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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 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Optimized Incorporation of Furan into Diketopyrrolopyrrole-Based Conjugated Polymers for Organic Field-Effect Transistors

Flexible electronics have received considerable attention in the past decades due to their promising application in rollable display screens, wearable devices, implantable devices, and other electronic applications. Here, in particular, conjugated polymers are favored for flexible electronics due to their mechanical flexibility and potential for solution-processed fabrication techniques, such as blade-coating, roll-to-roll printing, and high-throughput printing allowing for high-performance transistor devices. Thiophene is the prevailing conjugated unit to construct these conjugated polymers due to its favorable electronic properties. On the other hand, furans are among the few conjugated moieties that are easily derived from bio renewable resources. To promote sustainability, we selectively introduced furan into the conjugated backbone of a high-mobility polymer scaffold and systematically studied the effect on the microstructure and charge transport. We show that partially and selectively replacing thiophene units with furan can yield nearly comparable performance compared to the all-thiophene polymer. This strategy offers an improvement in the sustainability of the polymer by incorporating bio-sourced furan without sacrificing the high-performance characteristics. Meanwhile, polymers with incorrect or complete furan incorporation show reduced mobilities. This work serves to develop coherent structure–morphology–performance relationships; such knowledge will establish guidelines for the future development of sustainable, furan-based conjugated materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

High-throughput screening to predict highly active dual-atom catalysts for electrocatalytic reduction of nitrate to ammonia

Ammonia is an essential chemical owing to its importance in fertilizer production and other industrial applications. Electrocatalytic nitrate reduction to ammonia (NO 3 RR) holds great promise for low-temperature ammonia production while simultaneously addressing nitrate-based environmental concerns. To provide the mechanistic understanding needed to design an effective electrocatalyst, we systematically investigated the catalytic performance of metal-based dual-atom catalysts (DACs) anchored on two-dimensional (2D) expanded phthalocyanine (Pc) for NO 3 RR. We found that NO 3 RR can efficiently produce ammonia on Cr 2 -Pc, V 2 -Pc, Ti 2 -Pc, and Mn 2 -Pc surfaces with low limiting potentials of – 0.02, – 0.25, – 0.34, and – 0.41 V RHE , respectively. Moreover, using the free energy difference of *NO 3 - and *H as a descriptor, we found that the hydrogen evolution reaction is significantly suppressed on the DAC surface due to an ensemble effect in which the two metal atoms cooperate to selectively form ammonia. We performed high-throughput screening to develop an efficient metal-based DAC for NO 3 - reduction, followed by a mechanistic study to elucidate the NO3RR pathway on the DAC. Finally, this work provides design information for advancing sustainable ammonia synthesis under ambient conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Multi-service battery energy storage system optimization and control

Battery energy storage systems (BESS) have become fundamental part of modern power systems due to their capability to provide multiple grid services. As the renewable penetration increases, BESS procurement is also expected to increase where it is envisioned to play a systematic and strategical role in power systems planning and operation. Hence, in this paper we present a multiple grid service procurement and operation for BESS - ranging from energy arbitrage, reserve/regulation services, power factor correction, and demand management. The proposed framework considers an optimal multi-temporal dimension, designed to be operable for both planning and real-time operation. Moreover, non-linearity inherent to BESS services and uncertainty associated to market forecasts variables are addressed using techniques such as polyhedral norms and robust optimization approaches. Here, the developed model is tested using a utility-scaled BESS and the obtained results show the effectiveness of the systematic BESS multi-service planning and operation approach.

