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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Elucidating the Dynamic Nature of Fuel Cell Electrodes as a Function of Conditioning: An ex Situ Material Characterization and in Situ Electrochemical Diagnostic Study

To increase the commercialization of fuel cell electric vehicles, it is imperative to improve the activity and performance of electrocatalysts through combined efforts focused on material characterization and device-level integration. Obtaining fundamental insights into the ongoing structural and compositional changes of electrocatalysts is crucial for not only transitioning an electrode from its as-prepared to functional state, also known as 'conditioning', but also for establishing intrinsic electrochemical performances. Here, we investigated several oxygen reduction reaction (ORR) electrocatalysts via in situ and ex situ characterization techniques to provide fundamental insights into the interfacial phenomena that enable peak ORR mass activity and high current density performance. A mechanistic understanding of a fuel cell conditioning procedure is described, which encompasses voltage cycling and subsequent voltage recovery (VR) steps at low potential. In particular, ex situ membrane electrode assembly characterization using transmission electron microscopy and ultra-small angle X-ray scattering were performed to determine changes in carbon and Pt particle size and morphology, while in situ electrochemical diagnostics were performed either during or after specific points in the testing protocol to determine the electrochemical and interfacial changes occurring on the catalyst surface responsible for oxygen transport resistances through ionomer films. The results demonstrate that the voltage cycling (break-in) step aids in the removal of sulfate and fluoride and concomitantly reduces non-Fickian oxygen transport resistances, especially for catalysts where Pt is located within the pores of the carbon support. Subsequent low voltage holds at low temperature and oversaturated conditions, i.e., VR cycles, serve to improve mass activities by a factor of two to three, through a combined removal of contaminants, surface-blocking species (e.g., oxides), and rearrangement of the catalyst atomic structure (e.g., Pt-Pt and Pt-Co coordination).

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Elucidating the Role of Ionomer in the Performance of Platinum Group Metal-free Catalyst Layer via in situ Electrochemical Diagnostics

The ionomer content in platinum group metal (PGM)-free polymer electrolyte fuel cell (PEFC) cathode catalyst layer (CCL) plays an important role in the electrode gas transport properties, proton conductivity, and hence, membrane electrode assembly (MEA) performance. In this work, the ionomer content in the CCL is varied, influencing electrode microstructure by altering porosity, tortuosity, as well as ionomer distribution and coverage of the catalyst particles. A novel technique consisting of a H 2 pump, combined with a Pt black sensor layer, is used to measure the bulk mass transport resistance of a series of PGM-free CCL prepared with different ionomer contents. The values for bulk electrode mass transport resistance are contrasted with electrode proton transport resistance in the cathode catalyst layer, establishing a clearly defined trade-off between two key performance limiting phenomena and identifying a need for novel PGM-free electrode fabrication strategies.

25 ENERGY STORAGE↗
DOE OSTI2021

Mitigation of PtCo/C Cathode Catalyst Degradation via Control of Relative Humidity

Maintaining the high performance of proton-exchange membrane fuel cells (PEMFC) over the course of its lifetime is a key enabling factor for its successful commercialization as a primary power source in zero-emission transportation applications. In this context, it is important to mitigate the degradation of PtCo-alloy based cathode catalysts used for oxygen reduction reaction (ORR). PtCo-alloy catalysts exhibit high activity at beginning-of-life (BOL) which tends to decrease during operation due to loss of electrochemical surface area (ECSA) and dissolution-contamination related effects of the Co-alloying component. Here, we demonstrate the use of relative humidity (RH) of the inlet gases as a controllable parameter to mitigate the degradation of PtCo-alloy catalyst degradation. We employ a catalyst-specific voltage cycling accelerated stress test (AST) durability protocol as a function of inlet RH to degrade PtCo catalysts. A series of in situ electrochemical diagnostics and ex situ characterizations have been carried out to investigate the catalyst layer characteristics at end-of-test (EOT). Our results show that at sub-saturated conditions of durability protocol operation, PtCo catalyst sustains higher EOT H 2 /air performance due to better retention of ECSA and smaller impact of Co 2+ dissolution/contamination.

