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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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Machine Learning Reveals the Critical Interactions for SARS-CoV-2 Spike Protein Binding to ACE2
SARS-CoV and SARS-CoV-2 bind to the human ACE2 receptor in practically identical conformations, although several residues of the receptor-binding domain (RBD) differ between them. Herein, we have used molecular dynamics (MD) simulations, machine learning (ML), and free-energy perturbation (FEP) calculations to elucidate the differences in binding by the two viruses. Although only subtle differences were observed from the initial MD simulations of the two RBD–ACE2 complexes, ML identified the individual residues with the most distinctive ACE2 interactions, many of which have been highlighted in previous experimental studies. FEP calculations quantified the corresponding differences in binding free energies to ACE2, and examination of MD trajectories provided structural explanations for these differences. Lastly, the energetics of emerging SARS-CoV-2 mutations were studied, showing that the affinity of the RBD for ACE2 is increased by N501Y and E484K mutations but is slightly decreased by K417N.
Characterizing Hydrated Polymers via Dielectric Relaxation Spectroscopy: Connecting Relative Permittivity, State of Water, and Salt Transport Properties of Sulfonated Polysulfones
Sulfonated polysulfone is a promising membrane material for separation and energy generation processes that rely on membranes to control the rates of small-molecule (e.g., water and ions) transport. The interactions among water molecules, ions, and the sulfonate groups in these polymers play a key role in controlling these rates of transport, but much remains unknown about these fundamental interactions in sulfonated polymers. In this study, we used dielectric relaxation spectroscopy to characterize water molecule dynamics in sulfonated polysulfone and Nafion. We found that the charged sulfonate groups contribute to a restriction of water molecule dynamics (i.e., a reduction in the characteristic time scale of dipolar motions) in a manner that is governed by the concentration and nature (i.e., conjugate base strength) of the sulfonate group. Additionally, we develop strategies to use these data to aid in modeling ion transport in sulfonated polysulfone. These results may be useful to guide engineering strategies for polymeric membranes.
Microwave-Absorbing Foams with Adjustable Absorption Frequency and Structural Coloration
Microwave-absorbing materials with regulatable absorption frequency and optical camouflage hold great significance in intelligent electronic devices and advanced stealth technology. Herein, we present an innovative microwave-absorbing foam that can dynamically tune microwave absorption frequencies via a simple mechanical compression while in parallel enabling optical camouflage over broad spectral ranges by adjusting the structural colors. In this study, the vivid colors spanning different color categories generated from thin-film interference can be precisely regulated by adjusting the thickness of the conformal TiO 2 coatings on Ni/melamine foam. Enhanced interfacial and defect-induced polarizations resulting from the introduction of TiO 2 coating synergistically contribute to the dielectric attenuation performance. Consequently, such a foam exhibits exceptional microwave absorption capabilities, and the absorption frequency can be dynamically tuned from the S band to the Ku band by manipulating its compression ratio. Additionally, simulation calculations validate the adjustable electromagnetic wave loss behavior, offering valuable insights for the development of next-generation intelligent electromagnetic devices across diverse fields.
Electrical Detection of Single-Domain Néel Vector Reorientation across the Spin–Flop Transition in Cr 2 O 3 Crystals
Electrical transport measurements in heterostructures of antiferromagnetic Cr 2 O 3 bulk crystals and a thin Pt layer exhibit sharp responses as the Néel vector of Cr 2 O 3 undergoes the spin−flop transition. This abrupt change can arise from several distinct mechanisms including magnetostriction, proximity-induced anomalous Hall, spin Hall anomalous Hall, and spin Hall planar Hall effects. While large Pt devices sensing multiple up/ down domains can produce indistinguishable Hall signal jumps due to different initial Néel vector orientations, smaller Pt devices that sense single domains isolate the proximity-induced Hall signals. This allows direct electrical detection of Néel vector reorientation across the spin−flop transition in single-domain regions. Furthermore, the single-domain state can be prepared by magnetic field cooling or magnetoelectric cooling. We demonstrate a method to control and characterize the three-dimensional orientation of single-domain Néel vectors by exploiting Hall measurements and cooling techniques, crucial for future antiferromagnetic spintronic applications.
