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At least 253 records · Page 14

Cracking Behavior of Irradiated Ex-Plant Materials

The cracking behavior of reactor core internal materials is a key factor for the long-term safety and availability of light water reactors. Subject to high-temperature coolant, thermal and mechanical loading, and neutron irradiation, reactor core internal materials are susceptible to several degradation mechanisms during power operation. To understand the long-term effects of neutron irradiation, irradiated materials harvested from a decommissioned reactor were studied for their cracking susceptibility and fracture resistance. Small compact-tension specimens were machined from different locations on the baffle plates with irradiation doses ranging from 0.06 to 48.5 dpa. Crack growth rate and fracture toughness J-resistance (J-R) curve tests were performed on these specimens in a simulated light water reactor environment, and the fracture morphologies of the tested samples were examined with a scanning electron microscope. All samples behaved similarly under cyclic loading, and no deteriorated corrosion-fatigue behavior was observed in the test environments. Under constant load, no elevated cracking susceptibility was observed either in these samples at low stress intensity factors. However, a rapid cracking behavior featuring very high crack growth rates was observed in several high-dose samples. This rapid crack growth behavior was activated when the applied stress intensity factor, K, was sufficiently high. Once activated, the rapid crack growth remained steady even when the K was lowered to the pre-activation level and stopped only when the K was reduced drastically. Yet, the rapid crack growth could be re-activated repeatedly in these samples by raising the K above the initial activation level. This rapid cracking response may be related to the severe irradiation embrittlement experienced by these samples. The J-R curve tests performed with these samples showed a significant decline in fracture toughness with increasing neutron irradiation. Local cracking at the crack tip facilitated by the severe irradiation embrittlement of this material may be responsible for the rapid crack growth behavior demonstrated by this decommissioned material.

36 MATERIALS SCIENCE↗

Evaluating the Durability of Balance of Systems Components Using Combined-Accelerated Stress Testing

The degradation of photovoltaic (PV) balance of systems (BoS) components is not well-studied, but the consequences include: offline-modules, -strings, -inverters; system shutdown; arc-faults; and fires. A utility provider experienced a ~30% failure rate in their power transfer chain, attributed to branch connectors. Field-failed specimen assemblies were therefore examined, consisting of cable connector, branch connector and discrete fuse components. Unused field-vintage specimens are presently being examined using combined-accelerated stress testing (C-AST) to clarify the most influential environmental stressors as well as the effect of external mechanical perturbation. A benchtop prototype fixture was used to develop the perturbation capability for C-AST. The benchtop experiments were also used to develop the in-situ data acquisition of specimen: current, voltage, and temperature. A significant increase in operating temperature, ~100 deg C from ~40 deg C, and a different failure mode was observed immediately once periodic mechanical perturbation was applied. The current at failure was decreased from 35 A (with failure occurring in the fuses) to 15 A (failure at the male/female metal pin connection). After initial examination using X-ray computed tomography, the external plastic was machined away from failed specimens to allow failure analysis, including the extraction of the internal convolute springs for morphological examination (optical- and electron-microscopy). Chemical composition analysis included: energy-dispersive X-ray spectroscopy, differential scanning calorimetry, and Fourier transform infrared spectroscopy.

balance of systems↗

Electrochemical Imaging of Interfaces in Energy Storage via Scanning Probe Methods: Techniques, Applications, and Prospects

Developing a deeper understanding of dynamic chemical, electronic, and morphological changes at interfaces is key to solving practical issues in electrochemical energy storage systems (EESSs). To unravel this complexity, an assortment of tools with distinct capabilities and spatiotemporal resolutions have been used to creatively visualize interfacial processes as they occur. This review highlights how electrochemical scanning probe techniques (ESPTs) such as electrochemical atomic force microscopy, scanning electrochemical microscopy, scanning ion conductance microscopy, and scanning electrochemical cell microscopy are uniquely positioned to address these challenges in EESSs. We describe the operating principles of ESPTs, focusing on the inspection of interfacial structure and chemical processes involved in Li-ion batteries and beyond. We discuss current examples, performance limitations, and complementary ESPTs. Finally, we discuss prospects for imaging improvements and deep learning for automation. We foresee that ESPTs will play an enabling role in advancing EESSs as we transition to renewable energies.

