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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Origins of the change in mechanical strength of silicon/gold nanocomposites during irradiation

Abstract Silicon-based layered nanocomposites, comprised of covalent-metal interfaces, have demonstrated elevated resistance to radiation. The amorphization of the crystalline silicon sublayer during irradiation and/or heating can provide an additional mechanism for accommodating irradiation-induced defects. In this study, we investigated the mechanical strength of irradiated Si-based nanocomposites using atomistic modeling. We first examined dose effects on the defect evolution mechanisms near silicon-gold crystalline and amorphous interfaces. Our simulations reveal the growth of an emergent amorphous interfacial layer with increasing dose, a dominant factor mitigating radiation damage. We then examined the effect of radiation on the mechanical strength of silicon-gold multilayers by constructing yield surfaces. These results demonstrate a rapid onset strength loss with dose. Nearly identical behavior is observed in bulk gold, a phenomenon that can be rooted to the formation of radiation-induced stacking fault tetrahedra which dominate the dislocation emission mechanism during mechanical loading. Taken together, these results advance our understanding of the interaction between radiation-induced point defects and metal-covalent interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Heavily neodymium doped ceria as an effective barrier layer in solid oxide electrochemical cells

10 mol% gadolinium doped ceria (GDC10) is widely used as a barrier layer between oxygen electrode and electrolyte to prevent interfacial reactions. A 50 mol% neodymium doped ceria (NDC50) barrier layer has been proposed and studied in this paper. Symmetrical cells with NDC50 and GDC10 barrier layers, Nd 2 NiO 4+δ (NNO)–Ce 0.5 Nd 0.5 O 2-δ (NDC50) electrode, and YSZ electrolyte have been systematically studied using impedance spectroscopy (EIS) at various temperatures and oxygen partial pressure (pO 2 ). The NDC50 barrier layer has significantly decreased polarization resistance across a wide temperature and pO 2 range compared to the GDC10 barrier layer. The rare earth C-type structure of the NDC50 barrier layer causes barrier free migration of oxygen ions resulting in improved ionic conductivity compared to GDC10. Finally, distribution of relaxation time (DRT) modeling has been used to obtain insights into the electrode processes.

08 HYDROGEN↗
DOE OSTI2024

Development and crystal structures of a potent second-generation dual degrader of BCL-2 and BCL-xL

Overexpression of BCL-xL and BCL-2 play key roles in tumorigenesis and cancer drug resistance. Advances in PROTAC technology facilitated recent development of the first BCL-xL/BCL-2 dual degrader, 753b, a VHL-based degrader with improved potency and reduced toxicity compared to previous small molecule inhibitors. Here, we determine crystal structures of VHL/753b/BCL-xL and VHL/753b/BCL-2 ternary complexes. The two ternary complexes exhibit markedly different architectures that are accompanied by distinct networks of interactions at the VHL/753b-linker/target interfaces. The importance of these interfacial contacts is validated via functional analysis and informed subsequent rational and structure-guided design focused on the 753b linker and BCL-2/BCL-xL warhead. This results in the design of a degrader, WH244, with enhanced potency to degrade BCL-xL/BCL-2 in cells. Using biophysical assays followed by in cell activities, we are able to explain the enhanced target degradation of BCL-xL/BCL-2 in cells. Most PROTACs are empirically designed and lack structural studies, making it challenging to understand their modes of action and specificity. Our work presents a streamlined approach that combines rational design and structure-based insights backed with cell-based studies to develop effective PROTAC-based cancer therapeutics.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Aluminium composites prepared by laser cladding assisted by friction stir processing

Abstract A laser cladding and friction stir processing hybrid method was employed to produce an Al matrix composite layer. The microstructure, phase composition, microhardness and conductivity of the composites were investigated. A laser cladding layer with a thickness of approximately 200 μ m was prepared on a 1060 aluminium plate and it was broken up and distributed on the Al matrix after friction stir processing. The particle/Al interfaces exhibited extremely good interfacial integrity. Microstructural observations revealed that an obvious in situ reaction occurred at the particle/Al interfaces, which effectively improved the bonding between the reinforcement phase and the matrix. TEM analysis and selected area diffraction enabled the identification of the intermetallic compounds and confirmed them to be Al 5 Fe 2 and Al 3 Fe. The average microhardness values of the friction stir processed composites reached approximately 85 HV. The electrical resistivity of the friction stir processed composites is slightly higher than that of the aluminium matrix.

