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At least 469 records · Page 26

Floatable Protective Layers: a Strategy to Minimize Solid Electrolyte Interphase Growth and Maximize the Lithium Utilization

Abstract Maximizing lithium (Li) utilization is crucial for enhancing the long‐term stability of Li‐based batteries. In anode‐free Li batteries (AFLBs), although the initial formation of solid electrolyte interphase (SEI) is beneficial on limiting further reaction between Li and electrolyte, large volume change of Li metal anode (LMA) during cycling often leads to continuous breakdown and re‐formation of SEI and formation of inactive Li, hindering its efficiency. In this study, a novel strategy is presented to protect Li metal by applying a floatable protection layer (FPL) on a copper substrate, enabling large Li particles to be primarily deposited below FPL, but SEI to be primarily formed above FPL. This approach effectively minimizes the direct contact between electrolyte and freshly deposited Li, therefore mitigating the continuous side reactions and early failure of AFLBs. As a result, Li consumption is minimized, and the overall stability of the battery is significantly enhanced. Further development of this approach can also be used to improve the performance of other Li‐based batteries for large‐scale applications.

Lim, Hyung‐Seok [Energy and Environment Directorat↗

Summertime Marine Boundary Layer Cloud, Thermodynamic, and Drizzle Morphology over the Eastern North Atlantic: A Four-Year Study

Abstract Summertime remote sensor and in situ data from 2016 to 2019 collected at the ARM Eastern North Atlantic (ENA) Observatory are combined with aircraft measurements from the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign to quantify marine boundary layer (MBL) cloud, thermodynamic, and drizzle morphology in the region. A radar reflectivity–rainfall rate relationship ( Z – R ) is developed from aircraft data and 6-h cloud morphological regimes are identified from ENA data using a k -means algorithm driven by three independent inputs quantifying cloud thickness, drizzle intensity, and cloud field geometric complexity. Four separate MBL structural regimes representing non- or weakly drizzling single-layer stratocumulus, drizzling stratocumulus and cumulus-coupled stratocumulus, deep convection, and broken clouds embedded in northerly flow are identified. Single-layer stratocumulus is indicated when weak subtropical anticyclones are significantly west of the ENA site, and the MBL is cooler and drier than when drizzling and cumulus-coupled stratocumulus and broken clouds are observed. Drizzling and cumulus-coupled stratocumulus clouds are observed on the eastern flank of strong subtropical anticyclones in deep warm moist air masses with wind speeds exceeding 7 m s −1 and strong near-surface wind shear. Broken clouds exhibit strong wind shear near the inversion, while single-layer stratocumulus clouds have lower wind speeds and minimal shear. Net latent heat fluxes in the subcloud layer resulting from a combination of the ocean surface heat flux and evaporating drizzle average near zero over long periods in drizzling and cumulus-coupled stratocumulus. The ECMWF reanalysis version 5 (ERA5) is found to accurately represent single-layer stratocumulus properties, while producing significant discrepancies when drizzling stratocumulus and cumulus-coupled stratocumulus are observed.

54 ENVIRONMENTAL SCIENCES↗

Dual‐Gradient Construction on Li‐Rich Cathodes for High Stability Lithium Battery

Abstract The practical applications of high‐energy Li‐rich layered oxides (LLOs) have been hindered by the severe performance degradation including voltage decay and capacity fading. The gradient construction toward high‐activity interior and high‐stability exterior, typically realized by gradually changed transition metal (TM) gradient in LLOs, can alleviate the performance degradation to certain degrees. In this study, a gradient design of Al/Mg dopants is demonstrated for the TM‐gradient LLOs to further harmonize the high‐activity interior and high‐stability exterior, thereby forming the dual (TM and doping) gradient. As a result, superior capacity retention of 86% and a minor voltage decay of 0.54 mV cycle −1 are achieved at 1 C after 300 cycles. The improved electrochemical stability of the dual‐gradient LLO is attributed to the enhanced surface stability and suppressed bulk structure degeneration of LLOs upon electrochemical cycling. The dual‐gradient design serves as an important approach to fabricate high‐performance bulk LLOs toward applications.

Wu, Tianhao↗

Investigation of Coupled Processes in Fractures and the Bordering Matrix via a Micro‐Continuum Reactive Transport Model

Abstract In multi‐mineral fractured rocks, the altered porous layer on the fracture surface resulting from preferential dissolution of the fast‐reacting minerals can have profound impacts on subsequent chemical‐physical alteration of the fractures. This study adopts the micro‐continuum approach to provide further understanding of reactive transport processes in the altered layer (AL), and mass exchanges with the bordering matrix and fracture. The modeling framework couples the Darcy‐Brinkman‐Stokes (DBS) solver in COMSOL Multiphysics and the geochemical modeling capability of CrunchFlow. Three‐dimensional steady state simulations with systematically varied chemical‐physical parameters of the AL were performed to examine the impacts of individual factors and processes. Our simulation results confirm previous observations that dissolution of the fast‐reacting mineral (i.e., calcite) is largely controlled by diffusion across the AL. We also show that dissolution of the slow‐reacting mineral (i.e., dolomite), which controls AL development and fracture enlargement, increases with surface area and has a complex dependence on different local rate‐limiting processes. In particular, advection can result in evident spatial variations in the local dissolution rates of dolomite, although it does not affect the bulk chemistry significantly. The difference in the spatial patterns between simulations with and without advection in the AL is more noticeable in the locations with smaller apertures, with up to 20% difference in local reaction rates. Therefore, it is important to include a full depiction of advection, diffusion, and reactions for accurately capturing local dynamics that control long‐term fracture evolution.

