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At least 235 records · Page 13

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DOE OSTI2015

Development and assessment of a physics-based simulation model to investigate residential PM 2.5 infiltration across the US housing stock

The Lawrence Berkeley National Laboratory Population Impact Assessment Modeling Framework (PIAMF) was expanded here to enable determination of indoor PM 2.5 concentrations and exposures in a set of 50,000 homes representing the US housing stock. A mass-balance model is used to calculate time-dependent pollutant concentrations within each home. The model includes size- and species-dependent removal mechanisms. The particle model was applied to the housing samples of the Relationship of Indoor, Outdoor, and Personal Air (RIOPA) and The Detroit Exposure and Aerosol Research Study (DEARS) studies to compare model- and measurement-based estimates of indoor PM 2.5 of outdoor origin. Model-derived distributions of infiltration factors (ratio of indoor PM 2.5 of outdoor origin to outdoor PM 2.5 ) are compared to measurement-based distributions obtained in studies conducted in 11 US cities.

42 ENGINEERING↗

DOE OSTI2018

High performance metal-supported solid oxide fuel cells with infiltrated electrodes

High power density is required to commercialize solid oxide fuel cells for vehicular applications. High performance of metal supported solid oxide fuel cells (MS-SOFCs) is achieved via catalyst composition, electrode structure, and processing optimization. The full cell configuration consists of a dense ceramic electrolyte and porous ceramic backbones (electrodes) sandwiched between porous stainless steel metal supports. The conventional YSZ electrolyte and backbones are replaced with more conductive and thinner 10Sc1CeSZ ceramics. MS-SOFCs are co-sintered in a single step and subsequently infiltrated with nanocatalysts. Five categories of cathode catalysts are screened in full cells, including: perovskites, nickelates, praseodymium oxide, binary layered composites, and ternary layered composites. Various anode compositions are also tested. The conventional LSM cathode catalyst is replaced with more active Pr 6 O 11 and the Ni content of the SDC-Ni anode is increased. The resulting cells achieve a peak power of 1.56, 2.0, and 2.85 W cm -2 at 700, 750, and 800 °C, respectively, with 3%H 2 O/H 2 as fuel and cathode exposed to air. Multiple cells show reproducible performance (P max = 1.50 ± 0.06 W cm -2 ) and OCV (1.10 ± 0.02 V). Finally, the performance is further increased with cathode exposed to pure oxygen (2.0 W cm -2 at 700 °C).

25 ENERGY STORAGE↗

DOE OSTI2016

Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study

We have investigated the growth of zinc oxide in a polymer matrix by sequential infiltration synthesis (SiS). The atomic cycle-by-cycle self-terminating reaction growth investigation was done using photoluminescence (PL), Raman, and X-ray photoemission spectroscopy (XPS). Results show clear differences between Zn atom configurations at the initial stages of growth. Mono Zn atoms (O-Zn and O-Zn-O) exhibit pure UV emission with little evidence of deep level oxygen vacancy states (VO). Dimer Zn atoms (O-Zn-O-Zn and O-Zn-O-Zn-O) show strong UV and visible PL emission from VO states 20 times greater than that from the mono Zn atom configuration. After three precursor cycles, the PL emission intensity drops significantly exhibiting first evidence of crystal formation as observed with Raman spectroscopy via the presence of longitudinal optical phonons. We also report a first confirmation of energy transfer between polymer and ZnO where the polymer absorbs light at 241 nm and emits at 360 nm, which coincides with the ZnO UV emission peak. Our work shows that ZnO dimers are unique ZnO configurations with high PL intensity, unique O1s oxidation states, and sub-10 ps absorption and decay, which are interesting properties for novel quantum material applications.

infiltration↗

DOE OSTI2023

Molecular-Weight-Dependent Infiltration and Adsorption of Polymers into Nanochannels

The mesoporous silica shell coating hydrogenolysis nano-catalysts alters the molecular weight distributions of cleaved polymer chains compared to catalysts without a shell. The shell, composed of radially aligned narrow cylindrical nanopores, reduces the formation of low-valued gaseous products and increases the median molecular weight of the product, thus enhancing the value of the products for polymer upcycling. Here, to understand the role of the mesoporous shell, we have studied the spatial distribution of polystyrene chains, used as a model polymer, in the nanochannels in both the melt phase and solution phase. In the melt, we observed from small-angle X-ray scattering experiments that the infiltration rate of the polymer into the nanochannels is inversely proportional to the molecular weight, which is consistent with theory. In theta solution experiments using UV–vis spectroscopy, we found that the shell significantly enhances polymer adsorption compared to nanoparticles without pores. In addition, the degree of polymer adsorption is not a monotonic function of molecular weight but initially increases with the molecular weight before eventually decreasing. The molecular weight for the peak adsorption increases with the pore diameter. This adsorption behavior is rationalized as resulting from a balance between the mixing entropy gain by surface adsorption and the conformational entropy penalty incurred by chains confined in the nanochannels. The spatial distribution of polymer chains in the nanochannels is visualized by energy-dispersive X-ray spectroscopy (EDX), and inverse Abel-transformed data reveals a less uniform polymer distribution along the primary pore axis for longer chains.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Controlling Nanoscale Pore Size and Wall Composition in Polycarbonate Membranes via Atomic Layer Deposition and Sequential Infiltration Synthesis: Implications for High Water Permeance