Wei, Yanni (ORCID:0000000244443642)↗
DOE OSTI2020

Development of Lattice-Mismatched GaInAsP for Radiation Hardness

We develop lattice-mismatched GaInAsP as an alternative alloy to pure As-based alloys currently used in III-V multijunction solar cells. Increasing the alloy phosphorous and indium content while maintaining an optimal bandgap may allow high efficiency multijunction devices with increased radiation hardness. Here, 1.0-eV GaInAsP is developed and implemented into single and multijunction solar cell devices. The lattice-mismatched GaInAsP must be grown strain free, and the subcell thickness must be maintained below the thickness where surface-driven phase separation occurs. As observed in transmission electron microscopy and cathodoluminescence imaging, phase separation strengthens in the GaInAsP layer and leads to interfacial defect formation when the cell thickness is too great. We show single junction 1.0-eV Ga 0.5 In 0.5 As 0.7 P 0.3 with excellent carrier collection and a bandgap-voltage offset of 0.40 V. This material quality approaches that of 1.0-eV Ga 0.7 In 0.3 As used in inverted metamorphic multijunction devices, but has increased phosphorus content and consequently is expected to have a higher radiation resistance. We incorporate the 1.0-eV GaInAsP subcell into a 3-junction inverted metamorphic solar cell to test the performance of the subcell in a multijunction. No additional loss is observed upon integration into a multijunction cell: both the carrier collection and voltage of the GaInAsP subcell are unchanged from single junction devices. While further materials development and radiation testing is still required, these preliminary results indicate that lattice-mismatched GaInAsP can be effectively used in multijunction solar cells to replace radiation-soft materials.

14 SOLAR ENERGY↗
DOE OSTI2022

Transmission Electron Microscopy Study on the Effect of Thermal and Electrical Stimuli on Ge2Te3 Based Memristor Devices

Memristor devices fabricated using the chalcogenide Ge 2 Te 3 phase change thin films in a metal-insulator-metal structure are characterized using thermal and electrical stimuli in this study. Once the thermal and electrical stimuli are applied, cross-sectional transmission electron microscopy (TEM) and X-ray energy-dispersive spectroscopy (XEDS) analyses are performed to determine structural and compositional changes in the devices. Electrical measurements on these devices showed a need for increasing compliance current between cycles to initiate switching from low resistance state (LRS) to high resistance state (HRS). The measured resistance in HRS also exhibited a steady decrease with increase in the compliance current. High resolution TEM studies on devices in HRS showed the presence of residual crystalline phase at the top-electrode/dielectric interface, which may explain the observed dependence on compliance current. XEDS study revealed diffusion related processes at dielectric-electrode interface characterized, by the separation of Ge 2 Te 3 into Ge- and Te- enriched interfacial layers. This was also accompanied by spikes in O level at these regions. Furthermore, in-situ heating experiments on as-grown thin films revealed a deleterious effect of Ti adhesive layer, wherein the in-diffusion of Ti leads to further degradation of the dielectric layer. This experimental physics-based study shows that the large HRS/LRS ratio below the current compliance limit of 1 mA and the ability to control the HRS and LRS by varying the compliance current are attractive for memristor and neuromorphic computing applications.