25 ENERGY STORAGE↗
DOE OSTI2026

Effects of Dissolution Regimes on Flow Channelization and Solute Transport in 3D Fracture Networks: Insights From Graph‐Based Reactive Transport Modeling

We investigate how mineral dissolution reshapes flow pathways and solute transport in three‐dimensional discrete fracture networks using a computationally efficient graph‐based reactive transport model. The DFNs are inspired by field‐site observations of fractured carbonate and represent realistic connectivity and structural heterogeneity. Flow is simulated with the Reynolds equation, and dissolution follows first‐order kinetics with diffusive limitations captured through an effective mass‐transfer coefficient. By systematically varying two key dimensionless parameters, the effective Damköhler number (Da), governing reaction versus advection rates, and a transport parameter (Da), analogous to the Thiele modulus, distinct flow channelization regimes emerge: mildly channelized at low G, highly channelized at intermediate Da, and extreme wormhole formation at high Da and low G. Eulerian and Lagrangian analyses, including breakthrough curves, particle tortuosity, dispersivity, and flow channeling indicators quantitatively characterize the progression of dissolution‐driven network restructuring. Across all regimes, initial fracture heterogeneity persists. The results underscore how the interplay between this initial structure, advection, reaction, and diffusion critically shapes subsurface flow pathways, with implications for applications ranging from groundwater remediation to enhanced geothermal systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

First results from the search for muon neutrino disappearance with ICARUS

After successful operation at LNGS and a major upgrade at CERN, the 760-ton ICARUS T600 detector has been running at Fermilab since 2020, collecting neutrino interactions from the BNB and NuMI beams. In late 2025, ICARUS reached five years of continuous data taking, demonstrating the maturity of large-scale LAr-TPC technology and its relevance for future experiments such as DUNE. This contribution presents the first ICARUS search for muon-neutrino disappearance in the BNB. Charged-current 1μNp events selected from 2022–2023 data are compared to simulations and interpreted, for the first time, within a two-neutrino approximation of the 3+1 sterile-neutrino model, including systematic uncertainties from flux, interaction, and detector effects. Although currently limited by systematic uncertainties, this first oscillation analysis probes the parameter space suggested by existing νμ-disappearance results and lays the groundwork for future SBN combined analyses with SBND, which will significantly improve sensitivity to sterile-neutrino scenarios.

Artero Pons, Maria [Padua U.; INFN, Padua]↗
DOE OSTI2026

First results from the search for muon neutrino disappearance with ICARUS

After successful operation at LNGS and a major upgrade at CERN, the 760-ton ICARUS T600 detector has been running at Fermilab since 2020, collecting neutrino interactions from the BNB and NuMI beams. In late 2025, ICARUS reached five years of continuous data taking, demonstrating the maturity of large-scale LAr-TPC technology and its relevance for future experiments such as DUNE. This contribution presents the first ICARUS search for muon-neutrino disappearance in the BNB. Charged-current 1μNp events selected from 2022–2023 data are compared to simulations and interpreted, for the first time, within a two-neutrino approximation of the 3+1 sterile-neutrino model, including systematic uncertainties from flux, interaction, and detector effects. Although currently limited by systematic uncertainties, this first oscillation analysis probes the parameter space suggested by existing νμ-disappearance results and lays the groundwork for future SBN combined analyses with SBND, which will significantly improve sensitivity to sterile-neutrino scenarios.

Artero Pons, Maria [Padua U.; INFN, Padua]↗
DOE OSTI2026

First Results from the Search for Muon-Neutrino Disappearance with the ICARUS Detector

After successful operation at LNGS and a major upgrade at CERN, the 760-ton ICARUS T600 detector has been running at Fermilab since 2020, collecting neutrino interactions from the BNB and NuMI beams. In late 2025, ICARUS reached five years of continuous data taking, demonstrating the maturity of large-scale LAr-TPC technology and its relevance for future experiments such as DUNE. This contribution presents the first ICARUS search for muon-neutrino disappearance in the BNB. Charged-current 1$\mu$Np events selected from 2022–2023 data are compared to simulations and interpreted, for the first time, within a two-neutrino approximation of the 3+1 sterile-neutrino model, including systematic uncertainties from flux, interaction, and detector effects. Although currently limited by systematic uncertainties, this first oscillation analysis probes the parameter space suggested by existing $\nu_\mu$ disappearance results and lays the groundwork for future SBN combined analyses with SBND, which will significantly improve sensitivity to sterile-neutrino scenarios.