58 GEOSCIENCES↗

Predicting the Evolution of Shallow Cumulus Clouds With a Lotka‐Volterra Like Model

Abstract In numerical weather prediction and climate models, boundary‐layer clouds are controlled by a wide range of subgrid‐scale processes. However, understanding the nature of these processes and their role in the evolution of the cloud size distribution as a whole has been elusive. To address this issue, we adopt a novel empirical framework from the field of population dynamics to model the evolution of cloud size statistics by using the shallow cumulus properties obtained from a large‐eddy simulation (LES). Our approach involves representing the cloud size distribution and the total cloud area using a revised Lotka‐Volterra model and ridge linear model, respectively. The physical interpretation of the total cloud area and coefficients obtained from the optimization of the models reveals three stages probably interpreted by dominant processes: the formation of new clouds, the growth of single clouds, and a steady state with organized transitions involving the growth and decay of multiple clouds. Furthermore, we showcase the potential of this framework to serve as a component of scale‐aware parameterizations of shallow‐convective clouds in atmospheric models.

54 ENVIRONMENTAL SCIENCES↗

Extensive hydrogen incorporation is not necessary for superconductivity in topotactically reduced nickelates

Abstract A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phaseviaa topotactic reaction with a strongly reducing agent such as CaH 2 . Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La 1−x X x NiO 2 / SrTiO 3 (X= Ca and Sr) and Nd 6 Ni 5 O 12 / NdGaO 3 films, along with non-superconducting NdNiO 2 / SrTiO 3 and (Nd,Sr)NiO 2 / SrTiO 3 . We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that extensive hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates.

Science & Technology - Other Topics↗

Nanoporous gold nanoleaf as tunable metamaterial

Abstract We have studied optical properties of single-layer and multi-fold nanoporous gold leaf (NPGL) metamaterials and observed highly unusual transmission spectra composed of two well-resolved peaks. We explain this phenomenon in terms of a surface plasmon absorption band positioned on the top of a broader transmission band, the latter being characteristic of both homogeneous “solid” and inhomogeneous “diluted” Au films. The transmission spectra of NPGL metamaterials were shown to be controlled by external dielectric environments, e.g. water and applied voltage in an electrochemical cell. This paves the road to numerous functionalities of the studied tunable and active metamaterials, including control of spontaneous emission, energy transfer and many others.

36 MATERIALS SCIENCE↗

An outlook into the flat land of 2D materials beyond graphene: synthesis, properties and device applications

Abstract The field of two-dimensional (2D) and layered materials continues to excite many researchers around the world who are eager to advance and innovate viable routes for large scale synthesis, doping and integration of monolayers and the development of unique characterization approaches for studying and harnessing exotic properties that will enable novel device applications. There has been a large interest in 2D materials beyond graphene, with particular emphasis on monoelemental materials (phosphorene, silicene, tellurene, etc. ), 2D compounds (MXenes, oxides, nitrides, carbides and chalcogenides), their alloys and layered van der Waals heterostructures. This is not only indicated by the significant increase in the number of peer reviewed publications each year in this area of research, but also by the surging number of conference sessions focusing on 2D materials beyond graphene. This Perspective article highlights some of the recent advances in the field from a diverse international community of theoretical and experimental researchers who participated in the symposium ‘Beyond Graphene 2D Materials—Synthesis, Properties and Device Applications’ at the Materials Research Society (MRS) Fall 2019 meeting.

McCreary, Amber (ORCID:0000000299885800)↗

Minnowbrook I: 1993 Workshop on End-Stage Boundary Layer Transition

This volume contains materials presented at the Minnowbrook I-1993 Workshop on End-Stage Boundary Layer Transition, held at the Syracuse University Minnowbrook Conference Center, New York, from August 15 to 18, 1993. This volume was previously published as a Syracuse University report edited by John E. LaGraff. The workshop organizers were John E. LaGraff (Syracuse University), Terry V. Jones (Oxford University), and J. Paul Gostelow (University of Technology, Sydney). The workshop focused on physical understanding of the late stages of transition from laminar to turbulent flows, with the specific goal of contributing to improving engineering design of turbomachinery and wing airfoils. The workshop participants included academic researchers from the United States and abroad, and representatives from the gas-turbine industry and U.S. government laboratories. To improve interaction and discussions among the participants, no formal papers were required. The physical mechanisms discussed were related to natural and bypass transition, wake-induced transition, effects of freestream turbulence, turbulent spots, hairpin vortices, nonlinear instabilities and breakdown, instability wave interactions, intermittency, turbulence, numerical simulation and modeling of transition, heat transfer in boundary-layer transition, transition in separated flows, laminarization, transition in turbomachinery compressors and turbines, hypersonic boundary-layer transition, and other related topics. This volume contains abstracts and copies of the viewgraphs presented, organized according to the workshop sessions. The workshop summary and the plenary discussion transcript clearly outline future research needs.

LaGraff, John E.↗

Superposition of intra- and inter-layer excitons in twistronic MoSe 2 /WSe 2 bilayers probed by resonant Raman scattering

Abstract Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe 2 /WSe 2 heterostructures, strong hybridization of both single particle and excitonic states can occur via single particle tunnelling. Here we use resonance Raman scattering to provide direct evidence for the hybridisation of excitons in twistronic MoSe 2 /WSe 2 structures, by observing scattering of specific excitons by phonons in both WSe 2 and MoSe 2 . We also demonstrate that resonance Raman scattering spectroscopy opens up a wide range of possibilities for quantifying the layer composition of the superposition states of the exciton and the interlayer hybridisation parameters in heterostructures of two-dimensional materials.

Materials Science↗