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At least 1,315 records · Page 73

AugerPrime surface detector electronics

Operating since 2004, the Pierre Auger Observatory has led to major advances in our understanding of the ultra-high-energy cosmic rays. The latest findings have revealed new insights that led to the upgrade of the Observatory, with the primary goal of obtaining information on the primary mass of the most energetic cosmic rays on a shower-by-shower basis. In the framework of the upgrade, called AugerPrime, the 1660 water-Cherenkov detectors of the surface array are equipped with plastic scintillators and radio antennas, allowing us to enhance the composition sensitivity. To accommodate new detectors and to increase experimental capabilities, the electronics is also upgraded. This includes better timing with up-to-date GPS receivers, higher sampling frequency, increased dynamic range, and more powerful local processing of the data. In this paper, the design characteristics of the new electronics and the enhanced dynamic range will be described. The manufacturing and test processes will be outlined and the test results will be discussed. The calibration of the SD detector and various performance parameters obtained from the analysis of the first commissioning data will also be presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Aqueous Polymer Modification of Cellulose Nanofibrils by Grafting‐Through a Reactive Methacrylate Group

Abstract Modifying the surface of cellulose nanofibrils (CNFs) produced by mechanical refinement with a variety of polymer functional groups in an entirely water‐based system is challenging because only surface hydroxyl groups are accessible. To address this limitation, an entirely water‐based, polymer modification scheme is developed. CNFs are functionalized with a reactive methacrylate functional group followed by subsequent grafting‐through polymerization. This modification worked with a variety of water‐soluble and water‐insoluble (meth)acrylates and (meth)acrylamides, grafting up to 45 wt% polymer on to the CNFs. The reaction conditions introducing the methacrylate functional group are adjusted to vary the degree of functionality. Soxhlet extraction of modified samples demonstrates that the reactive methacrylate group is necessary to facilitate polymer grafting. The degree of functionalization of the polymers is studied via quantitative transmission IR spectroscopy and the morphology of the resulting cellulose nanofibrils is studied via a combination of optical, scanning electron, and atomic force microscopy. High levels of polymer modification do not significantly affect the micrometer‐scale fibril morphology.

Kelly, Peter V.↗

Hybridizing Machine Learning and Physically-based Earth System Models to Improve Prediction of Multivariate Extreme Events (AI Exploration of Wildland Fire Prediction)

Focal Areas: This project responds to two focal areas identified in the DOE Call for AI4ESP White Papers: 1) Predictive modeling through the use of artificial intelligence (AI) techniques, and 2) insights gleaned from complex data using explainable AI and big data analytics. Science Challenge: Large wildland fires (hereafter wildfires) appearing as high-impact compound climate extreme events are closely related to hydroclimate and water cycle extremes that modulate surface fuel supply and combustibility. These compound events have multivariate climatic features (e.g., temperature, precipitation, relative humidity, wind, lightning) and societal drivers (e.g., forest management, land use change, human caused ignitions). Meanwhile, they induce strong feedbacks to the coupled atmosphere, biosphere, and hydrosphere by perturbing regional and global radiation budget as well as ecological, biogeochemical, and water cycles across multiple spatiotemporal scales. The nonlinear interactions between these natural and anthropogenic components of the Earth system are too complex to be completely and adequately represented in today’s Earth system models (ESMs). The inherent stochastic nature of fire activity at all scales further increases the difficulty of its prediction using ESMs that are usually developed from deterministic equations and parameterizations. Besides, concurrence of long-term (decadal to interdecadal) global climate change and fire regime shifts overlapping with short-term (intraseasonal to interannual) variations of regional fire weather and burning activity confound predictability of these compound extreme events. We propose to address the above scientific challenges by using machine learning (ML)-based data-driven modeling techniques to integrate observations and physically-based ESMs’ simulations in a computationally efficient hybrid prediction system. This prediction system is supposed to characterize the wildfire’s sensitivity to climate and exogenous drivers at high resolution (~ 0.25°) on subseasonal to seasonal (S2S) timescales providing improved predictability and explainability. We will use the system to help identify: (1) What are the computational elements of a hybrid system needed to predict compound climate extreme events such as global wildfires? (2) What are the key drivers (either natural or anthropogenic) that modulate short-term variations of multivariate fire weather and burning activity over different regions? How can one take advantage of those driver-response relationships to improve the predictability of large wildfires on S2S time scales? (3) What are the underlying physical mechanisms and sources of improved predictability? Which ML techniques are optimal in revealing and adapting these mechanisms?