Steklain, Andre [Parana Tech. Fed. U., Toledo] (OR↗
NASA NTRS1995

Excitable dynamics in high-Lewis number premixed gas combustion at normal and microgravity

Freely-propagating, premixed gas flames in high-Lewis (Le) number, quiescent mixtures are studied experimentally in tubes of various diameter at normal (lg) and microgravity (mu g). A premixture of lean butane and oxygen diluted with helium, argon, neon, nitrogen or a mixture of multiple diluents is examined such that the thermal diffusivity of the mixture (and to a lesser extent, the mass diffusivity of the rate-limiting component) is systematically varied. In effect, different diluents allow variation of the Le without changing the chemistry. The flames are recorded with high speed cinematography and their stability is visually assessed. Different modes of propagation were observed depending on the diameter of the tubes (different conductive heat loss), the composition of the mixture and the g-level. At 1g, four modes of propagation were observed in small and intermediate diameter tubes (large conductive heat loss): (1) steadily propagating flames, (2) radial and longitudinal pulsating flames, (3) 'wavering' flames, and (4) rotating spiral flames. As the diameter of the tube increases, the radial modes become more pronounced while the longitudinal modes systematically disappear. Also, multiple, simultaneous, spatially-separated 'pacemaker' sites are observed in intermediate and large diameter tubes. Each site starts as a small region of high luminosity and develops into a flamelet which assumes the form of one of the fore mentioned modes. These flamelets eventually interact, annihilate each other in their regions of intersection and merge at their newly created free-ends. For very large tubes, radially-propagating wave-trains (believed to be 'trigger waves') are observed. These are analogous to the radial pulsations observed in the smaller diameter tubes. At mu g, three modes of propagation have been observed: (1) steadily propagating flames, (2) radial and longitudinal pulsating flames, and (3) multi-armed, rotating flames. Since the pulsating mode exists at mu g and 1g, buoyant flicker is not the mechanism which drives the pulsations. Moreover, all of the instabilities at 1g and mu g have characteristic frequencies on the O(100Hz). This value is lower than the fundamental, longitudinal acoustic frequencies of the tubes which suggests that the instabilities are not acoustically driven. The patterns formed by this reaction bear remarkable similarities with the patterns formed in most excitable media when the behavior of the system is driven by couplings between chemical reaction and diffusion (e.g., Belousov-Zhabotinsky reaction, Patterns in slime molds, spiral waves in the retina of a bird's eye). While it is recognized that the chemical mechanism associated with this premixed gas reaction is exponentially sensitive to temperature and undoubtedly different from those which govern previously observed excitable media (most are isothermal, or weakly exothermic, liquid phase reactions), similar spatial and temporal patterns should not come as a complete surprise considering heat and mass diffusion are self similar. It is concluded that this premixed gas system is a definitive example of a diffusive-thermal, gas-phase oscillator based on these experimental results and their favorable comparison with theory.

Pearlman, Howard↗
DOE OSTI2024

Effects of catholyte aging on high-nickel NMC cathodes in sulfide all-solid-state batteries