25 ENERGY STORAGE↗
DOE OSTI2019

Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application

In this study, in situ electrochemical diagnostics designed to probe ionomer interactions with platinum and carbon were applied to relate ionomer coverage and conformation, gleaned from anion adsorption data, with O 2 transport resistance for low-loaded (0.05 mg Pt cm -2 ) platinum-supported Vulcan carbon (Pt/Vu)-based electrodes in a polymer electrolyte fuel cell. Coupling the in situ diagnostic data with ex situ characterization of catalyst inks and electrode structures, the effect of ink composition is explained by both ink-level interactions that dictate the electrode microstructure during fabrication and the resulting local ionomer distribution near catalyst sites. Electrochemical techniques (CO displacement and ac impedance) show that catalyst inks with higher water content increase ionomer (sulfonate) interactions with Pt sites without significantly affecting ionomer coverage on the carbon support. Surprisingly, the higher anion adsorption is shown to have a minor impact on specific activity, while exhibiting a complex relationship with oxygen transport. Ex situ characterization of ionomer suspensions and catalyst/ionomer inks indicates that the lower ionomer coverage can be correlated with the formation of large ionomer aggregates and weaker ionomer/catalyst interactions in low-water content inks. These larger ionomer aggregates resulted in increased local oxygen transport resistance, namely, through the ionomer film, and reduced performance at high current density. In the water-rich inks, the ionomer aggregate size decreases, while stronger ionomer/Pt interactions are observed. The reduced ionomer aggregation improves transport resistance through the ionomer film, while the increased adsorption leads to the emergence of resistance at the ionomer/Pt interface. Overall, the high current density performance is shown to be a nonmonotonic function of ink water content, scaling with the local gas (H 2 , O 2 ) transport resistance resulting from pore, thin film, and interfacial phenomena.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2021

Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Microstructure and Pt Accessibility

This work investigates how local ionomer/platinum (Pt) interactions and ionomer distribution in electrospun Pt/Vulcan nanofiber electrodes impact ionomer coverage, proton accessibility, and oxygen reduction reaction (ORR) performance in proton-exchange membrane fuel cells. Insights from various in situ electrochemical diagnostics were utilized in conjunction with ex situ microscopic characterization to understand how the electrode microstructure—both at the aggregate level and near the ionomer/platinum interface—is affected by electrospinning in comparison to ultrasonic spraying. The effect of the carrier polymer poly(acrylic acid) (PAA) concentration from 5–20 wt % (with respect to total ink solids) on the resulting nanofiber morphology is discussed. Electron microscopy observations and CO displacement measurements indicated that Pt/Vulcan nanofibers prepared with a higher PAA concentration (15 wt %) were conformally coated with a film of ionomer on the exterior of the fiber, which resulted in an overall lower ionomer coverage on both Pt and carbon throughout the fiber diameter. In contrast, 10 wt % PAA leads to a uniform intrafiber distribution of the ionomer within the fibers, increasing the overall ionomer coverage and proton accessibility under both wet and dry conditions. These differences in the local ionomer coverage on Pt between 10 and 15 wt % PAA were also attributed to differences in the adsorption/interaction affinities between PAA and the ionomer onto the catalyst surface in the ink using zeta potential measurements. Additional fuel cell electrochemical tests on the electrospun electrodes show improvements in ORR kinetics and high-current-density H 2 /air performance compared to the ultrasonically sprayed electrodes.

25 ENERGY STORAGE↗
DOE OSTI2020

In situ Diagnostics of Coupled Electrochemical-Mechanical Properties of Solid Electrolyte Interphases on Lithium Metal Rechargeable Batteries (Final Technical Report)

The fundamental understanding of the coupled mechanical/chemical degradation of the SEI layer during lithium cycling will enable the project to identify the desirable mechanical properties on SEI/lithium as a system and the specific transport properties that enable the homogenous lithium stripping/plating while avoiding the mossy structure. Furthermore, it will allow the project to develop a highly impactful strategy to protect lithium metal and achieve dendrite free high cycle efficiency, which can dramatically increase the energy density of lithium batteries for EV applications. During past three years, four coherent steps have been taken to solve the coupled mechanical and electrochemical degradation: (1) Developed a comprehensive set of in-situ diagnostic techniques to investigate the coupled mechanical/chemical properties of SEI layer and its impact on lithium striping/plating. (2) Identified failure mechanisms of SEI/Li as a whole electrode system using in-situ electrochemical tools. (3) Established a design strategy of protective coatings on Li metal to extend the cycle life Li meal electrode. (4) Developed novel surface coatings as the artificial SEI layer to protect Li metal and significantly extend cycle life. During past 3-year budget period, we have published over 16 peer-reviewed paper, filed 7 patents, and given over 30 invited talks. 5 graduated students and 2 postdocs were supported by this project.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Editors’ Choice—Ionomer Side Chain Length and Equivalent Weight Impact on High Current Density Transport Resistances in PEMFC Cathodes