Shallcross, Austin↗
NASA NTRS1986

Thermal and structural stability of cosputtered amorphous Ta(x)Cu(1-x) alloy thin films on GaAs

The characteristics of thin films of Ta-Cu, prepared over a wide range of compositions by cosputter deposition onto GaAs and fused quartz substrates, are studied by X-ray diffraction and van der Pauw resistivity measurement. Results show films to be amorphous over the range of 55-95 at. pct, and show Ta(93)Cu(7) barriers to be effective in preventing Au in-diffusion, with a 3000-A layer remaining unpenetrated after an annealing at 700 C for 20 min. Diffusion of Ga and/or As into amorphous 93 at. pct Ta is found to be more rapid than that of Au, and interfacial reactions were shown to form compounds including Ta3Au, CuAu, TaAs2, and Ga3Cu7 above 700 C.

Oh, J. E.↗
DOE OSTI2023

Interface property–functionality interplay suppresses bimolecular recombination facilitating above 18% efficiency organic solar cells embracing simplistic fabrication

Efficient exciton-to-charge generation from the introduction of non-fullerene acceptors (NFAs) has been an important breakthrough in organic solar cell (OSC) developments. However, low device fill factors (FFs) following significant free charge carrier recombination loss continue to undermine their marketplace potential. Previous studies have successfully uncovered the importance of donor and acceptor domains in promoting charge transport. However, the functionality of donor/acceptor (D/A) interfaces relevant to free charge recombination remains unclear despite such interfaces being present throughout the material. In this work, the disorder-induced uphill bulk-to-D/A interface transport energy landscape is unveiled to enhance the polaron recombination resistance thereby also mitigating the triplet state formation from back charge transfer. In simple words, increasing the interface disorder while keeping the purer domains highly ordered will impart greater bulk-to-interface differential energy which then serves as a recombination energy barrier. Herein, these are made possible by varying the NFA outer side chains from linear alkyls to bulkier 2D phenylalkyls which influence the donor–acceptor interaction and define the interfacial disorder. Meanwhile, the extent of interface disorder without tradeoff in geminate losses is dependent on electrostatics and nanomorphology driving efficient exciton dissociation. By understanding these interplays, remarkable FFs over 80% and power conversion efficiencies (PCEs) above 18% are revealed to remain accessible even with simple binary component device fabrication without additional components/treatments thereby maintaining the scalability. Consequently, the principles uncovered here will serve as the foundation to reach the optimum potential of binary and simple systems, a prerequisite to ultimately realize the most cost-effective OSC design strategies for practical applications.

14 SOLAR ENERGY↗
DOE OSTI2024

Interfacial defect reduction enhances universal power law response in Mo–SiNx granular metals

Granular metals (GMs), consisting of metal nanoparticles separated by an insulating matrix, frequently serve as a platform for fundamental electron transport studies. However, few technologically mature devices incorporating GMs have been realized, in large part because intrinsic defects (e.g., electron trapping sites and metal/insulator interfacial defects) frequently impede electron transport, particularly in GMs that do not contain noble metals. Here, we demonstrate that such defects can be minimized in molybdenum–silicon nitride (Mo–SiN x ) GMs via optimization of the sputter deposition atmosphere. For Mo–SiN x GMs deposited in a mixed Ar/N 2 environment, x-ray photoemission spectroscopy shows a 40%–60% reduction of interfacial Mo-silicide defects compared to Mo–SiN x GMs sputtered in a pure Ar environment. Electron transport measurements confirm the reduced defect density; the dc conductivity improved (decreased) by 10 4 –10 5 and the activation energy for variable-range hopping increased 10×. Since GMs are disordered materials, the GM nanostructure should, theoretically, support a universal power law (UPL) response; in practice, that response is generally overwhelmed by resistive (defective) transport. Here, the defect-minimized Mo–SiN x GMs display a superlinear UPL response, which we quantify as the ratio of the conductivity at 1 MHz to that at dc, Δσ ω ⁠. Remarkably, these GMs display a Δσ ω up to 10 7 , a three-orders-of-magnitude improved response than previously reported for GMs. By enabling high-performance electric transport with a non-noble metal GM, this work represents an important step toward both new fundamental UPL research and scalable, mature GM device applications.