Sulfide solid-state electrolytes (SSEs) in all-solid-state batteries (SSBs) are recognized for their high ionic conductivity and inherent safety. The LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode offers a high thermodynamic potential of approximately 3.8 V vs. Li/Li + and a theoretical specific capacity of 200 mA h g −1 . However, the practical utilization of NMC811 in sulfide SSBs faces significant interfacial challenges. The oxidation instability of sulfide solid electrolytes against NMC811 and the formation of the cathode electrolyte interphase (CEI) during cycling lead to degradation and reduced cell performance. Volumetric changes in NMC during lithiation and de-lithiation can also cause detachment from sulfide electrolytes or internal particle cracking. Despite extensive galvanostatic cycling studies to address the issues, the calendar life of sulfide SSBs remains poorly understood. Here, we systematically studied the effects of four different catholytes on the calendar aging of LiNbO 3 (LNO)-coated NMC811, including Li 6 PS 5 Cl (LPSCl), Li 3 InCl 6 –Li 6 PS 5 Cl (LIC–LPSCl), Li 3 YCl 6 –Li 6 PS 5 Cl (LYC–LPSCl), and Li 10 GeP 2 S 12 (LGPS). Our results indicate that LPSCl provides optimal capacity retention when stored at high state-of-charge (SOC) at room temperature, but the LIC–LPSCl cathode shows significant capacity degradation and chemical incompatibility. We also established an effective electrochemical calendar aging testing protocol to simulate daily usage, enabling quick inference of the calendar life of SSBs. In conclusion, this new testing approach accelerates materials selection strategies for high-nickel NMC composite cathodes in sulfide SSBs.

25 ENERGY STORAGE↗
DOE OSTI2024

The Effective Fragment Molecular Orbital Method: Achieving High Scalability and Accuracy for Large Systems

The effective fragment molecular orbital (EFMO) method has been developed to predict the total energy of a very large molecular system accurately (with respect to the underlying quantum mechanical method) and efficiently by taking advantage of the locality of strong chemical interactions and employing a two-level hierarchical parallelism. The accuracy of the EFMO method is partly attributed to the accurate and robust intermolecular interaction prediction between distant fragments, in particular, the many-body polarization and dispersion effects, which require the generation of static and dynamic polarizability tensors by solving the coupled perturbed Hartree–Fock (CPHF) and time-dependent HF (TDHF) equations, respectively. Solving the CPHF and TDHF equations is the main EFMO computational bottleneck due to the inefficient (serial) and I/O-intensive implementation of the CPHF and TDHF solvers. In this work, the efficiency and scalability of the EFMO method are significantly improved with a new CPU memory-based implementation for solving the CPHF and TDHF equations that are parallelized by either message passing interface (MPI) or hybrid MPI/OpenMP. Here, the accuracy of the EFMO method is demonstrated for both covalently bonded systems and noncovalently bound molecular clusters by systematically examining the effects of basis sets and a key distance-related cutoff parameter, R cut . R cut determines whether a fragment pair (dimer) is treated by the chosen ab initio method or calculated using the effective fragment potential (EFP) method (separated dimers). Decreasing the value of Rcut increases the number of separated (EFP) dimers, thereby decreasing the computational effort. It is demonstrated that excellent accuracy (<1 kcal/mol error per fragment) can be achieved when using a sufficiently large basis set with diffuse functions coupled with a small R cut value. With the new parallel implementation, the total EFMO wall time is substantially reduced, especially with a high number of MPI ranks. Given a sufficient workload, nearly ideal strong scaling is achieved for the CPHF and TDHF parts of the calculation. For the first time, EFMO calculations with the inclusion of long-range polarization and dispersion interactions on a hydrated mesoporous silica nanoparticle with explicit water solvent molecules (more than 15k atoms) are achieved on a massively parallel supercomputer using nearly 1000 physical nodes. In addition, EFMO calculations on the carbinolamine formation step of an amine-catalyzed aldol reaction at the nanoscale with explicit solvent effects are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Systematic planning of moving target defence for maximising detection effectiveness against false data injection attacks in smart grid