Cell voltage at high current densities (HCD) of an operating proton-exchange membrane fuel cell (PEMFC) suffers from losses due to the local-O 2 and bulk-H + transport resistances in the cathode catalyst layer (CCL). Particularly, the interaction of perfluorosulfonic acid (PFSA) ionomer with the carbon supported platinum catalyst plays a critical role in controlling reactant transport to the active site. In this study, we perform a systematic analysis of the side chain length and equivalent weight (EW) of PFSA ionomers on the CCL transport resistances. Ex situ measurements were carried out to quantify the ionomer characteristics such as the molecular weight, proton conductivity and water uptake. Nanomorphology of ionomers cast as 60–120 nm thin-films is characterized using grazing-incidence X-ray scattering. In situ fuel cell electrochemical diagnostic measurements were carried out to quantify the reactant (H + /O 2 ) transport properties of the CCL. Ionomer EW was found to play a major role with decreasing EW yielding higher proton conductivity and water uptake that led to lower bulk-H + and local-O 2 transport resistances in the CCL. Finally, a 1D-semi-empirical performance model has been developed to quantify the impact of ionomer EW on cell voltage loss factors.

08 HYDROGEN↗
DOE OSTI2020

Influence of Coating Method on the Performance of Roll-to-Roll Coated PEM Fuel Cell Catalyst Layers

As production of fuel cell vehicles and power systems increases there is a need to understand the process science of fuel cell manufacturing. Industrial production of polymer electrolyte membrane fuel cell (PEMFC) electrodes will rely on continuous roll-to-roll (R2R) coating methods to meet the rates needed for mass production. There are a variety of coating methods that could be used to coat catalyst layers. The different physics of each method may result in different morphologies and performance. Here we present the results of a study comparing fuel cell catalyst layers coated using two R2R coating methods: slot-die and gravure. These two methods were selected because the physics of applying the liquid to the substrate is very different between the two cases. Pt/C catalysts layers were coated directly onto carbon-fiber gas diffusion media to create gas diffusion electrodes (GDEs), without the use of a decal transfer process. These GDEs were assembled into membrane electrode assemblies (MEAs) by hot pressing to Nafion membranes. In situ performance and other electrochemical diagnostics were used to determine the influence of coating method on catalyst layer electrochemical properties. Electron microscopy was utilized to understand the influence of coating method on electrode morphology and its influence on electrochemical properties. We also explored the influence of solvent ratio to understand the potential coupling between ink formulation and coating methodology.

DIRECT ENERGY CONVERSION,MATERIALS SCIENCE↗
NASA NTRS2004

Manipulation of Microenvironment with a Built-in Electrochemical Actuator in Proximity of a Dissolved Oxygen Microsensor

Abstract - Biochemical sensors for continuous monitoring require dependable periodic self- diagnosis with acceptable simplicity to check its functionality during operation. An in situ self- diagnostic technique for a dissolved oxygen microsensor is proposed in an effort to devise an intelligent microsensor system with an integrated electrochemical actuation electrode. With a built- in platinum microelectrode that surrounds the microsensor, two kinds of microenvironments, called the oxygen-saturated or oxygen-depleted phases, can be created by water electrolysis depending on the polarity. The functionality of the microsensor can be checked during these microenvironment phases. The polarographic oxygen microsensor is fabricated on a flexible polyimide substrate (Kapton) and the feasibility of the proposed concept is demonstrated in a physiological solution. The sensor responds properly during the oxygen-generating and oxygen- depleting phases. The use of these microenvironments for in situ self-calibration is discussed to achieve functional integration as well as structural integration of the microsensor system.