25 ENERGY STORAGE↗

Predicting Cislunar Orbit Lifetimes from Initial Orbital Elements

The volume of space between Earth’s geosynchronous orbit out to the Moon’s sphere of influence, including the lunar Lagrange points, is crucial for the successful planning and execution of space missions, but not fully understood dynamically. This region is a part of cislunar space. Trajectories through cislunar space are influenced by the gravitational forces of the Sun, Earth, Moon, and other Solar System planets leading to typically unpredictable and chaotic trajectory behavior. It is therefore difficult to predict the stability of an trajectory through cislunar space from a set of initial conditions or orbital elements. We simulate one million cislunar orbits to train a self-organizing map (SOM) to cluster the trajectories and orbits into families based on how long they remain stable within the cislunar space. Using the trained SOM, we are able to predict the stable lifetime of a trajectory through cislunar space from a set of initial orbital elements to within an accuracy of 10% for 8% of simulated trajectories and within 50% for 43% of the simulated trajectories. Clustering in the SOM suggests that a variety of trajectory morphologies have similar lifetimes. Once trained, the SOM can predict the stable lifetime of a given cislunar trajectory within milliseconds. The methods developed in this work enable the rapid identification of stable cislunar orbits and trajectories that could be used for future space exploration. Moreover, the developed SOM method can generate orbital and trajectory lifetime estimates from minimal observational data, such as a single two line element, making it useful for early warning systems and large-scale sensor network operations.

79 ASTRONOMY AND ASTROPHYSICS↗

A novel in vivo mouse intervertebral disc degeneration model induced by compressive suture

Intervertebral disc degeneration (IDD) is the root cause of many musculoskeletal disorders of the spine. However, the etiology of IDD is complex and still not well understood. Animal models of IDD would be useful in deciphering the underlying mechanisms. But the existing animal models have their limitations. Therefore, to establish a novel mouse model that can simulate the human IDD process in vivo, we proposed to carefully circumcise the 2 mm-wide tail skin and then compressively sutured the defect with a simple end-to-end suture to exert excessive pressure on the disc. After 1-week, 2-week, and 4-week compression, the mice were sacrificed and the intervertebral discs were harvested for tissue analysis. The radiological, morphological, and molecular modifications of intervertebral discs were measured to characterize this model. Radiologically, the water content of the intervertebral disc decreased significantly after 2-week compression. Morphologically, the nucleus pulposus showed a decrease in volume and the number of notochordal cells. The compressive suture also broke the balance between anabolic and catabolic enzymes in nucleus pulposus, which led to the remodeling of the extracellular matrix in nucleus pulposus as the content of aggrecan and collagen II decreased. The compressive suture could induce intervertebral discs degeneration in a more reasonable way, which was solely influenced by mechanical loading, as the mice caudal vertebrae still moved freely after the operation. This kind of animal model could be adapted as a reliable in vivo mouse IDD model for the research regarding the etiology and treatments of IDD.

60 APPLIED LIFE SCIENCES↗

Prediction of gas hydrate saturation using machine learning and optimal set of well-logs

We report resistivity and acoustic logs are widely used to estimate gas hydrate saturation in various sedimentary systems using one of the two popular methods ((1) acoustic velocity and (2) electrical resistivity), but the limitations of these two methods are often overlooked, which include (i) well-specific calibration of empirical exponents in the electrical resistivity method, (ii) assumption of known pore morphology for gas hydrates in the acoustic velocity method, and (iii) presence of unknown mineralogy and bulk modulus terms in the acoustic velocity method. NMR-density porosity-derived gas hydrate saturation based on the analysis of the transverse magnetization relaxation time (T2) is considered the most precise method, but acquisition of NMR-based logs is limited at relatively recent drilled sites; additionally, its use in conventional oil and gas reservoirs is not that common due to higher cost and operational deployment limitations associated with acquiring NMR well-logs. This study proposes a new method that predicts gas hydrate saturation (S h ) for any well using porosity, bulk density, and compressional wave (P wave) velocity well-logs with neural network (or stochastic gradient descent regression) without any well-specific calibration and/or other aforementioned shortcomings of the existing methods. The method is developed by examining the underlying dependency between S h and different combinations of well-logs, chosen from 6 routine logs, with 12 different machine learning (ML) algorithms. The accuracy of the proposed method in predicting S h is ~ 84%, which is better than the accuracy of seismic and electrical resistivity methods (≤ 75%) per the results reported by three different studies. The robustness of the method in the specific case of permafrost-associated gas hydrates is demonstrated with well-log data from two wells drilled on the Alaska North Slope.

