion for determining the rate of dealloying and ligament formation is highlighted. By elucidating the mechanistic influence of bulk and interfacial kinetic factors on the dealloyed morphology, this work helps to rationalize the contrasting morphologies observed in various dealloying systems.

Diffusion↗
DOE OSTI2025

Sn-InAs Nanowire Shadow-Defined Josephson Junctions

Hybrid superconductor–semiconductor platforms are foundational to advancing quantum information technologies, motivating the integration of materials with clean interfaces, robust superconductivity, and scalable architectures. Here, in this work, we report the synthesis and analysis of inclined InAs nanowires, conformally coated with β-Sn shells. These nanowires extend in opposite in-plane directions, forming a self-aligned, criss-cross network. This enables the deterministic formation of nanowire-shadow Josephson junctions through angle-controlled, low-temperature Sn deposition. Structural characterization shows uniform polycrystalline β-Sn shells forming a sharp, diffusion-free interface with InAs. Low-temperature transport measurements reveal a hard induced superconducting gap ≈ 600 μeV, switching currents up to ≈ 500 nA, and parallel magnetic field resilience beyond 1T. These results establish β-Sn/InAs nanowire networks as a promising platform for superconducting qubits, low-noise microwave devices, and the exploration of exotic superconducting phases including triplet pairing and topological superconductivity.

B-Sn↗
DOE OSTI2022

Chemical Potential Driven Reorganization of Anions between Stern and Diffuse Layers at the Air/Water Interface

We report ion adsorption and transfer at charged interfaces play key roles in various industrial and environmental processes. Molecular scale details of ion-ion, ion-water, and ion-surface interactions are still debated. Complex ions, such as SCN - and SeCN - , are particularly interesting due to their unexpected adsorption trends. Here, we combine vibrational sum frequency generation (VSFG) spectroscopy and surface-sensitive synchrotron X-ray studies to provide a detailed description of SeCN - adsorption at a floating charged monolayer. Polarimetry studies show that the average orientation of SeCN - anions with respect to the surface normal decreases from 45° to 22° with the increasing KSeCN concentration. Interfacial SeCN - coverage saturates at very low bulk concentrations, but their orientational organization, distribution between Stern and diffuse layers, and effects on the hydrogen-bonding network of the interfacial water continue to change with increasing bulk KSeCN concentration. These results show that the increasing chemical potential may lead to further reorganization of the adsorbed ions, even though the total interfacial ion population does not change. The reorganization of the interfacial ions and the water may be very important in chemical separations of heavy metals, where metal-anion complexes drive the selective ion transfer at aqueous interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

In situ synchrotron diffraction and modeling of non-equilibrium solidification of a MnFeCoNiCu alloy

The solidification mechanism and segregation behavior of laser-melted Mn 35 Fe 5 Co 20 Ni 20 Cu 20 was firstly investigated via in situ synchrotron x-ray diffraction at millisecond temporal resolution. The transient composition evolution of the random solid solution during sequential solidification of dendritic and interdendritic regions complicates the analysis of synchrotron diffraction data via any single conventional tool, such as Rietveld refinement. Therefore, a novel approach combining a hard-sphere approximation model, thermodynamic simulation, thermal expansion measurement and microstructural characterization was developed to assist in a fundamental understanding of the evolution of local composition, lattice parameter, and dendrite volume fraction corresponding to the diffraction data. This methodology yields self-consistent results across different methods. Via this approach, four distinct stages were identified, including: (I) FCC dendrite solidification, (II) solidification of FCC interdendritic region, (III) solid-state interdiffusion and (IV) final cooling with marginal diffusion. It was found out that in Stage I, Cu and Mn were rejected into liquid as Mn 35 Fe 5 Co 20 Ni 20 Cu 20 solidified dendritically. During Stage II, the lattice parameter disparity between dendrite and interdendritic region escalated as Cu and Mn continued segregating into the interdendritic region. After complete solidification, during Stage III, the lattice parameter disparity gradually decreases, demonstrating a degree of composition homogenization. The volume fraction of dendrites slightly grew from 58.3 to 65.5%, based on the evolving composition profile across a dendrite/interdendritic interface in diffusion calculations. Postmortem metallography further confirmed that dendrites have a volume fraction of 64.7 ± 5.3% in the final microstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Scanning ultrafast electron microscopy reveals photovoltage dynamics at a deeply buried $p^- \mathrm{Si/SiO_2}$ interface