54 ENVIRONMENTAL SCIENCES↗

Hinderance of C-S-H sheet piling during first drying using a shrinkage reducing agent: A SAXS study

The role of a shrinkage reducing agent (SRA) in the hardened cement paste during a first desorption process was investigated by measuring the small-angle X-ray scattering (SAXS). Fractal disc analysis and Guinier approximation were adopted to interpret the SAXS profiles. We experimentally confirmed that the presence of SRA molecules mitigated the piling of calcium-silicate hydrate (C-S-H) sheets, which could be monitored by the increase in the thickness of the disc, representing the agglomeration of C-S-H sheets. In addition, the basal spacing of C-S-H did not change during the drying. By contrast, the diameter of the discs monotonically decreased and showed a similar trend to that of samples lacking SRA. Based on these findings, we concluded that SRA molecules were on the surface of the C-S-H sheets and mitigated the piling, facilitating water removal from the C-S-H agglomeration in the RH range of 80–40%.

36 MATERIALS SCIENCE↗

Interfacial Ice Density Fluctuations Inform Surface Ice-Philicity

The propensity of a surface to nucleate ice or bind to ice is governed by its ice-philicity─its relative preference for ice over liquid water. However, the relationship between the features of a surface and its ice-philicity is not well understood, and for surfaces with chemical or topographical heterogeneity, such as proteins, their ice-philicity is not even well-defined. In the analogous problem of surface hydrophobicity, it has been shown that hydrophobic surfaces display enhanced low water-density (vapor-like) fluctuations in their vicinity. To interrogate whether enhanced ice-like fluctuations are similarly observed near ice-philic surfaces, here we use molecular simulations and enhanced sampling techniques. Using a family of model surfaces for which the wetting coefficient, k , has previously been characterized, we show that the free energy of observing rare interfacial ice-density fluctuations decreases monotonically with increasing k . By utilizing this connection, we investigate a set of fcc systems and find that the (110) surface is more ice-philic than the (111) or (100) surfaces. By additionally analyzing the structure of interfacial ice, we find that all surfaces prefer to bind to the basal plane of ice, and the topographical complementarity of the (110) surface to the basal plane explains its higher ice-philicity. Using enhanced interfacial ice-like fluctuations as a measure of surface ice-philicity, we then characterize the ice-philicity of chemically heterogeneous and topologically complex systems. In particular, we study the spruce budworm antifreeze protein (sbwAFP), which binds to ice using a known ice-binding site (IBS) and resists engulfment using nonbinding sites of the protein (NBSs). We find that the IBS displays enhanced interfacial ice-density fluctuations and is therefore more ice-philic than the two NBSs studied. We also find the two NBSs are similarly ice-phobic. By establishing a connection between interfacial ice-like fluctuations and surface ice-philicity, our findings thus provide a way to characterize the ice-philicity of heterogeneous surfaces.

crystals↗

L-Basin microbial monitoring program - evaluation of 20 years of monitoring

This report summarizes the results from over 20-years’ of activities for microbial monitoring of the bulk water, floc analysis, and test coupon surfaces for the Savannah River Site L Basin. The Microbial Monitoring Program provides important information for the characterization of overall water quality as it impacts the continued safe storage of spent nuclear fuel in L Basin. The potential impacts to fuel storage are: 1) microbial-influenced corrosion of the fuel; and 2) biofouling of the fuel storage systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Experimental investigation into coal wettability changes caused by reactions with scCO 2 -H 2 O

Geological CO 2 sequestration (GCS) can help mitigate global warming and enhance methane recovery from coal beds. However, few studies have linked the effects of CO 2 to surface chemistry changes controlling wetting behavior in deep coal beds. Contact angles (CAs) of CO 2 /N 2 -high volatile bituminous coal-water systems were measured under different temperatures and pressures. The surface chemistry and physical structure of coals were characterized to investigate changes in physicochemical properties and their relations with wettability after reactions. For N 2 treatment, the time-dependence of static and dynamic CAs were insignificant, ranging within 4°. For gaseous CO 2 treatment, the static CAs and the average advancing angles increased slightly. With supercritical (sc) CO 2 , both the static and dynamic CAs increased significantly, and θ adv changed to intermediate-wet (92°). Reactions with minerals exposed to scCO 2 resulted in greater surface roughness and heterogeneity, greater contact angle hysteresis and more surface sites occupied by scCO 2 rather than H 2 O. Increases in hydrophobic functional groups and decreases in hydrophilicity were shown by FTIR spectra, reflecting the shedding of polar oxygen-containing functional groups, reduction of hydrogen bonds, and increasing percentage of hydrocarbons. XRD patterns obtained following scCO 2 -treatment showed that crystallite growth and molecular polymerization were higher toward graphite-like. The calculated structural parameters of functional groups and crystallites both showed elevated coal rank. Changes in crystallite structure, notably higher carbon content and decreased negative surface charge, are unfavorable for water-wetting. Finally, this study contributes to understanding surface chemistry changes responsible for decreased wettability during CO 2 -enhanced coal bed methane recovery and GCS in coal reservoirs.