Kim, Chang-Soo↗
DOE OSTI2026

Identifying Critical Electrode Metrics for Efficient, Selective CO 2 Electrochemical Conversion

Low-temperature electrochemical CO 2 reduction (CO 2 R) in zero-gap membrane electrode assembly (MEA) reactors presents a scalable route to fuels and carbon utilization. However, performance at industrially relevant current densities hinges on mesoscale catalyst layer integration, particularly at the ionomer|catalyst interface. Here, we demonstrate a generalizable in situ electrochemical impedance spectroscopy (EIS) method. We utilize this technique to decouple electrode-level parameters that are correlated to the overall MEA performance. By performing this ex situ EIS method on CO 2 -to-CO catalyst-coated membranes with systematically varied ionomer-to-catalyst (I:C) ratios, we reveal a pronounced dependence of performance, ion transport resistance, and catalyst utilization on the I:C ratio as well as the electrode conditioning. We demonstrate that an optimal I:C ratio exists at which ion transport resistance is minimized and Faradaic efficiency for CO production is maximized. Beyond the electrodes examined, here we compare ion transport resistance to MEA selectivity/Faradaic efficiency obtained in prior studies, revealing a clear correlation between the two. These results suggest that ion transport resistance within the catalyst layer may be a quantitative predictor of MEA performance which underscores the importance of mesoscale integration in achieving scalable CO 2 R technologies.

08 HYDROGEN↗
DOE OSTI2025

Degradation of Fuel Cell Membrane Electrode Assemblies from Buses Operated More than 25,000 h

This study investigates the performance losses and degradation of proton-exchange-membrane fuel-cell stacks taken from the Alameda Contra Costa Transit District (AC Transit) bus system (Alameda and Contra Costa counties, California, United States) that were operated for over 25,000 h. Here, we focus on the origin of differences in electrochemical performance between beginning-of-life (BOL) and end-of-life states as well as diagnostic data acquired during the lifetime of the buses. In doing so, we employ in- and ex- situ characterization methods such as polarization curves, electrochemical impedance spectroscopy, electron microscopy, and X-ray characterization. Uniform degradation of the catalyst layer including Pt agglomeration/migration and electrode thinning was observed in all of the post-teardown measurements compared to BOL materials resulting from years of field operation. Despite these changes, the measured post-teardown performance suggests a sufficient output for the expected load, which indicate factors other than degradation of the membrane-electrode assemblies (MEAs) are likely responsible for the decommissioning of the stacks. The findings indicate that these MEA materials can enable long lifetime in fuel-cell vehicles, if the MEAs are not subjected to adverse operating conditions. The results also highlight the need for more in-vehicle diagnostics to maximize the lifetime of fuel cell vehicle (FCV) powerplants.

25 ENERGY STORAGE↗
DOE OSTI2019

Elucidation of Fe-N-C electrocatalyst active site functionality via in-situ X-ray absorption and operando determination of oxygen reduction reaction kinetics in a PEFC

In the past decade the notable effort placed on improving intrinsic electrochemical kinetics of platinum group metal (PGM)-free electrocatalysts for the oxygen reduction reaction (ORR) has led to a significant improvement in both performance and understanding of this class of electrocatalysts. However, a limited amount of this development and understanding has been undertaken using operando electrochemical diagnostics at the membrane electrode assembly (MEA) level. In this work, the operando ORR kinetics on an atomically dispersed iron-nitrogen-carbon ((AD)Fe-N-C) PGM-free electrocatalyst have been examined to extract the reaction order and the activation energy of the ORR. The experiments were carefully designed to ensure the stability/predictability of the electrocatalyst during the data collection process and thus validate the relevance of the values obtained for the aforementioned parameters. A kinetic model that considers a potential-dependent availability of active sites (θ) is proposed. Active site availability is shown to be a function of both the change in the oxidation state (nR) and the redox potential at which the metal center transitions from a higher oxidation state to a lower one (). The resulting model fitting parameters for nR and (0.71 and 0.788 V, respectively) obtained from the analysis of operando data correlate well with those from in situ X-ray absorption near edge structure measurements (nR=0.57) and in situ cyclic voltammetry measurements (0.75 V < <0.8 V) in the MEA environment. The resulting model provides an excellent fit of MEA performance across the range of pressures, temperatures, and potentials under which the data were collected.