58 GEOSCIENCES↗

High-fidelity micromechanical modeling of the effects of defects on damage and creep behavior in single tow ceramic matrix composite

Despite the superior properties of ceramic matrix composites (CMCs), their fabrication process generates inevitable defects with high density that significantly influence material integrity and residual useful life. Recent efforts have focused on CMC property prediction and investigation of their different inelastic mechanisms, but very limited work exists on understanding the influence of defects on inelastic responses of CMCs. Here, we introduce a three-dimensional micromechanics computational framework that includes experimentally informed material microstructure and architectural variabilities to investigate CMC response in the presence of manufacturing-induced defects. A developed microstructure generation algorithm is used to generate the representative volume elements in the micromechanics models from complex material morphology information obtained from extensive characterization studies of C/SiNC and SiC/SiNC CMCs. A fracture mechanics-informed matrix damage model is reformulated, in which the model considers the growth of porosity and microcracks in the as-received material. A progressive fiber damage model as well as Orthotropic viscoplasticity creep formulation are also utilized for the study. This methodology is implemented within the micromechanics framework to investigate the complex temperature- and time-dependent load transfer and damage mechanisms of CMCs under operation loading conditions. The developed framework explores the influence of as-received defects on the damage and creep behavior in service conditions. It also provides new insights into the effect of size, shape, distribution, and location of these defects on material response. The framework is then calibrated with unidirectional CMC minicomposite results available in the literature.

36 MATERIALS SCIENCE↗

Preliminary Characterization and Evaluation on FFF Manufactured 316H and ODS Steels

The Advanced Materials and Manufacturing Technology (AMMT) program develops cross-cutting technologies in support of a broad range of nuclear reactor technologies and maintains U.S. leadership in materials and manufacturing technologies for nuclear energy applications. The overarching vision of AMMT is to accelerate the development, qualification, demonstration, and deployment of advanced materials and manufacturing technologies to enable reliable and economical nuclear energy. Solid-state advanced manufacturing techniques can overcome some of the challenges in liquid-based additive manufacturing (AM) processes and should therefore be considered in material design and manufacturing as well. The work presented in this report forms part of a study on solid-state AM techniques of 316 stainless steels (SS) and oxide dispersion strengthened (ODS) steel components and supports the vision and goals of the AMMT program relevant to accelerate the development and deployment of advanced manufacturing processes. Achieving this can provide a safety improvement through larger safety margins, economic benefit for higher efficiency during operation, and a cost reduction through more effective manufacturing processes and less waste. This study provides preliminary information on development of the fused-filament fabrication (FFF) process using different powder types to demonstrate the sensitivity, and therefore the characterization of these sample components. The full solid-state manufacturing feasibility study will be completed and reported in a final feasibility evaluation during 2025. The study investigation used two 14YWT ODS powder batches, which provided information and the effect of different powder morphologies on manufacturability. The two 316SS powders demonstrated the effect of powder size on the manufacturability using FFF. Two product forms, namely a honeycomb structure and flat samples, were manufactured to demonstrate the flexibility of product form.

36 MATERIALS SCIENCE↗

Biofouling of filtration membranes in wastewater reuse: In situ visualization with confocal laser scanning microscopy

The filtration membranes utilized in advanced treatment of municipal wastewater are prone to biological fouling. Permeability loss and water recovery limitations due to fouling necessitate additional pretreatment and membrane cleaning, which raise the cost of water reuse. Better fouling mitigation calls for a deeper understanding of biofilm behavior on water reuse membranes. This study uses confocal microscopy to monitor biofouling under realistic conditions. To simulate water reuse, a miniature flow cell with microfiltration and ultrafiltration membranes was operated under typical filtration conditions using secondary effluent from California's East Bay Municipal Utility District. The growing biofilms were stained for extracellular polymeric substances and live and dead cells, and they were monitored in situ under filtration conditions with a confocal laser scanning microscope to produce 2-D and 3-D images. In situ image series revealed biofilm growth and removal processes including internal and external fouling, extracellular polymeric substance production, wrinkling, delamination, and film re-deposition. Additionally, changes in biofilm morphology between in situ and ex situ images highlighted limitations of ex situ imaging. Here, these results provide insight into the physical and biological mechanisms of biofouling in hopes of informing the development of improved techniques for biofouling mitigation.