01 COAL, LIGNITE, AND PEAT↗

pH-Driven Restructuring of Hydration Layers and Cation Adsorption at the Alumina–Water Interface

Oxide−water interfaces underpin ion separations, catalysis, and electrochemical energy technologies, where the electrical double layer (EDL) controls adsorption, transport, and reactivity. However, the molecular-scale links between pHdependent surface protonation, hydration-layer structure, and counterion adsorption remain poorly defined. Here, we combine in situ crystal truncation rod (CTR) and resonant anomalous X-ray reflectivity (RAXR) with streaming potential measurements and ab initio molecular dynamics (AIMD) simulations to resolve the chemical and structural evolution of the EDL at the single-crystal alumina (012)−water interface in 10 mM Rb + over pH 3−12. CTR measurements reveal two distinct adsorbed water layers at ∼2.2 and ∼3.5 Å above the surface. Each water layer shifts toward the substrate at transition pHs near 6.5 and 10.6, respectively, reflecting changes in primary hydration layer structure in response to the deprotonation of bridging and terminal aluminol groups. RAXR shows a 10-fold increase in Rb + coverage and a decrease in mean adsorption height from ∼3.5 to ∼2.7 Å with increasing pH, indicating enhanced counterion binding accompanied by Stern layer contraction. Streaming potential measurements demonstrate that the zeta potential, i.e., the potential at the hydrodynamic shear plane, is positive at pH 3 and becomes negative at pH ≥ 3.5. The negative charge magnitude increases with increasing pH, consistent with progressive surface deprotonation at higher pH. AIMD identifies inner- and outer-sphere Rb+ complexes whose adsorption heights and coordination geometries depend sensitively on the protonation state of surface oxygens, providing atomistic support for the experimentally inferred trends. These measurements establish two discrete, site-specific pH transitions in hydration-layer structure that track aluminol (de)protonation and quantitatively link them to a pH-driven contraction of the Stern layer (increasing Rb + coverage and decreasing adsorption height). This provides a direct structural basis for connecting surface acid−base chemistry to ion binding distances at an oxide−water interface.

Adsorption↗

Strong Local Evaporative Cooling Over Land Due to Atmospheric Aerosols

Abstract Aerosols can enhance terrestrial productivity through increased absorption of solar radiation by the shaded portion of the plant canopy—the diffuse radiation fertilization effect. Although this process can, in principle, alter surface evaporation due to the coupling between plant water loss and carbon uptake, with the potential to change the surface temperature, aerosol‐climate interactions have been traditionally viewed in light of the radiative effects within the atmosphere. Here, we develop a modeling framework that combines global atmosphere and land model simulations with a conceptual diagnostic tool to investigate these interactions from a surface energy budget perspective. Aerosols increase the terrestrial evaporative fraction, or the portion of net incoming energy consumed by evaporation, by over 4% globally and as much as ∼40% regionally. The main mechanism for this is the increase in energy allocation from sensible to latent heat due to global dimming (reduction in global shortwave radiation) and slightly augmented by diffuse radiation fertilization. In regions with moderately dense vegetation (leaf area index >2), the local surface cooling response to aerosols is dominated by this evaporative pathway, not the reduction in incident radiation. Diffuse radiation fertilization alone has a stronger impact on gross primary productivity (+2.18 Pg C y −1 or +1.8%) than on land evaporation (+0.18 W m −2 or +0.48%) and surface temperature (−0.01 K). Our results suggest that it is important for land surface models to distinguish between quantity (change in total magnitude) and quality (change in diffuse fraction) of radiative forcing for properly simulating surface climate.