Abstract Moving target defence (MTD) has been gaining traction to thwart false data injection attacks against state estimation (SE) in the power grid. MTD actively perturbs the reactance of transmission lines equipped with distributed flexible AC transmission system (D‐FACTS) devices to falsify the attacker's knowledge about the system configuration. However, the existing literature has not systematically studied what influences the detection effectiveness of MTD and how it can be improved based on the topology analysis. These problems are tackled here from the perspective of an MTD plan in which the D‐FACTS placement is determined. We first exploit the relation between the rank of the composite matrix and the detecting effectiveness. Then, we rigorously derive upper and lower bounds on the attack detecting probability of MTDs with a given rank of the composite matrix. Furthermore, we analyse existing planning methods and highlight the importance of bus coverage by D‐FACTS devices. To improve the detection effectiveness, we propose a novel graph theory–based planning algorithm to retain the maximum rank of the composite matrix while covering all necessary buses. Comparative results on multiple systems show the high detecting effectiveness of the proposed algorithm in both DC‐ and AC‐SE.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2022

Impact of ferromagnetic electrode length and thickness on Magnetic Tunnel Junction-Based Molecular Spintronic Devices (MTJMSD)

A knowledge gap exists about the impact of variation in length and thickness of ferromagnetic(FM) electrodes on molecular spintronics devices’ ability to manifest molecular coupling impact. Magnetic Tunnel Junction-Based Molecular Spintronic Devices (MTJMSDs) are potential candidates for inventing highly correlated materials and devices and investigating the fundamental science of organic spintronics. This paper reports our experi- mental observations providing the dramatic impact of variation in ferromagnetic electrode length and thickness on paramagnetic molecule-based MTJMSD. Room temperature transport studies were performed to investigate the effect of FM electrode thickness. On the other hand, magnetic force microscopy measurements were con- ducted to understand the effect of FM electrode length extending beyond the molecular junction area, i.e., the site where paramagnetic molecules bridged between two FM. In the strong molecular coupling regime, transport study suggested thickness variation caused ~1000 to million-fold differences in junction conductivity. MFM study revealed near-zero magnetic contrast for pillar-shaped MTJMSD without any extended FM electrode. However, MFM images showed a multitude of microscopic magnetic phases on cross junction shaped MTJMSD where FM electrodes extended beyond the junction area. To understand the intriguing experimental results, we conducted an in-depth theoretical study using Monte Carlo Simulation (MCS) approach. MCS study utilized a Heisenberg atomic model of cross junction shaped MTJMSD to gain insights about room temperature transport and MFM experimental observations of microscopic MTJMSD. To make this study applicable for a wide variety of MTJMSDs, we systematically studied the effect of variation in molecular coupling strength between magnetic molecules and ferromagnetic (FM) electrodes of various dimensions. Here, our theoretical results suggest 25 atoms thick FM electrode show very weak molecular coupling impact and of the same order of experimentally studied FM electrode dimensions showing weak effect. Also, MCS results agree with experimentally observed multiple magnetic phases on lengthy FM electrodes of an MTJMSD.

42 ENGINEERING↗
DOE OSTI2026

Adsorption, charge transfer and a coverage-driven transition of alkali metals on rutile TiO 2 (110)

The interaction of alkali metals with metal oxide surfaces is central to tuning surface reactivity in heterogeneous catalysis and photocatalysis. Here we present a comprehensive DFT+U study of the adsorption of alkali metals (Li, Na, K, Rb, Cs) on the (110) surface of rutile TiO 2 . At low coverage (θ = 1/8), all alkali metals bind preferentially to bridging oxygen sites with adsorption energies in the range −4.06 to −3.33 eV, transferring nearly one full electron (0.92–0.99 |e|) to the substrate and inducing Ti 4+ → Ti 3+ reduction. The excess charge localizes preferentially at subsurface Ti sites in the form of small polarons. Diffusion barriers indicate facile motion along bridging-oxygen rows, whereas inter-row hopping is strongly hindered. Coverage effects were examined systematically for potassium: adsorption energy and charge transfer per K atom decrease monotonically with increasing θ. Strikingly, a sharp energy discontinuity occurs between θ = 4/8 and θ = 5/8 (ΔE ≈ 1 eV per atom), which we identify as a coverage-driven structural transition arising from steric packing constraints and enhanced K–K electrostatic repulsion once every (1×1) surface cell is occupied. This structural transition perfectly correlates with a dramatic drop in the work function down to an ultra-low minimum of 0.84 eV at θ=5/8, followed by a metallization- driven recovery at higher coverages. Ab initio molecular dynamics simulations confirm zigzag K arrangements at moderate coverage (θ = 1/3), while at high coverage (θ = 2/3) short-range K–K correlations emerge without long-range order. These results provide atomistic insight into the structure–activity relationships underlying alkali promotion effects on oxide-supported catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1982