36 MATERIALS SCIENCE↗
NASA NTRS2011

Lightweight, Ultra-High-Temperature, CMC-Lined Carbon/Carbon Structures

Carbon/carbon (C/C) is an established engineering material used extensively in aerospace. The beneficial properties of C/C include high strength, low density, and toughness. Its shortcoming is its limited usability at temperatures higher than the oxidation temperature of carbon . approximately 400 C. Ceramic matrix composites (CMCs) are used instead, but carry a weight penalty. Combining a thin laminate of CMC to a bulk structure of C/C retains all of the benefits of C/C with the high temperature oxidizing environment usability of CMCs. Ultramet demonstrated the feasibility of combining the light weight of C/C composites with the oxidation resistance of zirconium carbide (ZrC) and zirconium- silicon carbide (Zr-Si-C) CMCs in a unique system composed of a C/C primary structure with an integral CMC liner with temperature capability up to 4,200 F (.2,315 C). The system effectively bridged the gap in weight and performance between coated C/C and bulk CMCs. Fabrication was demonstrated through an innovative variant of Ultramet fs rapid, pressureless melt infiltration processing technology. The fully developed material system has strength that is comparable with that of C/C, lower density than Cf/SiC, and ultra-high-temperature oxidation stability. Application of the reinforced ceramic casing to a predominantly C/C structure creates a highly innovative material with the potential to achieve the long-sought goal of long-term, cyclic high-temperature use of C/C in an oxidizing environment. The C/C substructure provided most of the mechanical integrity, and the CMC strengths achieved appeared to be sufficient to allow the CMC to perform its primary function of protecting the C/C. Nozzle extension components were fabricated and successfully hot-fire tested. Test results showed good thermochemical and thermomechanical stability of the CMC, as well as excellent interfacial bonding between the CMC liner and the underlying C/C structure. In particular, hafnium-containing CMCs on C/C were shown to perform well at temperatures exceeding 3,500 F (.1,925 C). The melt-infiltrated CMC-lined C/C composites offered a lower density than Cf/SiC. The melt-infiltrated composites offer greater use temperature than Cf/SiC because of the more refractory ceramic matrices and the C/C substructure provides greater high-temperature strength. The progress made in this work will allow multiple high-temperature components used in oxidizing environments to take advantage of the low density and high strength of C/C combined with the high-temperature oxidation resistance of melt-infiltrated CMCs.

Wright, Matthew J.↗
DOE OSTI2026

Comparative study on the formation of Cr and Ti ohmic contacts to (001) β -Ga 2 O 3

Here, a comparative study of Cr/Au and Ti/Au ohmic contacts on (001) β-Ga 2 O 3 was conducted. The electrical behavior from current-voltage measurements and the interfacial composition and microstructure as determined from high-resolution transmission electron microscopy (TEM) with energy dispersive x-ray analysis were compared for the different contacts at selected points in an annealing series (300–700 °C, 1 min. anneals in N 2 ). Cr/Au contacts became ohmic at temperatures (300–350 °C) approximately 50–100 °C lower than Ti/Au contacts (400–450 °C). Cr/Au and Ti/Au contacts demonstrated optimal ohmic behavior (lowest resistance) when annealed to 450–500 and 500–600 °C, respectively, with Ti/Au contacts yielding a lower total resistance than Cr/Au. Cross-sectional TEM images of Cr/Au contacts annealed at 450 °C revealed the presence of Au nanoclusters at the Ga 2 O 3 interface and CrO x layers at both the top of the contact and the Ga 2 O 3 interface. Whereas TiO x also formed at the top and bottom interfaces in 450 °C-annealed Ti/Au contacts, the TiO x surface layer appeared to be variable in thickness and/or discontinuous, unlike the CrO x surface layer. Au nanoclusters were not detected at the interface in the Ti/Au contacts. The interdiffusion and oxidation observed in both contact metallizations point to the need for diffusion barriers that may allow these contacts to be used in future Ga 2 O 3 -based devices that operate at elevated temperatures.

