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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 811 records · Page 45
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Hydrophobic Metal–Organic Frameworks Enable Superior High-Pressure Ammonia Storage through Geometric Design

Hydrophobic metal–organic frameworks (MOFs) are typically overlooked for ammonia storage due to weak host–guest interactions. Here, we demonstrate that four structurally analogous aluminum-based MOFs exhibit a counterintuitive behavior whereby framework geometry, rather than ligand hydrophilicity, determines high-pressure NH 3 adsorption performance. The hydrophobic CAU-23 achieved an exceptional capacity matching hydrophilic analogs despite its poor low-pressure uptake. This pressure-dependent enhancement stems from the unique 4-cis-4-trans geometry of CAU-23 compared to the purely cis arrangement of MIL-160 and KMF-1 and the alternating cis-trans configuration of MOF-303. Critically, CAU-23 retained 95% capacity over three high-pressure cycles, whereas hydrophilic MOFs suffered 39–46% irreversible losses due to strong NH 3 -framework interactions that compromise structural integrity. Grand canonical Monte Carlo simulations reveal that high pressure enables NH 3 clustering through intermolecular hydrogen bonding, bypassing the need for strong host–guest interactions. High-pressure powder X-ray diffraction measurements confirm the exceptional mechanical resilience of CAU-23, showing complete structural recovery upon decompression despite exhibiting the highest pressure sensitivity among the studied MOFs. An extended analog, HE-CAU-23, validates this design principle with further enhanced capacity. Furthermore, these findings reveal a paradigm shift toward hydrophobic MOFs with optimized geometry for high-performance and regenerable gas storage applications.

MOFs↗
DOE OSTI2026

Photocatalytic Ammonia Synthesis using Fe-Based MOFs: The Role of Ligand Functionalization

Photocatalytic ammonia (NH 3 ) synthesis offers a carbon-neutral alternative to the Haber−Bosch process, which generates 42 million metric tons of CO 2 equivalent emissions annually. However, solar-to-ammonia conversion with contemporary photocatalysts remains far from practical requirements, and understanding the limiting factors in systems with well-defined active sites is crucial. Here, we show how the μ 3 -oxo-centered trinuclear Fe cluster in MIL-101(Fe) functions as the catalytic motif for N 2 -to-NH 3 conversion through combined experimental and computational investigations. Comparative studies with a molecular analogue demonstrate that the cluster is stabilized within the MOF framework, sustaining redox cycling and maintaining high catalytic activity. We systematically functionalized the dicarboxylate ligands of MIL-101(Fe) with −NH 2 , −Br, −NO 2 , −F, and −CF 3 to probe how ligand chemistry modulates Fe electron density, N 2 adsorption capacity, and proton availability, correlating these properties with catalytic performance using spectroscopic and surface characterization techniques alongside timeresolved infrared to assess excited-state lifetimes. F-functionalization optimally balances N 2 activation, proton availability at Fe active sites, and excited-state lifetimes, boosting NH 3 production by ∼ 60% relative to unmodified MIL-101(Fe). This study of ligandfunctionalized MIL-101(Fe) MOFs uncovers the underlying structure-activity relationships and advances design principles for solardriven NH 3 synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Engineering Structural Transitions in a Multilevel Molecular Switch via Intermolecular Coupling

Controlling molecular conformations with atomic precision is essential for advancing molecular functional electronics, as well as our understanding of molecular dynamics. While switching between bistable molecular conformers is common in nature, creating systems with multiple, addressable states remains synthetically challenging. Here, we demonstrate a bottom-up strategy in which intermolecular interactions give rise to multilevel functionality within a simple two-molecule assembly. Using low-temperature scanning tunneling microscopy, we show that a pyrrolidine dimer on Cu(100) exhibits six distinct adsorption conformations, exceeding the four expected from two independent bistable units. This unusual complexity arises from the interplay between intermolecular van der Waals attraction and steric repulsion, which reshapes the potential energy landscape and changes a single high-energy transition into a sequential two-step pathway. Each step is driven by low-energy inelastic electron excitations, achieving a switching efficiency an order of magnitude higher than that of the monomer. Here, by tuning the bias voltage and tip–molecule distance, we achieve deterministic control over multiple stable states, establishing a general design principle for on-demand engineering of collective molecular behavior and energy-efficient multilevel molecular devices.