Effects of the mode of storage on the capacity fading of the sintered nickel electrodes

A systematic investigation of the effect of temperature and two conditions of storage, shortened and open circuit, on the capacity fading of sintered nickel electrodes in NiCd batteries was conducted. All testing was done on sintered electrodes in flooded cells. Cycling tests to measure the capacity were performed at room temperature. The capacity out to one volt, a capacity useful for satellite applications. Test results indicated that: the shortened electrode showed a higher rate of loss than the open circuit electrodes; there was an increase in both modes with an increase in temperature; there was a loss of capacity with time of storage; a general degradation was observed as a function of time; shortened electrodes showed a higher end of charge than the open circuit ones; and at room temperature there was a lower loss in the open circuit electrode than in the shortened one.

Vyes, B.↗
NASA NTRS1994

Is there a role for a test controller in the development of new ATC equipment?

Earl Wiener points out that human factors problems fixed during the R & D stage are paid for once. When they are not fixed during R & D, they are then paid for every day. How users are involved in the R & D process to assist in developing equipment is a critical issue. Effective involvement can produce real improvements. Ineffective involvement can produce inefficient kludges or systems that are actually dangerous. The underlying problem is the management of information and ideas. To develop a really generative system a great deal would have to change in the way that the FAA innovates. Use of test controllers would solve only some of the problems. For instance, we have cockpit resource management now for pilots; we may have it soon for controllers. But the management of ideas in the innovation process also needs intellectual resource management. Simply involving users is not enough. Brought in at the wrong point in the development process, users can block or compromise innovation. User involvement must be carefully considered. A test controller may be one solution to this problem. It might be necessary to have several kinds of test controllers (en route versus TRACON, for instance). No doubt further problems would surface in getting test controllers into operation. I would recommend that the FAA engage in a series of case studies of controller involvement in the innovation process. A systematic comparison of effective and ineffective cases would do much to clarify what we ought to do in the future. Unfortunately, I have been unable to find any cases where test controllers have been used. Perhaps we need to create some, to see how they work.

Westrum, Ron↗
NASA NTRS1993

Convergence acceleration of implicit schemes in the presence of high aspect ratio grid cells

The performance of Navier-Stokes codes are influenced by several phenomena. For example, the robustness of the code may be compromised by the lack of grid resolution, by a need for more precise initial conditions or because all or part of the flowfield lies outside the flow regime in which the algorithm converges efficiently. A primary example of the latter effect is the presence of extended low Mach number and/or low Reynolds number regions which cause convergence deterioration of time marching algorithms. Recent research into this problem by several workers including the present authors has largely negated this difficulty through the introduction of time-derivative preconditioning. In the present paper, we employ the preconditioned algorithm to address convergence difficulties arising from sensitivity to grid stretching and high aspect ratio grid cells. Strong grid stretching is particularly characteristic of turbulent flow calculations where the grid must be refined very tightly in the dimension normal to the wall, without a similar refinement in the tangential direction. High aspect ratio grid cells also arise in problems that involve high aspect ratio domains such as combustor coolant channels. In both situations, the high aspect ratio cells can lead to extreme deterioration in convergence. It is the purpose of the present paper to address the reasons for this adverse response to grid stretching and to suggest methods for enhancing convergence under such circumstances. Numerical algorithms typically possess a maximum allowable or optimum value for the time step size, expressed in non-dimensional terms as a CFL number or vonNeumann number (VNN). In the presence of high aspect ratio cells, the smallest dimension of the grid cell controls the time step size causing it to be extremely small, which in turn results in the deterioration of convergence behavior. For explicit schemes, this time step limitation cannot be exceeded without violating stability restrictions of the scheme. On the other hand, for implicit schemes, which are typically unconditionally stable, there appears to be room for improvement through careful tailoring of the time step definition based on results of linear stability analyses. In the present paper, we focus on the central-differenced alternating direction implicit (ADI) scheme. The understanding garnered from this analyses can then be applied to other implicit schemes. In order to systematically study the effects of aspect ratio and the methods of mitigating the associated problems, we use a two pronged approach. We use stability analyses as a tool for predicting numerical convergence behavior and numerical experiments on simple model problems to verify predicted trends. Based on these analyses, we determine that efficient convergence may be obtained at all aspect ratios by getting a combination of things right. Primary among these are the proper definition of the time step size, proper selection of viscous preconditioner and the precise treatment of boundary conditions. These algorithmic improvements are then applied to a variety of test cases to demonstrate uniform convergence at all aspect ratios.