Chakraborty, TC↗

The controlling role of atmosphere in dawsonite versus gibbsite precipitation from tetrahedral aluminate species

In highly alkaline solution, aluminum speciates as the tetrahedrally coordinated aluminate monomer, Al(OH)4- and/or dimer Al2O(OH)62-, yet precipitates as octahedrally coordinated gibbsite (Al(OH)3). This tetrahedral to octahedral transformation governs Al precipitation, which is crucial to worldwide Al production, and to the processing of caustic high-level radioactive wastes. Despite its significance, the transformation pathway remains unknown. Here we explore the roles of atmospheric water and carbon dioxide in mediating the transformation of the tetrahedrally coordinated potassium aluminate dimer salt (K2Al2O(OH)6) to gibbsite versus potassium dawsonite (KAl(CO3)(OH)2). A combination of in-situ attenuated total reflection infrared spectroscopy, ex-situ micro X-ray diffraction, and multivariate curve resolution-alternating least squares chemometrics analysis reveals that humidity plays a key role in the transformation by limiting the amount of alkalinity neutralization by dissolved CO2. Lower humidity favors higher alkalinity and incorporation of carbonate species in the final Al product to form KAl(CO3)(OH)2. Higher humidity enables more acid generation that destabilizes dawsonite and favors gibbsite as the solubility limiting phase. Because the transformation was restricted to occur in thin water films, the results suggest that transition from tetra- to octahedrally coordinated Al does not have to occur in bulk solution, as has often been hypothesized, but may instead appear on the source mineral surface.

Dembowski, Mateusz↗

Exploring the influence of interfacial solvation on electrochemical CO 2 reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy

Although interfacial solvation plays an important role in determining carbon dioxide reduction (CO 2 R) kinetics, present understanding of the potential dependent properties of the electrochemical double layer under conditions relevant for CO 2 R remains limited. This article summarizes the development and recent applications of plasmon-enhanced vibrational sum frequency generation (VSFG) spectroscopy to study the effects of cation hydration and interfacial solvation on CO 2 R using CO as a vibrational Stark reporter. Results show that electrolyte cations retain their entire solvation shell upon adsorption to inactive sites, while active sites retain only a single water layer between the gold surface and the cation. Measurements also show that the total interfacial electric field can be separated into two contributions: one from the electrochemical double layer (Stern field) and another from the polar solvation environment (Onsager field). Surprisingly, correlating VSFG spectra with reaction kinetics reveals that it is the solvation-mediated Onsager field that governs the chemical reactivity at the electrode/electrolyte interface. Measuring the interfacial water spectra during electrocatalysis also provides evidence for the proton source during H2 evolution, which competes with CO 2 R in aqueous electrolyte. These findings highlight the importance of directly probing cation hydration and interfacial solvation, which mediates reaction kinetics at electrochemical interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Role of water vapour in the absorption of nanosecond 266-nm laser pulses by atmospheric air

The absorption of the Nd : YAG fourth harmonic in air and binary mixtures of water vapour with nitrogen and oxygen at atmospheric pressure has been measured as a function of pulse energy (peak intensity). The mixtures obtained by adding equal amounts of water vapour to dry nitrogen and oxygen have been found to differ significantly in absorption. Preliminary quantitative data have been obtained for two- and three-photon absorption cross sections of water and oxygen molecules: σ{sup (2)}(H{sub 2}O) = (4 ± 1) ± 10{sup –49} cm{sup 4} s and σ{sup (3)}(O{sub 2}) = (5.6 ± 1.4) ± 10{sup –78} cm{sup 6} s{sup 2}. The absorption of 266-nm pulses with peak intensities from 0.05 to 2 GW cm{sup –2} in the near-surface atmosphere has been shown to be determined by two-photon absorption in water vapour and three-photon absorption in oxygen. In moist air containing 1 % water vapour, the absorption coefficient for 266-nm laser pulses exceeds that in dry air by four to five times. There is no absorption in nitrogen. We have developed a technique for photoacoustic measurements of multiphoton absorption cross sections in single-component gases and gas mixtures. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Geophysical Characterization and Monitoring of the 200 Area Treated Effluent Disposal Facility to Support Permit Renewal; TEDF Geophysical Monitoring