Molecular interactions↗
DOE OSTI2026

Low-Temperature Non-Oxidative Coupling of Methane on Atomically Dispersed Titanium–Aluminum–Boron Nanopowder

Nonoxidative coupling of methane represents a long-standing challenge in heterogeneous catalysis, as it requires activation of the carbon–hydrogen (C–H) bond, controlled carbon–carbon (C–C) bond formation, and effective hydrogen management without relying on oxidants. Here, we report a low-temperature C–H activation and nonoxidative C–C coupling of methane over atomically dispersed titanium–aluminum–boron nanopowder (Ti–Al–B NP) utilizing a catalytic microreactor coupled to synchrotron single-photon photoionization reflectron time-of-flight mass spectrometry. The soft-ionization, in situ probing method detects the nascent reaction products and radical intermediates under operando conditions, including methyl radical, C2 hydrocarbons, and molecular hydrogen. Methane activation is initiated at 800 K, approximately 700 K below the gas-phase decomposition threshold, leading predominantly to ethylene formation with selectivity reaching up to 78% among the C–C coupled products. Electronic structure calculations on model Ti–Al–B clusters elucidate a cooperative catalytic mechanism in which titanium enables methane adsorption and C–H activation, boron acts as a reversible hydrogen reservoir, and aluminum stabilizes methylene intermediates, thereby facilitating selective C–C coupling and dehydrogenation. These findings establish a distinct catalyst architecture for nonoxidative methane coupling based on earth abundant elements alternative to expensive platinum and other noble metal-containing conventional catalysts and provide molecular-level design principles for controlling dehydrogenation and subsequent C–C bond formation in challenging light alkane conversions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Selective Bidentate Coordination Reconstructs Residual PbI 2 to Homogenize Interfacial Energetics in Perovskite Solar Cells

Spatially heterogeneous interfacial energetics, often originating from residual lead iodide (PbI 2 ), represent a fundamental bottleneck to both the efficiency and operational stability of perovskite photovoltaics. Conventional PbI 2 passivation strategies based on monodentate ligands or highly polar solvents either interact weakly with PbI 2 or undesirably perturb the underlying three-dimensional perovskite lattice. Here, we report a diammonium bidentate strategy that selectively reconstructs residual PbI 2 into corner-sharing PbI 6 octahedra while preserving the bulk perovskite. Enabled by dual-site coordination, a newly designed thiophene-based bidentate ligand (MeXT) stabilizes PbI 6 units during passivation and establishes spatially homogeneous interfacial energetics. Perovskite solar cells incorporating MeXT achieve 26.19% power conversion efficiency and retain over 80% of their initial efficiency after 1000 h of continuous 1-sun illumination at 75 °C. This dual-anchor coordination passivation strategy establishes a general design principle for selectively treating residual PbI 2 and creating electronically coherent and operationally stable interfaces in perovskite photovoltaics.

ligands↗
DOE OSTI2026

Interfacial Charge Transfer Pathways in Photoelectrochemical H 2 Evolution by a Single-Component Molecular Catalyst on a Conductive Metal Oxide