Activation energy↗
DOE OSTI2026

Prelithiated SiO x /Graphite-NMC811 Cells: Capacity Loss, Impedance Rise and Hidden Degradation Pathways Revealed Using Three-Electrode Diagnostics

Electrodes containing SiO x /graphite (Gr) materials are attractive as anodes for high-energy lithium-ion batteries. However, their mechanical deformation, electrochemical response, and impedance evolution during long-term cycling are strongly coupled, complicating accurate diagnosis of performance fade mechanisms. In this work, the behavior of electrochemically prelithiated SiO x /Gr anodes paired with NMC811 cathodes is systematically investigated using techniques that include in-situ dilatometry, three-electrode electrochemistry, and multiscale post-cycling microscopy. The SiO x /Gr electrode exhibits a maximum expansion of 49% upon lithiation to 10 mV vs Li + /Li, with 84% of the expansion and 91% of the capacity being reversible. In full cells, relatively stable cycling with only 12% capacity fade over 500 cycles is observed. Three-electrode experiments reveal cell-level impedance growth, which is dominated by the NMC811 cathode: the SiO x /Gr anode exhibits minimal net impedance rise and an initial impedance decrease at low potentials. Despite this apparent electrochemical stability, cross-sectional SEM, PFIB tomography, and cryo-STEM reveal irreversible anode thickening caused by the accumulation of an inorganic-rich solid electrolyte interphase (SEI) permeating the anode bulk. Electrode potential-shift analysis further demonstrates that Li + ions released from lithium reservoirs in the prelithiated anode mask true lithium inventory loss during aging. These results demonstrate that low-expansion SiO x /Gr anodes can simultaneously exhibit favorable cycling and impedance metrics while undergoing substantial, hidden degradation, underscoring the importance of electrode-resolved diagnostics for evaluating prelithiated silicon-based anodes.

25 ENERGY STORAGE↗
DOE OSTI2020

Correlative acoustic time-of-flight spectroscopy and X-ray imaging to investigate gas-induced delamination in lithium-ion pouch cells during thermal runaway

It remains difficult to detect internal mechanical deformation and gas-induced degradation in lithium-ion batteries, especially outside specialized diagnostics laboratories. In this work, we demonstrate that electrochemical acoustic time-of-flight (EA-ToF) spectroscopy can be used as an insightful and field-deployable diagnostic/prognostic technique to sense the onset of failure. A 210 mAh commercial lithium-ion cell undergoing thermal abuse testing is probed with in situ and operando EA-ToF spectroscopy, together with simultaneous fractional thermal runaway calorimetry (FTRC) and synchrotron X-ray imaging. The combination of X-ray imaging and EA-ToF analysis provides new understanding into the through-plane mechanical deformation in lithium-ion batteries through direct visualisation and the acoustic ToF response. Internal structural changes, such as gas-induced delamination, are identified using EA-ToF spectroscopy due to variations in the attenuation and signal peak shifts. This is corroborated using X-ray imaging, demonstrating EA-ToF spectroscopy as a promising technique for detecting onset of battery failure.

25 ENERGY STORAGE↗
DOE OSTI2023

Fundamental Understanding of Dynamic Interfacial Phenomena in Solid State Batteries

Solid-state batteries (SSBs) are considered as one of the most promising battery technologies for resolving the intrinsic limitations of current lithium-ion batteries, such as safety and insufficient energy density. However, the degradation associated with interfaces in SSBs is still a critical issue leading to short cycle life. To get fundamental understanding of the failure mechanism of the interfaces, we first developed a comprehensive set of in situ diagnostic techniques combined with atomic/continuum modeling schemes to investigate and understand the coupled mechanical/chemical degradation associated with dynamic interfacial phenomena in SSBs. Specifically, we focused on in situ observations and characterizations of lithium plating-stripping processes, lithium dendrite formation, interphase formation, and the induced interfacial stresses, as well as the mechanical and electrochemical properties of interfaces and interphases. The final project report first gives an overview of the project background, objectives, technical approaches, and final deliverables for all the budget periods; then follows with a summary on main accomplishments based on main tasks. We particularly would like to highlight some capabilities developed from this project which can also be implemented to our advanced battery development.

