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Chueh, William

Publications and source records attributed to Chueh, William.

12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Learning heterogeneous reaction kinetics from X-ray movies pixel-by-pixel

Reaction rates at spatially heterogeneous, unstable interfaces are notoriously difficult to quantify, yet are essential in engineering many chemical systems, such as batteries 1 and electrocatalysts 2. Experimental characterizations of such materials by operando microscopy produce rich image datasets 3–6, but data-driven methods to learn physics from these images are still lacking because of the complex coupling of reaction kinetics, surface chemistry and phase separation 7. Here we show that heterogeneous reaction kinetics can be learned from in situ scanning transmission X-ray microscopy (STXM) images of carbon-coated lithium iron phosphate (LFP) nanoparticles. Combining a large dataset of STXM images with a thermodynamically consistent electrochemical phase-field model, partial differential equation (PDE)-constrained optimization and uncertainty quantification, we extract the free-energy landscape and reaction kinetics and verify their consistency with theoretical models. We also simultaneously learn the spatial heterogeneity of the reaction rate, which closely matches the carbon-coating thickness profiles obtained through Auger electron microscopy (AEM). Across 180,000 image pixels, the mean discrepancy with the learned model is remarkably small (<7%) and comparable with experimental noise. Our results open the possibility of learning nonequilibrium material properties beyond the reach of traditional experimental methods and offer a new non-destructive technique for characterizing and optimizing heterogeneous reactive surfaces.

Chueh, William↗
DOE OSTI2023

Correlating Tomographic Chemical Inhomogeneity and Low Energy Electronic Structure in Layered Quantum Materials

Photoemission spectroscopy (PES) is a suite of experimental tools to learn about the electronic and chemical structure of materials and surfaces. Normally implemented in a surface-sensitive manner, the research performed under this grant focused on pushing PES into less explored regimes, to reveal bulk electronic structure, to reveal tomographic (layer-resolved) chemistry and electronic structure of layered materials and heterostructures, and to reveal interface phenomena at the junction of two different materials. Standing wave (SW) spectroscopies have also been applied to PdCoO2, a material of interest due to its high conductivity and electron-hydrodynamic tendencies. This material can be modeled as an alternating layered structure consisting of metallic Pd layers and insulating CoO2 layers. Using SW XPS, the total electronic structure has been decomposed into contributions from the two layers, and computations highlighted the different many-body interactions in the two layers (Comm. Phys. 4, 143 (2021)). We have also used hard-x-ray angle-resolved photoemission spectroscopy (ARPES), to investigate LaB6, a technologically important material with widespread application as a cathode material for electron microscopes. We measured the bulk electronic structure of this material and found that the one-step model of photoemission better captured the electronic structure and correlations. This model treats the three steps of the photoemission process—excitation, transport of the photoelectron to the crystal surface, and escape into the vacuum—as a single quantum mechanically coherent process (Phys. Rev. Mater. 5, 055002 (2021)). We also applied x-ray photoelectron spectroscopy, implemented in a near total reflection grazing incidence geometry to elucidate technologically relevant interfaces, such as those between a substrate and photoresist (J. Phys. D: Appl. Phys. 54 464002 (2021)).

36 MATERIALS SCIENCE↗
DOE OSTI2017

Direct Mapping of Band Positions in Doped and Undoped Hematite during Photoelectrochemical Water Splitting

Photoelectrochemical water splitting is a promising pathway for the direct conversion of renewable solar energy to easy to store and use chemical energy. The performance of a photoelectrochemical device is determined in large part by the heterogeneous interface between the photoanode and the electrolyte, which we here characterize directly under operating conditions using interface-specific probes. Utilizing X-ray photoelectron spectroscopy as a noncontact probe of local electrical potentials, we demonstrate direct measurements of the band alignment at the semiconductor/electrolyte interface of an operating hematite/KOH photoelectrochemical cell as a function of solar illumination, applied potential, and doping. Here, we provide evidence for the absence of in-gap states in this system, which is contrary to previous measurements using indirect methods, and give a comprehensive description of shifts in the band positions and limiting processes during the photoelectrochemical reaction.

14 SOLAR ENERGY↗
DOE OSTI2016

Surface-Modified Electrodes: Enhancing Performance Guided by Insitu Spectroscopy and Microscopy

The aim of this project is to understand the nature of active sites and degradation mechanisms in solid-oxide fuel cells cathodes. Using Co and Fe-based perovskite oxides as model systems, we developed a comprehensive understanding of the active site and degradation. In particular, we correlated cation segregation, precipitation and surface reconstruction to electrochemical activity and stability. We show that in conventional materials, the most active cathodes are not the most stable ones. A novel strategy of cation segregation buffer layer was proposed and developed to overcome this limitation. A nanoscale barrier layer was inserted a few nanometer below the surface of the cathodes which prevents the cations from diffusing from the bulk to the surface. We report a LSCF-based cathode with record performance and stability, reach an impressive 0.03 Ω cm 2 at 650 °C in air. This modification strategy is expected to lead to more active and stable solid-oxide fuel cells, and ultimately lead to lower cost in commercial systems.

25 ENERGY STORAGE↗
DOE OSTI2016

High Efficiency Solar Thermochemical Reactor for Hydrogen Production

Overall objectives of the project were: Verify the potential for solar thermochemical cycles for hydrogen production to be competitive in the long term and by 2020, develop this technology to produce hydrogen with a projected cost of $3.00/gge at the plant gate; and, Develop a high-efficiency particle bed reactor for producing hydrogen via a thermochemical water-splitting (WS) cycle, and demonstrate eight continuous hours of operation on a solar simulator producing greater than 3 L of H 2 .

08 HYDROGEN↗
DOE OSTI2012

Probing surface & transport phenomena in energy materials under operating conditions

Efficient conversion of energy between sunlight, chemical bonds, and electricity is crucial towards a closed-loop energy cycle. We have applied synchrotron-based X ray spectroscopy and microscopy techniques to investigate the conversion of electricity to and from chemical bonds in fuel cells, electrolyzers, and intercalation batteries. Using these techniques, we have tracked the motions from electrons, oxygen ions, and lithium ions at interfaces and in the bulk of electrochemically-active materials. New insights in gas-solid surface electrochemistry, and solid-solid phase transformation are guiding the development of better materials for a wide range of energy conversion and storage devices.

Chueh, William↗
DOE OSTI2011

Mechanisms for Charge-Transfer Processes at Electrode/Solid-Electrolyte Interfaces

This report summarizes the accomplishments of a Laboratory-Directed Research and Development (LDRD) project focused on developing and applying new x-ray spectroscopies to understand and improve electric charge transfer in electrochemical devices. Our approach studies the device materials as they function at elevated temperature and in the presence of sufficient gas to generate meaningful currents through the device. We developed hardware and methods to allow x-ray photoelectron spectroscopy to be applied under these conditions. We then showed that the approach can measure the local electric potentials of the materials, identify the chemical nature of the electrochemical intermediate reaction species and determine the chemical state of the active materials. When performed simultaneous to traditional impedance-based analysis, the approach provides an unprecedented characterization of an operating electrochemical system.

36 MATERIALS SCIENCE↗