Dye-sensitized photoelectrosynthesis cells traditionally combine a photosensitizing dye to harvest light and a catalyst to generate chemical fuels on a semiconductor. Here, in this work, a photoactive catalyst capable of both light absorption and fuel formation, [Cp*Ir(4,4′-Y 2 -bpy)Cl][Cl] (Cp* = pentamethylcyclopentadienyl, bpy = 2,2′-bipyridine, Y = CH 2 PO 3 H 2 ), is anchored to a mesoporous tin-doped indium oxide (ITO) electrode and facilitates photoelectrochemical H 2 evolution in water without the need for additional photosensitizers or sacrificial reductants. Spectroelectrochemistry indicates a single-site H 2 evolution mechanism involving charge injection to ITO, in contrast to the bimetallic mechanism observed in solution. Cyclic voltammetry and variable-potential chronoamperometry under illumination probe competing pathways via interfacial electron transfer between the Ir hydride excited state and the conductive ITO electrode. A Marcus theory framework provides reorganization energies for competing interfacial electron transfer pathways from potential-dependent quantum yield measurements. The light-driven H 2 evolution catalysis on conducting oxide proceeds with high Faradaic efficiency and current densities comparable to photoelectrodes utilizing p-type semiconductors. By uncovering the principal electron transfer pathways that govern photocatalytic efficiency, this study establishes design principles for hybrid molecular photoelectrocatalysts.

catalysts↗
DOE OSTI2026

High-Voltage Sodium–Metal Batteries with Asymmetric Fluoroalkoxylated Organoborate Anion Chemistry

The high reactivity of sodium (Na) metal restricts its compatibility to ether-based electrolytes, while the poor oxidative stability of ethers precludes their coupling to high-voltage cathodes, fundamentally limiting the operating voltage and energy density of sodium–metal batteries (SMBs). We present here a coordination-asymmetry strategy to reconcile this thermodynamic mismatch by generating in situ an asymmetric fluoroalkoxylated organoborate anion, [FB(OCH(CF 3 ) 2 ) 3 ] − (BOF – ), via a Lewis acid–base adduct reaction in ether electrolyte. The asymmetric ligand architecture differentiates oxidative and fluorination pathways: oxidizable B–O moieties mediate controlled interfacial reconstruction, whereas the terminal B–F units supply fluorine for chemical passivation. This self-adaptive chemistry yields nanoscale, conformal, compositionally graded interphases: a boron-oxide/boron-oxycarbide-rich cathode-electrolyte interphase (CEI) that mitigates ether oxidation and a bilayered inorganic–organic solid–electrolyte interphase (SEI) that regulates Na deposition. The nanostructured interphases enable highly reversible Na plating/stripping with an average Coulombic efficiency (CE) of 99.98% and sustain stable 4.3 V operation of anode-free SMBs in oxidation-prone ether electrolytes. Furthermore, this work establishes asymmetric boron coordination as a molecular-level design principle for creating chemically adaptive interphases that overcome the redox asymmetry in energy-dense electrochemical systems.

Anions↗
DOE OSTI2026

Enhanced Catalytic Dechlorination of Polyvinyl Chloride (PVC) and H2 Production Enabled by Synergistic Gaδ+/Ga0 Active Sites in Liquid Metal Particles

Polyvinyl chloride (PVC) is ubiquitous yet challenging to recycle due to its tendency to thermally decompose above 250 °C, releasing toxic, corrosive chlorinated compounds, and its inability to melt. Here, we report a catalytic strategy for PVC upcycling at 160 °C using gallium liquid metal particles (Ga-LMP) featuring a dynamic Ga-GaOOH core–shell architecture. These catalysts enable concurrent dechlorination and hydrogen evolution, yielding up to 7% H2 (based on initial hydrogen atoms in PVC) along with a highly dechlorinated (>95%) carbonaceous solid and aqueous HCl. Mechanistic investigations combining X-ray photoelectron spectroscopy, infrared spectroscopy, solid-state NMR, inelastic neutron scattering, and ab initio molecular dynamics reveal a synergistic interplay between Gaδ+ sites in the GaOOH shell and metallic Ga0 in the core. Cationic Ga initiates C–Cl bond activation and HCl formation, while progressive reduction of the shell exposes Ga0 sites that promote C–H activation and H2 evolution. Control experiments with a Ga salt and bulk Ga liquid metal confirmed that neither oxidation state alone can achieve both transformations efficiently. This work establishes a dynamic dual-site paradigm for liquid metal catalysis, in which the in situ evolution and coexistence of oxidized and metallic species enable sequential and cooperative bond activation pathways. These findings provide a general design principle for novel liquid metal catalysts that target challenging polymer transformations under mild conditions.