The Treated Effluent Disposal Facility (TEDF), located in the 200 East Area of the Hanford Site, is a site where non-hazardous and non-radioactive liquid wastes are disposed into two state-permitted infiltration basins. In 2016, the Washington State Department of Ecology denied a permit renewal request for TEDF due to the inability to adequately assess the impact of TEDF discharge water on the underlying groundwater quality. TEDF overlies the relatively impermeable Ringold Lower Mud (RLM) unit, whose upper contact lies in the vadose zone approximately 30 m below ground surface and approximately 10 m above the water table boundary. The RLM is assumed to isolate TEDF discharge water from the natural groundwater aquifer, which is monitored using wellbores screened below the RLM. Therefore, samples collected from monitoring wells near TEDF are not considered representative of TEDF discharge water. Rather, TEDF discharge water is assumed to mound on top of the RLM to form a perched aquifer. To support permitting of the TEDF, a new monitoring well is required that can be used to sample water from the presumed perched water aquifer above the RLM. Ideally, the screened section of the well would be located at the peak of the perched water mound(s), which presumably occurs at the point of maximum vertical flux from TEDF to the RLM, or equivalently where the dominant infiltration flow paths reach the RLM. This report describes how time-lapse 3D electrical resistivity tomography (ERT) was used in conjunction with nominal TEDF discharge operations to image the dominant flow paths from each pond to the RLM. Results are summarized in Figure ES.1. Figure ES.1A shows a satellite image of the TEDF overlain by an array of surface ERT electrodes. The solid and dashed black circles denote the zones of maximum vertical flux at the RLM within the south and north ponds, respectively, and presumably the regions where perched water peaks during discharge. Figure ES.1B shows time-lapse difference imaging results approximately 15 days after switching discharge from the south pond to the north pond. Blue iso-surfaces beneath the north pond denote regions of increasing bulk electrical conductivity caused by increasing saturation due to infiltrating water. Red iso-surfaces beneath the south pond denote regions that were previously saturated during the south pond discharge and are now de-saturating, causing a decrease in bulk electrical conductivity. In both cases, the zones of maximum change mark the dominant flow paths to the RLM. Figure ES.1C shows time-lapse imaging results approximately 15 days after switching discharge from the north pond to the south pond. In this case, blue iso-surfaces mark the dominant flow paths to the RLM from the south pond. The red iso-surfaces mark the dominant flow paths that existed during discharge to the north pond. The regions of maximum change in bulk conductivity (due to saturation or desaturation) that mark the primary flow paths are equivalent in both cases and denoted by the dashed solid and black circles. If a perched water zone forms on the RLM, it is likely to mound within or near the dashed circle during discharge to the north pond, and in the solid circle during discharge to the south pond. In other words, if perched water mounding occurs, the circles mark the optimum locations suggested by the ERT imaging for monitoring boreholes to be placed, enabling samples to be collected that are representative of TEDF discharge impacts on groundwater quality.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Charge accumulation and solvation in $β$-NiOOH: Surface chemistry of an OER catalyst from ML-aided simulations

Electrochemical water splitting is a key technology for a sustainable energy transition, providing a route to store surplus electricity from renewable sources. A central bottleneck is the sluggish oxygen evolution reaction (OER), which drives the search for catalysts that are active, stable, and inexpensive enough for large-scale deployment. Within this context, pure and doped NiO x H y combine high activity with low cost, making them prime candidates for alkaline OER. Yet, despite extensive study, the atomistic structure of NiOOH under operando conditions and the associated reaction mechanisms remain debated. Here, we investigate the structural complexity of pure β-NiOOH, the scaffold for its doped derivatives. We systematically investigate the oxidation of the surface adsorbates via proton-coupled electron transfer steps across relevant facets and sites, identifying the most probable sequence of deprotonation events. Our results reveal asymmetric charge accumulation on Wulff-relevant surfaces and show how applied potential can promote morphological restructuring. Explicit solvation is included through machine-learning interatomic potential molecular dynamics of the NiOOH/water interface, which allows us to resolve the hydrophobic and hydrophilic character of different surfaces and the associated interfacial water structure. Together, these insights demonstrate how surface chemistry and solvation jointly govern the stability of NiOOH and the accumulation of surface charge, with possible implications for catalytic performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radiative feedbacks on land surface change and associated tropical precipitation shifts

Changes in land surface albedo and land surface evaporation modulate the atmospheric energy budget by changing temperatures, water vapor, clouds, snow and ice cover, and the partitioning of surface energy fluxes. Here idealized perturbations to land surface properties are imposed in a global model to understand how such forcings drive shifts in zonal mean atmospheric energy transport and zonal mean tropical precipitation. For a uniform decrease in global land albedo, the albedo forcing and a positive water vapor feedback contribute roughly equally to increased energy absorption at the top of the atmosphere (TOA), while radiative changes due to the temperature and cloud cover response provide a negative feedback and energy loss at TOA. Decreasing land albedo causes a northwards shift in the zonal mean intertropical convergence zone (ITCZ). The combined effects on ITCZ location of all atmospheric feedbacks roughly cancel for the albedo forcing; the total ITCZ shift is comparable to that predicted for the albedo forcing alone. For an imposed increase in evaporative resistance that reduces land evaporation, low cloud cover decreases in the northern mid-latitudes and more energy is absorbed at TOA there; longwave loss due to warming provides a negative feedback on the TOA energy balance and ITCZ shift. Imposed changes in land albedo and evaporative resistance modulate fundamentally different aspects of the surface energy budget. However, the pattern of TOA radiation changes due to the water vapor and air temperature responses are highly correlated for these two forcings because both forcings lead to near-surface warming.

