arXiv subjects

Adam Z. Weber

Publications and source records attributed to Adam Z. Weber.

5 recordsLinked to original sources

arXiv2026

Proton-electron coupled catalyst for ionomer-free electrochemical energy conversion

Efficient electrochemical energy devices are vital to renewable energy technology, yet coordinating the effective flow of electrons, ions, and chemical species continues to be a major challenge. In conventional proton-exchange membrane fuel cell (PEMFC) catalyst layers, proton and electron transport are supplied separately through percolating carbon networks and ionomer binders, rendering the catalyst largely passive and imposing fundamental trade-offs between reactant accessibility, ionic conductivity, and catalyst activity. Here, we introduce a one-dimensional proton-electron coupled catalyst (PECC) design, a transport-integrated electrocatalyst architecture in which the catalyst itself simultaneously supplies electronic and protonic transport to catalyst active sites. Using this PECC, PEMFCs can have an ionomer-free cathode catalyst layer (CCL), resulting in a dramatic 95% reduction in non-Fickian oxygen transport and boosting power density by 34% and 85% compared to traditional CCLs, with cathode Pt loadings of approximately 0.090 mg/cm^2 and 0.037 mg/cm^2, respectively. Meanwhile, PECC retains 65% of its mass activity and exhibits 32% higher power density than its ionomer-based CCL counterpart after 30k accelerated stressed test. Similar mass transport improvements have been observed in the electrochemical hydrogen pump (EHP) using PECC in the catalyst layers. Molecular dynamics simulations show the PECC's proton conductivity is 249% higher than Nafion. This PECC catalyst structure addresses core transport problems in PEMFCs, leading to almost 20% improvement in fuel efficiency and opens up new possibilities for designing high-performance, cost-effective electrochemical devices.

cond-mat.mtrl-sci↗

arXiv2025

Membrane-Electrode Assemblies for Electrochemical Reduction of CO2 to Ethylene: Design for Minimal Energy Consumption

Membrane-electrode-assembly (MEA) cells with copper (Cu) cathodes show strong potential for electrochemical CO2 reduction to ethylene (C2H4), but achieving high C2H4 selectivity remains a challenge due to competing hydrogen evolution. This selectivity is highly sensitive to the local microenvironment near the Cu catalyst surface. In this study, a 1-D, multiphysics continuum model is utilized to investigate how MEA cell performance and faradaic efficiency (FE) to C2H4 are affected by both component properties and operating conditions, with particular focus on coupled transport and reaction phenomena. Key parameters include cathode electrochemically active surface area (ECSA) and catalyst layer thickness. Halving catalyst layer thickness increases FE to C2H4 by 2% and lowers the cell voltage by 40 mV. In contrast, a tenfold decrease in ECSA results increases the FE to C2H4 by 7% but leads increase cell voltage at a given current density by 150 mV. This tradeoff occurs because the potential distribution within the cathode catalyst layer is the primary driving force for C2H4 formation. Increased cell voltage also raises the energy cost of C2H4 production. This model framework enables techno-economic assessments and identifies key factors that must be optimized to enable economically viable production of C2H4 via electrochemical reduction of CO2.

physics.chem-ph↗

arXiv2024

Operando probing of nanocracking in CuO-derived Cu during CO$_2$ electroreduction

Identifying and controlling active sites in electrocatalysis remains a grand challenge due to restructuring of catalysts in the complex chemical environments during operation. Inactive precatalysts can transform into active catalysts under reaction conditions, such as oxide-derived Cu (OD-Cu) for CO$_2$ electroreduction displaying improved production of multicarbon (C$_{2+}$) chemicals. Revealing the mechanism of active site origin in OD-Cu catalysts requires in situ/operando characterizations of structure, morphology, and valence state evolution with high spatial and temporal resolution. Applying newly developed electrochemical liquid cell transmission electron microscopy combined with X-ray absorption spectroscopy, our multimodal operando techniques unveil the formation pathways of OD-Cu active sites from CuO bicrystal nanowire precatalysts. Rapid reduction of CuO directly to Cu within 60 seconds generates a nanocrack network throughout the nanowire, via formation of "boundary nanocracks" along the twin boundary and "transverse nanocracks" propagating from the surface to the center of the nanowire. The nanocrack network further reconstructs, leading to a highly porous structure rich in Cu nanograins, with a boosted specific surface area and density of active sites for C$_{2+}$ products. These findings suggest a means to optimize active OD-Cu nanostructures through nanocracking by tailoring grain boundaries in CuO precatalysts. More generally, our advanced operando approach opens new opportunities for mechanistic insights to enable improved control of catalyst structure and performance.

cond-mat.mtrl-sci↗

arXiv2023

Operando Label-free Optical Imaging of Solution-Phase Ion Transport and Electrochemistry

Ion transport is a fundamental process in many physical, chemical, and biological phenomena, and especially in electrochemical energy conversion and storage. Despite its immense importance, demonstrations of label-free, spatially and temporally resolved ion imaging in the solution phase under operando conditions are not widespread. Here we spatiotemporally map ion concentration gradient evolution in solution and yield ion transport parameters by refining interferometric reflection microscopy, obviating the need for absorptive or fluorescent labels. As an example, we use an electrochemical cell with planar electrodes to drive concentration gradients in a ferricyanide-based aqueous redox electrolyte, and we observe the lateral spatiotemporal evolution of ions via concentration-dependent changes to the refractive index. Analysis of an evolving spatiotemporal ion distribution directly yields the diffusivity of the redox-active species. The simplicity of this approach makes it amenable to probing local ion transport behavior in a wide range of electrochemical, bioelectronic, and electrophysiological systems.

physics.app-ph↗

arXiv2019

Electric Field Intensity Modulated Scattering as a Thin-Film Depth Probe

Grazing incidence x-ray scattering provides nanostructural information for thin film samples, but single images generally do not provide information on film thickness or the full complex index of refraction. Additionally, for thin films that possess stratification of scatterers vertically within a sample, it can be difficult to determine where those scatterers are positioned. We present an in-situ method to extract film thickness, the index of refraction, and depth information using scattering images taken across a range of incident angles. The underlying theory is presented, and we validate the technique using two sets of polymer thin films. Finally, we discuss how it can be implemented as a general beamline procedure. This technique is applicable to any thin-film material and has potentially far-reaching impact by enabling depth-sensitive information in situ at any grazing incidence-capable beamline.

physics.app-ph↗