Zingg, Benjamin [ORNL] (ORCID:0009000914530153)↗
DOE OSTI2026

Gold Quantum Rods: Modulation of Singlet and Triplet Exciton Populations by the Rod Length

Abstract Gold quantum rods (QRs) of Au60, Au78, Au96, and Au114 (protected by thiolate ligands) exhibit exclusive fluorescence, which is different from the shorter Au42 QR with dual emission (fluorescence + phosphorescence). Herein, we report the excitation wavelength-dependent near-infrared-II photoluminescence (PL) and exciton dynamics of this series of QRs. Interestingly, the fluorescence quantum yield (QY) of the QRs is much higher (2–10×) when the lowest singlet excited state (S1) is excited compared to the excitation of high-lying states (Sn). A metastable intermediate singlet state (denoted S′) is identified by transient absorption spectroscopy when Sn is excited, and this S′ state leads to fast “skybridge” intersystem crossing (ISC), which contributes primarily (>60%) to the total triplet population. With increasing aspect ratio (AR) of QRs (from 6.3 to 18.7), nonradiative processes accelerate, leading to fast decay of the S1 state (hence, less QY) and of the T1 state (barely phosphorescent). A detailed energy flow mechanism is determined for the QRs after photoexcitation, which offers a design principle for manipulation of exciton dynamics toward potential utilization of higher excited states in applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

A Multifunctional Cosolvent Pair Reveals Molecular Principles of Biomass Deconstruction

The complex structure of plant cell walls resists chemical or biological degradation, challenging the breakdown of lignocellulosic biomass into renewable chemical precursors that could form the basis of future production of green chemicals and transportation fuels. In this report, experimental and computational results reveal that the effect of the tetrahydrofuran (THF)–water cosolvents on the structure of lignin and on its interactions with cellulose in the cell wall drives multiple synergistic mechanisms leading to the efficient breakdown and fractionation of biomass into valuable chemical precursors. Molecular simulations reflect that THF–water is an excellent “theta” solvent, such that lignin dissociates from itself and from cellulose and expands to form a random coil. The expansion of the lignin molecules exposes interunit linkages, rendering them more susceptible to depolymerization by acid-catalyzed cleavage of aryl-ether bonds. Nanoscale infrared sensors confirm cosolvent-mediated molecular rearrangement of lignin in the cell wall of micrometer-thick hardwood slices and track the disappearance of lignin. At bulk scale, adding dilute acid to the cosolvent mixture liberates the majority of the hemicellulose and lignin from biomass, allowing unfettered access of cellulolytic enzymes to the remaining cellulose-rich material, allowing them to sustain high rates of hydrolysis to glucose without enzyme deactivation. Through this multiscale analysis, synergistic mechanisms for biomass deconstruction are confirmed, portending a paradigm shift toward first-principles design and evaluation of other cosolvent methods to realize low cost fuels and bioproducts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Understanding and Design of Bidirectional and Reversible Catalysts of Multielectron, Multistep Reactions

The catalytic properties of the enzymes that transform H2 set very high standards for chemists who aim at designing synthetic electrocatalysts of H2 oxidation and production. Of particular relevance is the observation that some hydrogenases wired to electrodes function in either direction of the reaction depending on the driving force that is applied, and at a significant rate as a result of even a very small deviation from equilibrium. We call the former property "bidirectionality", and the latter "reversibility". Bidirectional and reversible catalysts of H2 oxidation and production have only recently been synthesized. Here we introduce the kinetic modelling of bidirectional two-electron redox reactions in the case of molecular catalysts and enzymes that are either attached to an electrode or diffusing in solution in the vicinity of an electrode. Our theoretical findings are illustrated by previous results obtained with hydrogenases and Nickel diphosphine molecular catalysts. We emphasize that trying to discuss bidirectionality and reversibility in relation to a single redox potential leads to an impasse: the catalyst undergoes two redox transitions, and two catalytic potentials must be defined, which may depart from the two potentials measured in the absence of catalysis. The difference between the two catalytic potentials defines the reversibility; the difference between their average value and the open circuit potential defines the directionality. We aim at giving rules that help discriminate between distinct mechanisms ("ECEC", "EECC" etc.) based on the voltammetric responses, and we discuss the design principles of bidirectionality and reversibility in terms of kinetics. In particular we conclude that neither bidirectionality nor reversibility requires that the catalytic energy landscape be flat. However, sinks and high energy intermediates may negatively impact the catalytic rates. The "efficiency" of a bidirectional catalyst appears to be defined by various figures of merit (rates, directionality, reversibility) that need to be recognized before they can be optimized simultaneously. E.S.W. was supported by the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy (USDOE), Office of Science, Office of Basic Energy Sciences (BES). The work discussed here was originally supported for WJS by the Office of Science Early Career Research Program through the USDOE, with current funding from the USDOE, BES, Chemical Sciences, Geosciences, and Biosciences program.