36 MATERIALS SCIENCE↗
NASA NTRS2023

A Review on the Coalescence of Confined Drops with a Focus on Scaling Laws for the Growth of the Liquid Bridge

The surface–tension-driven coalescence of drops has been extensively studied because of the omnipresence of the phenomenon and its significance in various natural and engineering systems. When two drops come into contact, a liquid bridge is formed between them and then grows in its lateral dimensions. As a result, the two drops merge to become a bigger drop. The growth dynamics of the bridge are governed by a balance between the driving force and the viscous and inertial resistances of involved liquids, and it is usually represented by power–law scaling relations on the temporal evolution of the bridge dimension. Such scaling laws have been well-characterized for the coalescence of unconfined or freely suspended drops. However, drops are often confined by solid or liquid surfaces and thus are a different shape from spheres, which affects their coalescence dynamics. As such, the coalescence of confined drops poses more complicated interfacial fluid dynamics challenges compared to that of unconfined drops. Although there have been several studies on the coalescence of confined drops, they have not been systematically reviewed in terms of the properties and geometry of the confining surface. Thus, we aim to review the current literature on the coalescence of confined drops in three categories: drop coalescence on a solid surface, drop coalescence on a deformable surface, and drop coalescence between two parallel surfaces with a small gap (i.e., Hele-Shaw cell), with a focus on power–law scaling relations, and to suggest challenges and outlooks for future research on the phenomena.

Sangjin Ryu↗
DOE OSTI2025

Interfacial reconstruction effects in insulating double perovskite Nd2NiMnO6/SrTiO3 and Nd2NiMnO6/NdGaO3 thin films

Ferromagnetic insulating (FMI) double perovskite oxides (DPOs) A2BB′O6 with near-room-temperature Curie temperatures are promising candidates for ambient-temperature spintronics applications. To realize their potential, epitaxial stabilization of DPO films and understanding the effect of multiple broken symmetries across the film/substrate interface are crucial. This study investigates ultrathin films of the FMI Nd2NiMnO6 grown on SrTiO3 (STO) and NdGaO3 (NGO) substrates. By comparing growth on these substrates, we examine the influence of polarity and structural symmetry mismatches, which are absent in the NGO system. The interface exhibits immeasurable resistance in both cases. Using synchrotron x-ray diffraction, we show that films have three octahedral rotational domains because of the structural symmetry mismatch with the STO substrate. Furthermore, our coherent Bragg rod analysis of specular x-ray diffraction reveals a significant modification of the out-of-plane lattice parameter within a few unit cells at the film/substrate interface and the surface. This arises from polarity compensation and surface symmetry breaking, respectively. These structural alterations influence the Mn orbital symmetry, a dependence that we further confirm through x-ray linear dichroism measurements. Since the ferromagnetism in insulating DPOs is mediated by orbital-dependent superexchange interactions [Phys. Rev. Lett. 100, 186402 (2008)0031-900710.1103/PhysRevLett.100.186402], our study provides a framework for understanding the evolution of magnetism in ultrathin geometry.

Bhattacharya, Nandana↗
DOE OSTI2020

Fabrication of high-performance gas-diffusion-electrode based membrane-electrode assemblies