Localized Orbital Excitation Drives Bond Formation in Plasmonic Catalysis
Localized surface plasmons generated on metallic nanostructures can be used to accelerate molecular transformations; however, the efficiency is limited by the challenge to control the energy/charge transfer at the interfaces. Here, we combine density functional theory (DFT) calculations and experiments to reveal the mechanism of nitrophenol reduction on Au nanoparticles under visible-light irradiation and propose a strategy to further enhance the reaction rates. DFT calculations show a reduced activation barrier under electronic excitation on Au(111), thus explaining the measured higher rates under visible-light irradiation. Furthermore, we propose a heterostructure with Au nanoparticles covered by a thin film of hexagonal boron nitride; the latter is used to decouple the molecular orbitals from the metal to enable charge localization in the molecule. DFT calculations show that, by this electronic decoupling, the activation barrier can be lowered by a factor of five. Furthermore, this work thus provides a valuable strategy for optimizing catalytic efficiency.
Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride
It is well established that hydrogen binding energy (HBE) is a key descriptor for hydrogen evolution reaction (HER) activity, and such a relationship is a useful tool for searching efficient and cost-effective HER catalysts. However, in almost all cases, the HBE values are obtained from density functional theory (DFT) calculations. Here in this study, temperature programmed desorption (TPD) was used to experimentally determine the HBE values of metal monolayers supported on molybdenum nitride (Mo 2 N), and electrochemical measurements were performed on the same surfaces. Combined DFT and kinetic Monte Carlo (kMC) simulations were used to validate the trend observed with TPD and the electrochemical HER activity. Depositing one monolayer of Pt on Mo 2 N led to similar HBE values seen for bulk Pt, and electrochemical measurements showed that monolayer Pt on Mo 2 N had similar HER activity to that of bulk Pt. Similar studies were also performed for monolayer Pd on Mo 2 N to confirm the correlation. This work also demonstrates that Mo 2 N is a promising support to reduce precious metal loading in HER catalysts.
Enhancing Acidic Oxygen Evolution Activity by Supporting Iridium Electrocatalysts on Tantalum Carbide
For a high-performance proton exchange membrane water electrolyzer (PEMWE), acidic oxygen evolution reaction (OER) electrocatalysts require highly dispersed iridium oxide (IrO x ) nanoparticles. Although carbon-based materials have been explored as promising supports for IrO x nanoparticles, their limited stability under harsh oxidative and acidic PEMWE conditions remains a significant challenge. Here, in this study, we report the synthesis and in situ characterization of active and durable IrOx electrocatalysts supported on electrochemically stable and electrically conducting tantalum carbide (TaC). When applied in a PEMWE, the IrO x /TaC electrocatalyst achieves a cell voltage of 1.71 V at 1.0 A cm –2 , outperforming the commercial IrO 2 catalyst (1.82 V at 1.0 A cm –2 ). Furthermore, the IrO x /TaC catalyst maintains a stable operation for 200 h at 0.5 A cm –2 with a low degradation rate of 36 μV h –1 . Density functional theory calculations further confirm that Ir–O–Ta bond formation at the IrO x /TaC interface reduces the overpotential of the OER compared to IrO 2 . This study underscores the pivotal role of supporting IrO x over stable and conducting metal carbides, providing guidance for the design of advanced acidic OER catalysts.
Iridium Oxide Supported on Bimetallic Nitrides as Anodic Catalysts in Acidic and Seawater Environments
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Membranes for Lithium Recovery From Conventional and Unconventional Sources
Lithium has been deemed a critical mineral of national importance that finds uses in a wide range of applications, and its demand has been rising significantly in recent years. The urgency of meeting this demand requires lithium extraction from various aqueous sources such as continental brines, geothermal brines, seawater, produced water, and battery waste. While direct lithium extraction (DLE) technologies such as adsorption, ion exchange, and solvent extraction have emerged as possible solutions, membrane technologies are also being investigated for various sources and at different stages of the recovery process. Here, we analyze the application of membranes for pretreatment of lithium source waters, bring management, lithium/magnesium separation, lithium/sodium separation, and lithium hydroxide conversion, and evaluate performance metrics for critical lithium separations from the literature. We explore the potential of membranes at every stage of the recovery process and describe their current status and future prospects. We describe hypothetical process trains with integrated membrane technologies for each source type and address their feasibility and challenges. The potential energy and water impacts of membrane-integrated and conventional DLE processes are also critically considered alongside performance and selectivity metrics, and this is illustrated using examples and calculated from published technical reports. This paper thus provides a comprehensive overview of the application of membranes along every stage of the lithium recovery process, emphasizing the versatility and potential of membrane technologies for critical mineral recovery.