Polymer membranes have a wide variety of applications, ranging from water treatment to energy storage. Many of these applications require precise control over the membrane porosity and surface chemistry. In this study, we explore the modification of isoporous polycarbonate (PC) track-etched membranes (PCTEs) by atomic layer deposition (ALD) and sequential infiltration synthesis (SIS) to tune the pore size and the pore wall surface chemistry. We first performed a detailed study of Al 2 O 3 ALD and SIS in PCTE using a variety of in situ and ex situ measurements. We discovered that short precursor exposure times are critical to achieve conformal Al 2 O 3 ALD in the PCTE nanopores, while longer precursor exposure times resulted in Al 2 O 3 SIS within the bulk of the PC leaving the membranes brittle. Next, we tuned the PCTE pore size via Al 2 O 3 ALD and studied its effect on the water contact angle and the water permeance. Here, we found that the membranes became more hydrophilic, and the permeance decreased with increasing ALD Al 2 O 3 cycles. Finally, we studied the effect of hydrophilic (SnO 2 )/hydrophobic (In 2 O 3 ) ALD metal oxide coatings on membrane properties. We found that the most hydrophilic SnO 2 showed the highest water flux and the least hydrophilic In 2 O 3 showed the lowest water flux through the PCTE membranes. Our results demonstrate that ALD is an effective method to tune the surface and transport properties of PCTE membranes, but care must be exercised to avoid SIS and bulk modification of the polymer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Nanoporous Dielectric Resistive Memories Using Sequential Infiltration Synthesis

Resistance switching in metal–insulator–metal structures has been extensively studied in recent years for use as synaptic elements for neuromorphic computing and as nonvolatile memory elements. However, high switching power requirements, device variabilities, and considerable trade-offs between low operating voltages, high on/off ratios, and low leakage have limited their utility. Here, we have addressed these issues by demonstrating the use of ultraporous dielectrics as a pathway for high-performance resistive memory devices. Using a modified atomic layer deposition based technique known as sequential infiltration synthesis, which was developed originally for improving polymer properties such as enhanced etch resistance of electron-beam resists and for the creation of films for filtration and oleophilic applications, we are able to create ~15 nm thick ultraporous (pore size ~5 nm) oxide dielectrics with up to 73% porosity as the medium for filament formation. We show, using the Ag/Al 2 O 3 system, that the ultraporous films result in ultrahigh on/off ratio (>10 9 ) at ultralow switching voltages (~±600 mV) that are 10× smaller than those for the bulk case. In addition, the devices demonstrate fast switching, pulsed endurance up to 1 million cycles. and high temperature (125 °C) retention up to 10 4 s, making this approach highly promising for large-scale neuromorphic and memory applications. Additionally, this synthesis methodology provides a compatible, inexpensive route that is scalable and compatible with existing semiconductor nanofabrication methods and materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Resolving the Atomic Structure of Sequential Infiltration Synthesis Derived Inorganic Clusters

Sequential infiltration synthesis (SIS) is a route to the precision deposition of inorganic solids in analogy to atomic layer deposition but occurs within (vs upon) a soft material template. SIS has enabled exquisite nanoscale morphological complexity in various oxides through selective nucleation in block copolymers templates. However, the earliest stages of SIS growth remain unresolved, including the atomic structure of nuclei and the evolution of local coordination environments, before and after polymer template removal. We employed In K-edge extended X-ray absorption fine structure and atomic pair distribution function analysis of high-energy X-ray scattering to unravel (1) the structural evolution of InO x H y clusters inside a poly(methyl methacrylate) (PMMA) host matrix and (2) the formation of porous In 2 O 3 solids (obtained after annealing) as a function of SIS cycle number. Early SIS cycles result in InO x H y cluster growth with high aspect ratio, followed by the formation of a three-dimensional network with additional SIS cycles. That the atomic structures of the InO x H y clusters can be modeled as multinuclear clusters with bonding patterns related to those in In 2 O 3 and In(OH) 3 crystal structures suggests that SIS may be an efficient route to 3D arrays of discrete-atom-number clusters. As a result, annealing the mixed inorganic/polymer films in air removes the PMMA template and consolidates the as-grown clusters into cubic In 2 O 3 nanocrystals with structural details that also depend on SIS cycle number.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Chemical vapor infiltration of additively manufactured preforms: Pore-resolved simulations and experimental validation