ultrafiltration↗

The quenching of galaxies, bulges, and disks since cosmic noon

Here, we present an analysis of the quenching of star formation in galaxies, bulges, and disks throughout the bulk of cosmic history, from z = 2 – 0. We utilise observations from the Sloan Digital Sky Survey and the Mapping Nearby Galaxies at Apache Point Observatory survey at low redshifts. We complement these data with observations from the Cosmic Assembly Near-Infrared Deep Extragalactic Legacy Survey at high redshifts. Additionally, we compare the observations to detailed predictions from the LGalaxies semi-analytic model. To analyse the data, we developed a machine learning approach utilising a Random Forest classifier. We first demonstrate that this technique is extremely effective at extracting causal insight from highly complex and inter-correlated model data, before applying it to various observational surveys. Our primary observational results are as follows: at all redshifts studied in this work, we find bulge mass to be the most predictive parameter of quenching, out of the photometric parameter set (incorporating bulge mass, disk mass, total stellar mass, and B/T structure). Moreover, we also find bulge mass to be the most predictive parameter of quenching in both bulge and disk structures, treated separately. Hence, intrinsic galaxy quenching must be due to a stable mechanism operating over cosmic time, and the same quenching mechanism must be effective in both bulge and disk regions. Despite the success of bulge mass in predicting quenching, we find that central velocity dispersion is even more predictive (when available in spectroscopic data sets). In comparison to the LGalaxies model, we find that all of these observational results may be consistently explained through quenching via preventative ‘radio-mode’ active galactic nucleus feedback. Furthermore, many alternative quenching mechanisms (including virial shocks, supernova feedback, and morphological stabilisation) are found to be inconsistent with our observational results and those from the literature.

79 ASTRONOMY AND ASTROPHYSICS↗

Stochastic generation of electrolyzer anode catalyst layers

Here, we introduce a stochastic methodology to reproduce the complex pore structure observed in commercial iridium catalyst layers. This method preserves the α pore (pores smaller than 250 nm) and β pore (pores greater than or equal to 250 nm) regions of the catalyst layer. The morphology of the generated materials was validated by comparing the pore size distributions of generated materials against those obtained from commercial materials imaged using x-ray nano computed tomography. We further demonstrate that the pore size distributions of the generated materials are statistically indistinguishable from the imaged catalyst layers, indicating that the stochastic methodology is capable of accurately reproducing catalyst layer morphology. Pore network modelling was conducted on the generated catalyst materials to simulate single-phase permeability, electrical conductivity, and ionic conductivity, and these properties were found to be within experimentally measured ranges for electrolyzer catalyst layers. Additionally, simulations were performed on the generated materials with varying ionomer and iridium catalyst loadings. As the ionomer loading is added, proton conductivity increases exponentially, which demonstrates the importance of optimizing ionomer loading, considering that these effects will be exacerbated in the hydration and temperature conditions of operating electrolyzers. The stochastic material generation method presented in this work is a powerful tool for the development of novel low loading catalyst layers, where the effect of various structural parameters on electrolyzer performance characteristics can be explored.

36 MATERIALS SCIENCE↗

Fabrication of a composite anion exchange membrane with aligned ion channels for a high-performance non-aqueous vanadium redox flow battery

Fabrication of high-conductivity ion exchange membranes (IEMs) is crucial to improve the performance of non-aqueous vanadium redox flow batteries (NAVRFBs). In the present work, anion exchange membranes with high-conductivity were fabricated by aligning ion channels of the polymer electrolyte impregnated in porous polytetrafluoroethylene (PTFE) under electric fields. It was observed that the ion channels of the polymer electrolyte were uniformly orientated in the atomic-force microscopy image. Its morphological change could minimize detouring of the transport of BF 4 - ions. The results showed through-plane conductivity was improved from 12.7 to 33.1 mS cm -1 . The dimensional properties of the fabricated membranes were also enhanced compared with its cast membrane owing to the reinforcing effect of the substrate. Especially, the NAVRFB assembled with the optimized membrane showed increased capacities, with a 97% coulombic efficiency and 70% energy efficiency at 80 mA cm -2 . Furthermore, the optimized membrane made it possible to operate the NAVRFB at 120 mA cm -2 . Its operating current density was 120 times higher than that of a frequently used AHA membrane for RFBs.