This paper demonstrates the fabrication and processing steps required to produce high performance fuel cell membrane electrode assemblies (MEAs) based on spray-coated gas-diffusion electrodes (GDEs). It is demonstrated that coating the catalyst layer with a thin layer of ionomer and then hot pressing the GDEs to the membrane is required to achieve comparable catalyst activity and air performance to catalyst-coated-membrane MEAs. We show that there is a critical amount of ionomer required to achieve maximized performance. Using electron microscopy, we show that the combination of the ionomer overlayer and hot-pressing bonds the catalyst layer to the membrane, increasing the interfacial contact area and quality of this interface. We also find that the ionomer overlayer smooths the surface of the GDE and provides increased contact area between the GDE and the membrane. Additionally, we demonstrate that much less ionomer is required for high-performance than has been previously reported. Through model fitting of electrochemical impedance spectroscopy, we show that this improvement in the catalyst layer - membrane interface reduces the effective catalyst layer resistance, which reduces Ohmic losses and increases catalyst utilization.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2026

Evaluation of high-temperature properties of binary, eutectic Ni-X alloys (X = B, Ca, Ce, La, Y, Zr)

We investigated the high-temperature behavior of binary eutectic nickel-base alloys with low-solubility elements, towards developing alloys with new combinations of structural and functional (e.g. thermal or corrosion) properties. Based on thermodynamic screening, we cast binary near-eutectic Ni-B, Ni-Ca, Ni-Ce, Ni-La, Ni-Y, and Ni-Zr alloys and characterized their microstructure and high-temperature properties. All alloys (except Ni-Ca) contain a fine eutectic microstructure, containing submicron alternating lamellae of γ-Ni and continuous intermetallic phases. The eutectic microstructure did not significantly coarsen at 700°C (except for Ni-B), but measurably coarsened in all alloys at 900°C, most quickly in Ni-B, followed by Ni-Ce, Ni-La, Ni-Y, and Ni-Zr. Coarsening in these alloys occurs by fault migration; diffusion within the intermetallic, and its interfacial energy, likely influence coarsening kinetics. At room-temperature, all alloys possess negligible ductility due to the continuous, brittle intermetallic. At 700 and 900°C, the Ni-Zr alloy showed the best combination of strength and ductility. Oxidation experiments at 900°C on Ni-Zr and Ni-Ce revealed heavy internal oxidation of the continuous intermetallic phase. Overall, the Ni-Zr alloy showed good high-temperature coarsening resistance and strength, though ductility and oxidation resistance require improvement for use in structural applications. Possible routes for improving alloy properties via additive manufacturing are discussed.

Ekaputra, Clement [ORNL] (ORCID:0000000307166479)↗
DOE OSTI2024

Pathway to High Rate Capability in Interconnected Composite Electrolytes: A Case Study with a Single-Ion-Conducting Polymer

In a three-dimensional interconnected polymer/ceramic composite electrolyte (3D composite), both the polymer and ceramic electrolyte phases are individually connected with a polymer-rich surface layer to provide conformal contact with the electrodes. This work investigates how the transference number of the polymer phase affects the electrochemical properties of the 3D composite. Here, we fabricate a 3D composite using a “single-ion” conducting polymer electrolyte (PE), Li 1+x+y Al x Ti 2–x Si y P 3–y O 12 (LICGC) ceramic, and compare its electrochemical properties with the neat polymer, and with a 3D composite made with a dual-ion-conducting PE (we reported previously). Our results reveal that changing the polymer phase from a dual-ion-conducting PE to a single-ion-conducting PE results in a 9-fold increase in the limiting current density, although the interfacial impedance between the polymer and LICGC ceramic remains high (and contributes significantly to the total impedance of the 3D composite). Further, the limiting current density of the 3D composite is dictated by the PE and minimally affected by the ceramic scaffold. The ceramic scaffold, however, helps to ease the concentration gradient buildup within the PE and moderately improves the overall transference number. The LICGC scaffold does not provide any additional Li dendrite resistance due to its high reactivity with Li.