Buelow, B. E. O.↗
DOE OSTI2022

Tuning the Mechanical and Electric Properties of Conjugated Polymer Semiconductors: Side–Chain Design Based on Asymmetric Benzodithiophene Building Blocks

Understanding molecular design rules for stretchable polymer semiconductors is important for enabling next generation stretchable electronic circuits. To simultaneously improve both electrical properties and mechanical stretchability, a design strategy is reported in introducing conjugated rigid fused-rings with bulky side groups in semiconducting polymers. In this work, the understanding of this design concept is improved by systematically investigating the effect of different types of bulky side groups asymmetrically substituted on conjugated polymer semiconductor backbones. Specifically, four types of side groups are investigated, including naphthalene (NaPh), biphenyl (PhPh), thienylphenyl (ThPh), and alkylphenyl (C4Ph), asymmetrically substituted on benzodithiophene units, namely asy-BDT. With the four types of side groups installed on BDT-containing conjugated polymers in an asymmetrical fashion, it is observed that they reduced the polymer chain aggregation and film crystallinity, hence improving the film stretchability. Furthermore, the fully conjugated polymer back-bone allows maintenance of good charge carrier mobilities. Specifically, polymer PDPP-C4Ph (with C4Ph side groups) shows the highest mobility in the fully stretchable transistor and maintained its mobility even after being subjected to hundreds of stretching-releasing cycles at 25% strain. Altogether, the results provide anunderstanding of the use of asymmetrically substituted fused-ring conjugated polymer structures to tune mechanical and charge transport properties.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Irreparable Interphase Chemistry Degradation Induced by Temperature Pulse in Lithium‐Ion Batteries

Abstract While it is widely recognized that the operating temperature significantly affects the energy density and cycle life of lithium‐ion batteries, the consequence of electrode‐electrolyte interphase chemistry to sudden environmental temperature changes remains inadequately understood. Here, we systematically investigate the effects of a temperature pulse (T pulse) on the electrochemical performance of LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) pouch full cells. By utilizing advanced characterization tools, such as time‐of‐flight secondary‐ion mass spectrometry, we reveal that the T pulse can lead to an irreversible degradation of cathode‐electrolyte interphase chemistry and architecture. Despite negligible immediate impacts on the solid‐electrolyte interphase (SEI) on graphite anode, aggregated cathode‐to‐anode chemical crossover gradually degrades the SEI by catalyzing electrolyte reduction decomposition and inducing metallic dead Li formation because of insufficient cathode passivation after the T pulse. Consequently, pouch cells subjected to the T pulse show an inferior cycle stability to those free of the T pulse. This work unveils the effects of sudden temperature changes on the interphase chemistry and cell performance, emphasizing the importance of a proper temperature management in assessing performance.

Cui, Zehao↗