25 ENERGY STORAGE↗

Universal scaling laws of keyhole stability and porosity in 3D printing of metals

Metal three-dimensional (3D) printing includes a vast number of operation and material parameters with complex dependencies, which significantly complicates process optimization, materials development, and real-time monitoring and control. We leverage ultrahigh-speed synchrotron X-ray imaging and high-fidelity multiphysics modeling to identify simple yet universal scaling laws for keyhole stability and porosity in metal 3D printing. The laws apply broadly and remain accurate for different materials, processing conditions, and printing machines. We define a dimensionless number, the Keyhole number, to predict aspect ratio of a keyhole and the morphological transition from stable at low Keyhole number to chaotic at high Keyhole number. Furthermore, we discover inherent correlation between keyhole stability and porosity formation in metal 3D printing. By reducing the dimensions of the formulation of these challenging problems, the compact scaling laws will aid process optimization and defect elimination during metal 3D printing, and potentially lead to a quantitative predictive framework.

42 ENGINEERING↗

X-ray Computed Tomography of Irradiated and Unirradiated AGR-3/4 Compacts

X-ray Computed Tomography (XCT) has been utilized to image and characterize compacts from the combined third and fourth irradiation of the Advanced Gas Reactor (AGR) Program, AGR-3/4, fuel. The experiment contained tristructural isotropic (TRISO)-coated fuel particles as well as designed-to-fail (DTF) fuel particles. Two irradiated compacts, representing the lower and higher range of AGR-3/4 burnup (4.85% and 14.92% fissions per initial heavy metal atom FIMA) were examined. These represent the first known highly irradiated TRISO fuel compacts to be examined via X-ray CT. Additionally, two unirradiated compacts from the same production batch as the examined irradiation compacts were also imaged for a baseline comparison. As XCT of irradiated TRISO compacts is not a commonly implemented characterization technique, a significant portion of the report focuses on developed methodology and imaging conditions. A specialized sample shielding device was developed and fabricated specifically to limit received dose to staff during sample preparation for XCT and to minimize excess gamma radiation dose to sensitive electronic components with the utilized X-ray system. Significant penetration through the uranium oxycarbide fuel kernels by significantly hardening the X-ray beam with specialized proprietary filters acquired from Carl Zeiss NTS Ltd. The filter utilized resulted in an average X ray photon energy of ~110 keV which approaches uranium’s K-edge (~115 keV), maximizing penetration for a microfocus X-ray source. The gamma-radiation emitted from the irradiated AGR-3/4 TRISO compacts, has the same properties and mechanisms for interaction with matter as X-rays, thus the detection of gamma-radiation by the utilized X-ray detectors was initially a concern. However, although ?-rays did produce an observable signal on the X-ray detector, its contribution to the overall imaging results appeared negligible upon 3D reconstruction. The neglibile impact on the resulting 3D reconstructed volumes were likely the result of: (1) a significantly lower detection efficiency for ?-rays relative to X-rays; (2) An X-ray flux at the detector several orders of magnitude higher than that of the impinging ?-rays from the irradiated compacts. These results suggest that irradiated compacts with significantly higher radiation fields can be examined in the future if an acceptable route for sample handling and preparation can be determined. Additionally, the 3D imaging results of XCT can provide a valuable means of assessing compacts. While in many ways complimentary to traditional post irradiation examination techniques such as optical ceramography, XCT can provide additional insight into compact features traditionally difficult to discern directly from cross-sectional imaging alone. Preliminary analyses on kernel size, morphology (aspect ratio and sphericity), and kernel orientation were presented. Sphericity, a simple morphological shape descriptor, was utilized to screen for kernel extrusions within the high burnup compact. The number of kernel extrusions identified via XCT represented an approximate two-fold increase from the quantity of extruded particles observed (via optical ceramography) in adjacent compacts from the same irradiation capsule. While numerical analysis of the compact datasets was highly preliminary, initial results show promise for providing complimentary metrics to current AGR-3/4 PIE and potentially additional insight into the processes driving TRISO fuel degradation during reactor operation. Additional analyses to be performed at a later date include a more detailed examination of kernel size, kernel sphericity (and observed kernel extrusions), and sphericity. Given all particles can be observed in a single data volume possible correlation of spatial position with observed kernel features will also be made at a later date.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tailoring the γ-γ'-γ" dual superlattice microstructure of INCONEL® 725 by high temperature aging and Nb/Ta additions for superior creep properties