The densification of additively manufactured porous preforms by chemical vapor infiltration (CVI) is studied using pore-resolved simulations and experiments. Experimentally, 3D printed silicon carbide (SiC) preforms are subject to CVI synthesis using methyltrichlorosilane (MTS) precursor to obtain high purity SiC/SiC composites. Optical images of the cross sections of the processed preforms are analyzed to obtain the spatial porosity distribution. The numerical method is based on a level set formulation to capture the spatial distribution and time evolution of the pore scale microstructural characteristics. The coupled transport and kinetic effects are represented using a dimensionless Thiele modulus. Simulations are initialized using representative synthetic preform geometries comprising of packed particles based on the size distribution of the powder used for 3D printing. The simulation results are validated against the experimental observations in terms of total density and the distribution of residual porosity. The densification characteristics, porosity classification, concentration profiles, and structure functions are analyzed as functions of processing temperature and Thiele modulus.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Effects of temperature inversion on densification in chemical vapor infiltration

In a classical chemical vapor infiltration (CVI) process, the competing effects of chemical kinetics and reagent gas transport lead to non–uniform depositions such that outer layers of a preform densify faster leaving the core highly porous. Currently, CVI must be performed at a sufficiently low temperature to achieve good densification quality which leads to high processing time and cost. Volumetric heating of the preform, especially through microwaves, can create temperature inversion such that the core is hotter than the outer surface and potentially, overcome the challenges associated with isothermal CVI. Direct numerical simulations (DNS) of densification under various such temperature distributions indicate that microwave heating in CVI processing can lead to better (uniform) densification of porous preforms. Here the role of key parameters describing the temperature distributions on the densification behavior is investigated. Strategic temporal control of the temperature distribution shows that processing times can be reduced by almost half while maintaining a good densification quality similar to that of low–temperature isothermal processing. Inside–out densification due to the inverted temperature profile is a key distinguishing characteristic of microwave assisted CVI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Impact of Infiltration and Ventilation on Measured Space Conditioning Energy and Moisture Levels in the Hot-Humid Climate, Cocoa, Florida (Fact Sheet)

Air infiltration and ventilation in residential buildings is a very large part of the heating loads, but empirical data regarding the impact on space cooling has been lacking. Moreover, there has been little data on how building tightness might relate to building interior moisture levels in homes in a hot and humid climate. To address this need, BA-PIRC has conducted research to assess the moisture and cooling load impacts of airtightness and mechanical ventilation in two identical laboratory homes in the hot-humid climate over the cooling season.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2014

Flexible Residential Test Facility: Impact of Infiltration and Ventilation on Measured Cooling Season Energy and Moisture Levels

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2016

Flexible Residential Test Facility: Impact of Infiltration and Ventilation on Measured Cooling Season Energy and Moisture Levels

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2018

Infiltration Time Profiles for E-Area LLWF Intact and Subsidence Scenarios

To support future Unreviewed Disposal Question Evaluations (UDQEs), Special Analyses (SAs) and/or Performance Assessments (PAs) for the E-Area Low-Level Waste Facility (LLWF) at the Savannah River Site (SRS), the Hydrologic Evaluation of Landfill Performance (HELP) model and a newly developed, Python-based, probabilistic model employing a Monte Carlo sampling technique were used together to generate infiltration degradation curves over a 10,000-year simulation period for both intact and subsided slit- and engineered-trench closure-cap scenarios. The results will be used in PORFLOW transport model simulations of the E-Area LLWF trench units.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Development of Training Materials for Pathologists to Provide Machine Learning Validation Data of Tumor-Infiltrating Lymphocytes in Breast Cancer