Scalable Advanced Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 Cathode Materials from a Slug Flow Continuous Process
Not Available
Pretreatment with Sodium Methyl Mercaptide Increases Carbohydrate Yield during Kraft Pulping
Kraft pulping is the predominant technology in the pulp and paper industry for removing lignin from wood carbohydrates to produce paper, board, packaging, tissue, and specialty cellulose. However, the kraft process is energy intensive and expensive, and its yield is limited by the degradation of carbohydrates. Pretreatment can increase carbohydrate yield by limiting degradation via primary peeling of reducing end groups. However, protection of galactoglucomannan (GGM), the primary hemicellulose component of softwood, is minimal when conventional pretreatments are used. Here, we investigated the effectiveness of sodium methyl mercaptide pretreatment on southern pine wood chips under a range of experimental conditions. We found that pretreatment of biomass with 4.38% sodium methyl mercaptide at pH 12 and 105 °C for 60 min provided small but significant increases in xylan and cellulose yields relative to control conditions, but preservation of GGM was minimal. Furthermore, to provide insight into molecular-scale details of primary peeling, pretreatment, and alkaline hydrolysis, we performed classical molecular dynamics (MD) simulations under selected process conditions and quantum mechanical (QM) calculations of selected reactions. MD simulations showed that C1 of the GGM reducing end is more readily accessible by HO – and CH 3 S – ions than in cellulose. The free energy barrier for peeling calculated with QM is lower for GGM than for cellulose, indicating increased susceptibility to peeling. In addition, we found that GGM may be more susceptible to internal chain cleavage than cellulose. Thus, even though reducing end groups may be protected initially through pretreatment, new unprotected reducing end groups may be generated through alkaline hydrolysis. Taken together, these findings show the promise of methyl mercaptide as a pretreatment technology for cellulose retention and also provide molecular insight for improving its effectiveness toward GGM.
Theoretical Prediction and Experimental Verification of IrO x Supported on Titanium Nitride for Acidic Oxygen Evolution Reaction
Reducing iridium (Ir) catalyst loading for acidic oxygen evolution reaction (OER) is a critical strategy for large-scale hydrogen production via proton exchange membrane (PEM) water electrolysis. However, simultaneously achieving high activity, long-term stability, and reduced material cost remains challenging. To address this challenge, we develop a frame-work by combining density functional theory (DFT) prediction using model surfaces and proof-of-concept experimental ver-ification using thin films and nanoparticles. DFT results predict that oxidized Ir monolayers over titanium nitride (IrO x /TiN) should display higher OER activity than IrO x while reducing Ir loading. Further, this prediction is verified by depositing Ir monolayers over TiN thin films via physical vapor deposition. The promising thin film results are then extended to commercially viable powder IrO x /TiN catalysts, which demonstrate a lower overpotential and higher mass activity than commercial IrO 2 , and a long-term stability of 250 hours to maintain a current density of 10 mA cm -2 . The superior OER performance of IrO x /TiN is further confirmed using proton exchange membrane water electrolyzer (PEMWE), which shows a lower cell voltage than commercial IrO 2 to achieve a current density of 1 A cm -2 . Both DFT and in situ X-ray absorption spectroscopy reveal that the high OER performance of IrO x /TiN strongly depends on the IrO x - TiN interaction via direct Ir-Ti bonding. This study highlights the importance of close interaction between theoretical prediction based on mechanistic understanding and experimental verification based on thin film model catalysts to facilitate the development of more practical powder IrO x /TiN catalysts with high activity and stability for acidic OER.
Controlling Reaction Pathways of Ethylene Hydroformylation Using Isolated Bimetallic Rhodium–Cobalt Sites
Designing efficient ligand-free heterogeneous catalysts for ethylene hydroformylation to produce C 3 oxygenates is of importance for both fundamental research and practical applications, but it is often hindered by insufficient catalytic activity and selectivity. Here, this work designs isolated rhodium–cobalt (Rh–Co) sites confined within a ZSM-5 zeolite to enhance ethylene hydroformylation rates and selectivity while maintaining catalyst stability. By adjusting the Co/Al ratio in Co-ZSM-5, different sizes of Co are formed; subsequent Rh introduction produces isolated Rh 1 Co x clusters with different Rh–Co coordination numbers (CNs). In-situ characterizations and density functional theory calculations reveal that a Rh–Co CN of 3, corresponding to an isolated Rh 1 Co 3 site, provides optimal bindings to reaction intermediates and thus achieves the highest hydroformylation rates among supported Rh-based catalysts. This study demonstrates the role of coordination-tuning via a secondary metal in effectively controlling the reaction pathway over single Rh atom catalysts.