Fourmond, Vincent↗
DOE OSTI2024

Chemical Upcycling of Polyolefin Plastics Using Structurally Well-defined Catalysts

Single-use polyolefins are widely used in our daily life and industrial production due to their light weight, low cost, superior stability, and durability. However, the rapid accumulation of plastic waste and low-profit recycling methods resulted in a global plastic crisis. Catalytic hydrogenolysis is regarded as a promising technique, which can effectively and selectively convert polyolefin plastic waste to value-added products. In this perspective, we focus on the design and synthesis of structurally well-defined hydrogenolysis catalysts across mesoscopic, nanoscopic, and atomic scales, accompanied by our insights into future directions in catalyst design for further enhancing catalytic performance. These design principles can also be applied to the depolymerization of other polymers and ultimately realize the chemical upcycling of waste plastics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Reacting CO 2 with Light Alkanes to Value-Added Products

Catalytic conversion of anthropogenic carbon dioxide (CO 2 ) into value-added products is a promising strategy to mitigate global carbon emissions. Concurrently, the shale gas revolution has provided an abundant supply of light alkanes (methane, ethane, propane, and butane), presenting a unique opportunity to employ these underutilized hydrocarbons as an effective, low-cost hydrogen source for CO 2 reduction. In this Perspective, we summarize past efforts, current state, and future opportunities for reacting CO 2 with light alkanes to generate a diverse range of value-added products. Compared with direct alkane conversion, the introduction of CO 2 fundamentally alters reaction thermodynamics and kinetics, enabling selective C–H and C–C bond activation while suppressing catalyst deactivation from coke formation. Building on decades of research in dry reforming and CO 2 -assisted dehydrogenation, recent advances in catalyst design have enabled CO 2 -assisted dehydrogenation processes that approach chemical equilibrium for the selective production of olefins and syngas. Importantly, advances in catalyst design and reactor engineering have further expanded the product scope beyond gas-phase (syngas and olefins) to include liquid-phase (oxygenates and aromatics), and solid-phase products (carbon nanomaterials). We highlight key catalyst design principles for controlling reaction pathways and discuss major challenges and opportunities in developing selective and versatile platforms for the simultaneous upgrading of CO 2 and light alkanes.

CO2↗
DOE OSTI2015

Size and Temperature Dependence of Electron Transfer between CdSe Quantum Dots and a TiO 2 Nanobelt

Understanding charge transfer reactions between quantum dots (QD) and metal oxides is fundamental for improving photocatalytic, photovoltaic and electronic devices. The complexity of these processes makes it difficult to find an optimum QD size with rapid charge injection and low recombination. We combine time-domain density functional theory with nonadiabatic molecular dynamics to investigate the size and temperature dependence of the experimentally studied electron transfer and charge recombination at CdSe QD-TiO 2 nanobelt (NB) interfaces. The electron injection rate shows strong dependence on the QD size, increasing for small QDs. The rate exhibits Arrhenius temperature dependence, with the activation energy of the order of millielectronvolts. The charge recombination process occurs due to coupling of the electronic subsystem to vibrational modes of the TiO 2 NB. Inelastic electron-phonon scattering happens on a picosecond time scale, with strong dependence on the QD size. Our simulations demonstrate that the electron-hole recombination rate decreases significantly as the QD size increases, in excellent agreement with experiments. The temperature dependence of the charge recombination rates can be successfully modeled within the framework of the Marcus theory through optimization of the electronic coupling and the reorganization energy. Our simulations indicate that by varying the QD size, one can modulate the photoinduced charge separation and charge recombination, fundamental aspects of the design principles for high efficiency devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Optimization of Structural Flood Mitigation Strategies