The High Throughput Truthing project aims to develop a dataset for validating artificial intelligence and machine learning models (AI/ML) fit for regulatory purposes. The context of this AI/ML validation dataset is the reporting of stromal tumor-infiltrating lymphocytes (sTILs) density evaluations in hematoxylin and eosin-stained invasive breast cancer biopsy specimens. After completing the pilot study, we found notable variability in the sTILs estimates as well as inconsistencies and gaps in the provided training to pathologists. Using the pilot study data and an expert panel, we created custom training materials to improve pathologist annotation quality for the pivotal study. We categorized regions of interest (ROIs) based on their mean sTILs density and selected ROIs with the highest and lowest sTILs variability. In a series of eight one-hour sessions, the expert panel reviewed each ROI and provided verbal density estimates and comments on features that confounded the sTILs evaluation. We aggregated and shaped the comments to identify pitfalls and instructions to improve our training materials. From these selected ROIs, we created a training set and proficiency test set to improve pathologist training with the goal to improve data collection for the pivotal study. We are not exploring AI/ML performance in this paper. Instead, we are creating materials that will train crowd-sourced pathologists to be the reference standard in a pivotal study to create an AI/ML model validation dataset. The issues discussed here are also important for clinicians to understand about the evaluation of sTILs in clinical practice and can provide insight to developers of AI/ML models.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Additive Manufacturing of C/C-SiC Ceramic Matrix Composites by Automated Fiber Placement of Continuous Fiber Tow in Polymer with Pyrolysis and Reactive Silicon Melt Infiltration

An additive manufacturing process for fabricating ceramic matrix composites has been developed based on the C/C-SiC system. Automated fiber placement of the continuous carbon fibers in a polyether ether ketone matrix was performed to consolidate the carbon fibers into a printed preform. Pyrolysis was performed to convert the polymer matrix to porous carbon, and then Si was introduced by reactive melt infiltration to convert a portion of the carbon matrix to silicon carbide. The densities and microstructures were characterized after each step during the processing, and the mechanical properties were measured. The C/C-SiC composites exhibited a porosity of 10–20%, characteristic flexural strength of 234.91 MPa, and Weibull modulus of 3.21. The composites displayed toughness via a significant displacement to failure.

36 MATERIALS SCIENCE↗

NASA NTRS1994

Two-Layer Variable Infiltration Capacity Land Surface Representation for General Circulation Models

A simple two-layer variable infiltration capacity (VIC-2L) land surface model suitable for incorporation in general circulation models (GCMs) is described. The model consists of a two-layer characterization of the soil within a GCM grid cell, and uses an aerodynamic representation of latent and sensible heat fluxes at the land surface. The effects of GCM spatial subgrid variability of soil moisture and a hydrologically realistic runoff mechanism are represented in the soil layers. The model was tested using long-term hydrologic and climatalogical data for Kings Creek, Kansas to estimate and validate the hydrological parameters. Surface flux data from three First International Satellite Land Surface Climatology Project Field Experiments (FIFE) intensive field compaigns in the summer and fall of 1987 in central Kansas, and from the Anglo-Brazilian Amazonian Climate Observation Study (ABRACOS) in Brazil were used to validate the mode-simulated surface energy fluxes and surface temperature.

GENERAL CIRCULATION MODELS↗

NASA NTRS2018

Modeling the Effect of Damage on the Electrical Resistivity of Melt-Infiltrated SiC/SiC Composites

Electrical resistivity (ER) measurements are a possible health monitoring technique for CMC components in future aerospace applications. In order to use ER measurements to detect and identify damage, it is necessary to understand how each specific damage state will affect the ER response. In this paper, finite element models are developed and applied to quantify the effect of specific damage states on the electrical resistivity response in a melt-infiltrated silicon carbide (SiC) fiber-reinforced silicon carbide composite. The electrical resistivity of several damage states are calculated by simulating the electric current flow through the damaged micro-structure. This is achieved by performing the numerical solution of the steady-state conservation of charge density equation. Numerical results reveal that cracking of the inter-tow matrix has the most profound effect on the composite electrical resistivity. Also, fiber/matrix debonding at matrix cracks in the 0° tows (tows aligned with the loading direction) may cause a significant increase in the electrical resistivity, but only if the fiber coating resistivity is 1000 Ω-cm or less. Cracks in the 90° tows and the crack opening displacement have very little effect on the composite electrical resistivity.

finite element analysis↗

DOE OSTI2014

Technology Solutions Case Study: Impact of Infiltration and Ventilation on Measured Space Conditioning Energy and Moisture Levels in the Hot-Humid Climate

Air infiltration and ventilation in residential buildings is a very large part of the heating loads, but empirical data regarding the impact on space cooling has been lacking. Moreover, there has been little data on how building tightness might relate to building interior moisture levels in homes in a hot and humid climate. To address this need, BA-PIRC conducted research to assess the moisture and cooling load impacts of airtightness and mechanical ventilation in two identical laboratory homes in the hot-humid climate over the cooling season.

BA-PIRC↗