54 ENVIRONMENTAL SCIENCES↗

Altered morphology and diffusivity of water confined in MXenes: Machine learning–accelerated computations combined with experiments

Nanoconfined water exhibits unique properties compared to bulk water due to limited quantities, frustrated hydrogen bonding, and surface interactions, which are fundamental for energy storage and transport applications. We integrate machine learning–accelerated ab initio molecular dynamics with x-ray diffraction (XRD) and inelastic neutron scattering (INS) to systematically analyze the thermodynamic and dynamic behavior of water confined between functionalized (-F, -O, and -OH) two-dimensional (2D) Ti 3 C 2 T x MXene layers. As water intercalates between layers, the interlayer spacing exhibits layer-dependent staging characteristics. The water polarization can be flipped by the count and morphology of intercalated molecules interacting with MXene surface groups, resulting in varying electrostatic potential profiles. On the basis of interfacial electrostatic potential, hydrogen bond lifetime, and molecular orientation, we establish a linear combination of exponential model describing water diffusivity. These computational insights align well with experimental x-ray and neutron measurements, suggesting strategies for tuning water morphology and transport by tailoring MXene surface chemistry and water content for electrochemical energy storage and nanofluidic applications.

Tang, Jiawei [Southeast Univ., Nanjing (China)] (O↗

Broadband and filter radiometers at Ross Island, Antarctica: detection of cloud ice phase versus liquid water influences on shortwave and longwave radiation

Abstract. Surface radiometer data from Ross Island, Antarctica, collected during the austral summer 2015–2016 by the US Department of Energy Atmospheric Radiation Measurement (ARM) program West Antarctic Radiation Experiment (AWARE), are used to evaluate how shortwave and longwave irradiance respond to changing cloud properties as governed by contrasting meteorological regimes. Shortwave atmospheric transmittance is derived from pyranometer measurements, and cloud conservative-scattering optical depth is derived from filter radiometer measurements at 870 nm. With onshore flow associated with marine air masses, clouds contain mostly liquid water. With southerly flow over the Transantarctic Mountains, orographic forcing induces substantial cloud ice water content. These ice and mixed-phase clouds attenuate more surface shortwave irradiance than the maritime-influenced clouds and also emit less longwave irradiance due to colder cloud base temperature. These detected irradiance changes are in a range that can mean onset or inhibition of surface melt over ice shelves. This study demonstrates how basic and relatively low-cost broadband and filter radiometers can be used to detect subtle climatological influences of contrasting cloud microphysical properties at very remote locations.

54 ENVIRONMENTAL SCIENCES↗

Bridging interfacial properties and cell performance: A multiscale model for proton-exchange-membrane fuel cells

Here, to elucidate the impact of local interfaces on mass-transport resistance and overall cell performance of low-loaded proton-exchange-membrane fuel cells (PEMFCs), we present a multiscale modeling framework incorporating a novel modified agglomerate model. The model considers three distinct Pt-electrolyte interfaces: Pt on the carbon surface covered by either ionomer or water film and Pt inside carbon nanopores. Detailed mass-transport voltage-loss breakdowns reveal that coupled agglomerate-interface-scale mass transport dominates the mass-transport loss. The ionomer poisons the exterior-Pt surface through suppressing O 2 adsorption and intrinsic ORR activity, leading to low current-density performance. Conversely, interior-Pt interface enhances the kinetic performance but limits high current-density performance due to its low interfacial permeability. The exterior-Pt/water interface demonstrates superior kinetic performance and mass transport, though its practical implementation requires ensuring proton transport. By coupling the multiscale CL properties with ink parameters, the model identifies an optimal I to C ratio of approximately 0.5, a moderate value where the ionomer content is sufficient to guarantee proton transport without fully covering the Pt surface and forming large agglomeration, thus allowing the utilization of the Pt-water interface and avoiding high mass-transport loss. Overall, the model helps unravel limiting phenomena across different operating regimes and provides routes for optimizing performance.

Cell diagnostic↗