25 ENERGY STORAGE↗
DOE OSTI2026

Heteroepitaxial control of thickness, strain, and domain architecture in few-layer ferroelectric tin monochalcogenides

Thin-film epitaxy and epitaxial strain have been widely exploited to tune domain configurations, switching behavior, and ferroic properties in conventional three-dimensional ferroelectric thin films; however, its application to controlling the properties of two-dimensional (2D) ferroelectrics has remained largely unexplored. Here, using SnX (X = Se, S) as a model system, we demonstrate heteroepitaxial control of thickness, strain state, and domain architecture in few-layer ferroelectric SnX via growth on monolayer MoS2 van der Waals (vdW) templates. Compared with conventional growth, MoS2-templated heteroepitaxy promotes epitaxial alignment, yielding ultrathin SnSe films with improved crystalline quality, full areal coverage, and enlarged lateral dimensions. Strong interfacial epitaxial coupling induces pronounced in-plane strain and stabilizes a hierarchical ferroelastic domain architecture, in which long-range 90° stripe domains are further subdivided into nanoscale rotational variants, as revealed by scanning transmission electron microscopy and synchrotron X-ray microscopy. Piezoresponse force microscopy and second-harmonic polarimetry confirm robust in-plane polarization, while ferroelectricity in SnSe is established through polarization-electric field hysteresis and nonvolatile ferroelectric resistive switching with on/off ratios approaching 1000. A nonvolatile, switchable ferroelectric diode effect further evidences direct coupling between polarization and charge transport. Notably, ferroelectric switchability exhibits a strong thickness dependence and is preserved only below ∼10 layers. This vdW heteroepitaxial strategy is further extended to ferroelectric SnS. The seamless heteroepitaxial integration of 2D ferroelectrics with CMOS-compatible, wafer-scale MoS2 templates provides a general and scalable route for strain-enabled structural and ferroelectric engineering in emerging memory and low-power optoelectronic applications.

Wang, Yueyin↗
DOE OSTI2022

Characterization of the structure and chemistry of the solid–electrolyte interface by cryo-EM leads to high-performance solid-state Li-metal batteries

Solid-state lithium-metal (Li 0 ) batteries are gaining traction for electric vehicle applications because they replace flammable liquid electrolytes with a safer, solid-form electrolyte that also offers higher energy density and better resistance against Li dendrite formation. Solid polymer electrolytes (SPEs) are highly promising candidates because of their tunable mechanical properties and easy manufacturability; however, their electrochemical instability against lithium metal (Li 0 ), mediocre conductivity, and poorly understood Li 0 /SPE interphases have prevented extensive application in real batteries. In particular, the origin of the low Coulombic efficiency (CE) associated with SPEs remains elusive, as the debate continues as to whether it originates from unfavored interfacial reactions or lithium dendritic growth and dead lithium formation. In this work, we use state-of-the-art cryo-electromicroscopy (cryoEM) imaging and spectroscopic techniques to characterize the structure and chemistry of the interface between Li 0 and a polyacrylate-based SPE. Contradicting the conventional knowledge, we find that no protective interphase forms, owing to the sustained reactions between deposited Li dendrites and polyacrylic backbones and succinonitrile plasticizer. Due to the reaction induced volume change, large amounts of cracks form inside the Li dendrites with a stress corrosion-cracking behavior, indicating that Li0cannot be passivated in this SPE system. Based on this observation, we then introduce additive engineering leveraging on the knowledge of liquid electrolytes, and demonstrate that the Li 0 surface can be effectively protected against corrosion using fluoroethylene carbonate (FEC), leading to densely packed Li 0 domes with conformal and stable solid-electrolyte interphases (SEIs) films. Owing to the high room temperature ionic conductivity of 1.01 mS/cm -1 , the high transference number of 0.57 and the stabilized lithium electrolyte interface, this improved new SPE delivers an excellent lithium plating/stripping CE of 99% and 1800 hours of stable cycling in Li||Li symmetric cells (0.2 mA/cm -2 , 1mAh/cm -2 ). Furthermore, this improved cathodic stability along with the high anodic stability enables record high cycle life of >2000 cycles for Li||LiFePO 4 and >400 cycles for Li||LiCoO 2 full cells.

25 ENERGY STORAGE↗