25 ENERGY STORAGE↗
NASA NTRS2005

NASA Tech Briefs, June 2005

Topics covered include: Apparatus Characterizes Transient Voltages in Real Time; Measuring Humidity in Sealed Glass Encasements; Adaptable System for Vehicle Health and Usage Monitoring; Miniature Focusing Time-of-Flight Mass Spectrometer; Cryogenic High-Sensitivity Magnetometer; Wheel Electrometer System; Carbon-Nanotube Conductive Layers for Thin-Film Solar Cells; Patch Antenna Fed via Unequal-Crossed-Arm Aperture; LC Circuits for Diagnosing Embedded Piezoelectric Devices; Nanowire Thermoelectric Devices; Code for Analyzing and Designing Spacecraft Power System Radiators; Decision Support for Emergency Operations Centers; NASA Records Database; Real-Time Principal- Component Analysis; Fuzzy/Neural Software Estimates Costs of Rocket- Engine Tests; Multicomponent, Rare-Earth-Doped Thermal-Barrier Coatings; Reactive Additives for Phenylethynyl-Containing Resins; Improved Gear Shapes for Face Worm Gear Drives; Alternative Way of Shifting Mass to Move a Spherical Robot; Parylene C as a Sacrificial Material for Microfabrication; In Situ Electrochemical Deposition of Microscopic Wires; Improved Method of Manufacturing SiC Devices; Microwave Treatment of Prostate Cancer and Hyperplasia; Ferroelectric Devices Emit Charged Particles and Radiation; Dusty-Plasma Particle Accelerator; Frozen-Plug Technique for Liquid-Oxygen Plumbing; Shock Waves in a Bose-Einstein Condensate; Progress on a Multichannel, Dual-Mixer Stability Analyzer; Development of Carbon- Nanotube/Polymer Composites; Thermal Imaging of Earth for Accurate Pointing of Deep-Space Antennas; Modifications of a Composite-Material Combustion Chamber; Modeling and Diagnostic Software for Liquefying- Fuel Rockets; and Spacecraft Antenna Clusters for High EIRP.

Source record↗
DOE OSTI2026

A Lens into the Cu Nanograin by In Situ Vibrational Spectroscopy

Cu-based catalysts are uniquely capable of C-C coupling during electrochemical CO 2 reduction (CO 2 R), yet further mechanistic understanding remains hampered by the lack of spectroscopically resolved descriptors that demonstrate how surface adsorbates emerge and evolve within their catalytic environment. Here, in this study, we correlate in situ surface-enhanced Raman spectroscopy (SERS) and surface-enhanced infrared absorption spectroscopy (SEIRAS) to resolve the potential-dependent dynamics during CO 2 R on Cu nanograin catalysts. By building on previous benchmarking of low overpotential performance and nanograin structural evolution, we offer a diagnostic framework linking vibrational signatures to catalytic function, unveiling which species appear, persist, and turnover as the electrified surface and interfacial environment evolve under bias. The onset of linear CO is marked below -0.45 V, coincident with persistent adsorbed *OH/*O domains beyond the CO 2 R onset. In this context, Cu nanograins serve as a platform to dissect contributions of adsorbate coverage. By carefully dissecting the potential dependence of emergent twin-defect/step CO stretch bands (P1-P2), alongside the prototypical terrace-site CO stretch band (P3), we provide important context for interpreting coupled spectroscopic trends driven by coverage effects and resolve this for the evidently complex nanograin morphology. Together, these observations highlight the intertwined roles of surface stabilization and interfacial flux in steering multicarbon product formation. By directly linking vibrational signatures to catalytic behavior, this work aims to bridge the gap between observation and control and help guide toward a predictive framework of fine-tuned selectivity for CO 2 R.

Fonseca Guzman, Maria V. [University of California↗
DOE OSTI2023

Root Cause Analysis of Degradation in Protonic Ceramic Electrochemical Cell with Interfacial Electrical Sensors Using Data‐Driven Machine Learning

Abstract Protonic ceramic electrochemical cells (PCECs) offer promising paths for energy storage and conversion. Despite considerable achievements made, PCECs still face challenges such as physiochemical compatibility between componenets and suboptimal solid–solid contact at the interfaces between the electrolytes and electrodes. In this study, a novel approach is proposed that combines in situ electrochemical characterization of interfacial electrical sensor embedded PCECs and machine learning to quantify the contributions of different cell components to total degradation, as well as to predict the remaining useful life. The experimental results suggest that the overpotential induced by the oxygen electrode is 48% less than that of oxygen electrode/electrolyte interfacial contact for up to 1171 h. The data‐driven machine learning simulation predicts the RUL of up to 2132 h. The root cause of degradation is overpotential increase induced by oxygen electrode, which accounts for 82.9% of total cell degradation. The success of the failure diagnostic model is demonstrated by its consistency with degradation modes that do not manifest in electrolysis fade during early real operations. This synergistic approach provides valuable insights into practical failure diagnosis of PCECs and has the potential to revolutionize their development by enabling improved performance prediction and material selection for enhanced durability and efficiency.

25 ENERGY STORAGE↗