Next-generation energy systems require superior resistance to creep deformation due to the considerably prolonged exposure times at operating stress and temperature. To improve the elevated temperature properties of INCONEL® 725 (IN725), a corrosion resistant alloy, several variants with different Ti/Al ratio and judicious amounts of Nb and Ta were made. Furthermore, a high temperature aging (HTA) heat treatment, designed to promote favorable precipitate phase formation, was explored. These adjustments allowed to tailor the amount and type of precipitate strengthening which led to significant increases in time to failure. The Ti/Al ratio was used to favor the formation of γ' or γ" precipitates. Compact morphology precipitates, consisting of γ' precipitates surrounded by a γ" shell, were formed in alloys with a low Ti/Al ratio. The HTA increased the creep life of various alloy formulations up to a maximum improvement of 371% as compared to the standard aging heat treatment. The Nb and Ta additions had a similar effect on increasing creep life by promoting and stabilizing γ" precipitation. The positive effect of the additions was even more pronounced when coupled with the HTA. A phase stability study with up to 10,000 h exposure at 700°C revealed that the compact morphology helped in slightly reducing coarsening of the γ' precipitates, although the effect on creep was not significant. The findings of this study enable design of dual superlattice alloys through microstructural engineering that yields superior performance and can be applied to a wide range of alloys in the IN718 and derivatives family.

Antonov, Stoichko↗

The influence of electrode crack dimensions on the durability of polymer electrolyte membrane fuel cells

Electrode cracks in polymer electrolyte membrane fuel cells (PEMFCs) are correlated with early onset failures. Here, in this work we investigate the influence of cracked gas diffusion electrodes (GDEs) on the durability of the membrane electrode assembly (MEA) using a combined chemical-mechanical accelerated stress test (AST). Electrode crack dimensions were systematically tuned using ink formulations and material selection strategies. A parameter to describe the crack width areal density (Φ CW ) was used to quantify the degree of discontinuity in the electrode surfaces. Open circuit voltage (OCV) transient analyses were used to benchmark and characterize the failure mechanisms in the MEAs as a function of the Φ CW . While smaller electrode-level cracks, on the order of microns, yielded a 28 % decrease in operating lifetime, larger cracks that propagated from a discontinuous, microporous layer (MPL) coating, decreased the operating lifetime by 56 %. This work emphasizes the need for material processing strategies that consider defect tolerances to limit membrane failures in PEMFCs.

08 HYDROGEN↗

Deciphering electrocatalysts with multimodal operando approaches

Here, the electrocatalytic processes of a copper catalyst during nitrate electroreduction are unveiled by correlated operando microscopy and spectroscopy. Catalysts are vital to the modern chemical industry, yet their development has largely relied on trial-and-error approaches. Optimizing catalysts requires a fundamental understanding of their structure–chemical property behaviour under operational conditions. However, operando characterization remains challenging, especially for reactions occurring in the complex and dynamic liquid environments of electrochemical systems. Over the past decade, the rapid development of in situ and operando environmental transmission electron microscopy (ETEM) and microelectromechanical system (MEMS)-based closed-cell holders, enabling environmental studies within the vacuum environment of transmission electron microscopy (TEM), has substantively advanced understanding of heterogeneous catalysis, notably for gas-phase reactions. In situ ETEM enables the direct observation of the catalyst evolution in terms of structure, morphology and chemical state at the nano-to-atomic scale, providing insights into their correlation with catalytic performance.

36 MATERIALS SCIENCE↗

Nonpassivated Silicon Anode Surface

A stable solid electrolyte interphase (SEI) has been proven to be a key enabler to most advanced battery chemistries, where the reactivity between the electrolyte and the anode operating beyond the electrolyte stability limits must be kinetically suppressed by such SEIs. The graphite anode used in state-of-the-art Li-ion batteries presents the most representative SEI example. Because of similar operation potentials between graphite and silicon (Si), a similar passivation mechanism has been thought to apply on the Si anode when using the same carbonate-based electrolytes. Herein, we found that the chemical formation process of a proto-SEI on Si is closely entangled with incessant SEI decomposition, detachment, and reparation, which lead to continuous lithium consumption. Using a special galvanostatic protocol designed to observe the SEI formation prior to Si lithiation, we were able to deconvolute the electrochemical formation of such dynamic SEI from the morphology and mechanical complexities of Si and showed that a pristine Si anode could not be fully passivated in carbonate-based electrolytes.

25 ENERGY STORAGE↗