The understanding and control of charge carrier interactions with defects at buried insulator/semiconductor interfaces is essential for achieving optimum performance in modern electronics. In this work, we report on the use of scanning ultrafast electron microscopy (SUEM) to remotely probe the dynamics of excited carriers at a Si surface buried below a thick thermal oxide. Our measurements illustrate a previously unidentified SUEM contrast mechanism, whereby optical modulation of the space-charge field in the semiconductor modulates the electric field in the thick oxide, thus affecting its secondary electron yield. By analyzing the SUEM contrast as a function of time and laser fluence we demonstrate the diffusion mediated capture of excited carriers by interfacial traps.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Antiferromagnetic Fe Te 2 1 T - phase formation at the Sb 2 Te 3 / Ni 80 Fe 20 interface

Bilayer topological insulator/ferromagnet (TI/FM) heterostructures are promising for spintronic applications due to their low switching energy and therefore power efficiency. Until recently, the reactivity of TI with FM films was overlooked in the spin orbit-torque literature, even though there are reports that it is energetically favorable for TIs to react with transition metals and form interfacial layers. Here, in this study we fabricated a TI/FM heterostructure comprised of molecular beam epitaxy grown Sb 2 Te 3 and DC sputtered Ni 80 Fe 20 . Broadband ferromagnetic resonance revealed spin-pumping evident by the significant enhancement in Gilbert damping, which is likely a signature of the topological surface states or the presence of large spin-orbit-coupling in the adjacent Sb 2 Te 3 . With low-temperature magnetometry, an exchange bias is observed which indicates an exchange interaction between an antiferromagnet (AFM) and an adjacent FM. Cross-section high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) characterization of the Sb 2 Te 3 - Ni 80 Fe 20 bilayer revealed a complex interface showing diffusion of Fe and Ni into the Sb 2 Te 3 film yielding the formation of a FeTe 2 1T-type structural phase. Furthermore, density functional theory calculations revealed that the FeTe 2 1T-phase has an AFM ground state. Due to experimental limitations in the electron energy loss spectroscopy measurements precise chemistry of the interfacial phase could not be determined, therefore it is possible that the FeTe 2 1T and/or an intermixed (Fe 1-x Ni x )Te 2 1T is the AFM interfacial phase contributing to exchange bias in the system. This work emphasizes the chemical complexity of TI/FM interfaces that host novel, metastable magnetic topological phases and require more in-depth studies of other similar interfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Overcoming Anode Instability in Solid‐State Batteries through Control of the Lithium Metal Microstructure

Abstract Enabling the lithium metal anode (LMA) in solid‐state batteries (SSBs) is the key to developing high energy density battery technologies. However, maintaining a stable electrode–electrolyte interface presents a critical challenge to high cycling rate and prolonged cycle life. One such issue is the interfacial pore formation in LMA during stripping. To overcome this, either higher stack pressure or binary lithium alloy anodes are used. Herein, it is shown that fine‐grained ( d = 20 µm) polycrystalline LMA can avoid pore formation by exploiting the microstructural dependence of the creep rates. In a symmetric cell set‐up, i.e., LiǀLi 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO)ǀLi, fine‐grained LMA achieves > 11.0 mAh cm −2 compared to ≈ 3.6 mAh cm −2 for coarse‐grained LMA ( d = 295 µm) at 0.1 mA cm −2 and at moderate stress of 2.0 MPa. Smaller diffusion lengths (≈ 20 µm) and higher diffusivity pathway along dislocations ( D d ≈ 10 −7 cm 2 s −1 ), generated during cell fabrication, result in enhanced viscoplastic deformation in fine‐grained polycrystalline LMA. The electrochemical performances corroborate well with estimated creep rates. Thus, microstructural control of LMA can significantly reduce the required stack pressure during stripping. These results are particularly relevant for “anode‐free” SSBs wherein both the microstructure and the mechanical state of the lithium are critical parameters.

25 ENERGY STORAGE↗
DOE OSTI2022

Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries

The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni 2 P electrocatalyst supported on N, P co-doped graphene (Ni 2 P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni 2 P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li 2 S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni 2 P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm –2 , the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