The dynamics of flooding are primarily influenced by the shape, height, and roughness (friction) of the underlying topography. For this reason, mechanisms to mitigate floods frequently employ structural measures that either modify topographic elevation, for example, through the placement of levees and sandbags, or increase roughness, for example, through revegetation projects. However, the configuration of these measures is typically decided in an ad hoc manner, limiting their overall effectiveness. The advent of high–performance surface–water modeling software and improvements in black–box optimization suggest that a more principled design methodology may be possible. This paper proposes a new computational approach to the problem of designing structural mitigation strategies under physical and budgetary constraints. It presents the development of a problem discretization amenable to simulation–based, derivative–free optimization. However, meta–heuristics alone are found to be insufficient for obtaining quality solutions in a reasonable amount of time. As a result, this paper proposes novel numerical and physics–based procedures to improve convergence to a high–quality mitigation. Furthermore the efficiency of the approach is demonstrated on hypothetical dam break scenarios of varying complexity under various mitigation budget constraints. In particular, experimental results show that, on average, the final proposed algorithm results in a 65% improvement in solution quality compared to a direct implementation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

Metabolic and thermal stimuli control K 2P 2.1 (TREK-1) through modular sensory and gating domains

K 2P 2.1 (TREK-1) is a polymodal two-pore domain leak potassium channel that responds to external pH, GPCRmediated phosphorylation signals, and temperature through the action of distinct sensors within the channel. How the various intracellular and extracellular sensory elements control channel function remains unresolved. Here, we show that the K 2P 2.1 (TREK-1) intracellular C-terminal tail (Ct), a major sensory element of the channel, perceives metabolic and thermal commands and relays them to the extracellular C-type gate through transmembrane helix M4 and pore helix 1. By decoupling Ct from the pore-forming core, we further demonstrate that Ct is the primary heat-sensing element of the channel, whereas, in contrast, the pore domain lacks robust temperature sensitivity. Together, our findings outline a mechanism for signal transduction within K 2P 2.1 (TREK-1) in which there is a clear crosstalk between the C-type gate and intracellular Ct domain. In addition, our findings support the general notion of the existence of modular temperature-sensing domains in temperature-sensitive ion channels. This marked distinction between gating and sensory elements suggests a general design principle that may underlie the function of a variety of temperature-sensitive channels.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2016

Polar Metals by Geometric Design

Gauss's law dictates that the net electric field inside a conductor in electrostatic equilibrium is zero by effective charge screening; free carriers within a metal eliminate internal dipoles that may arise owing to asymmetric charge distributions(1). Quantum physics supports this view(2), demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals(3)-it is exceedingly unusual to find a polar metal that exhibits long-range ordered dipoles owing to cooperative atomic displacements aligned from dipolar interactions as in insulating phases(4). Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-film ANiO(3) perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements(5). We predict with ab initio calculations that cooperative polar A cation displacements are geometrically stabilized with a non-equilibrium amplitude and tilt pattern of the corner-connected NiO6 octahedra-the structural signatures of perovskites-owing to geometric constraints imposed by the underlying substrate. Heteroepitaxial thin-films grown on LaAlO3 (111) substrates fulfil the design principles. We achieve both a conducting polar monoclinic oxide that is inaccessible in compositionally identical films grown on (001) substrates, and observe a hidden, previously unreported(6-10), non-equilibrium structure in thin-film geometries. We expect that the geometric stabilization approach will provide novel avenues for realizing new multifunctional materials with unusual coexisting properties.

Kim, T. H.↗
DOE OSTI2016

Lithium-coated polymeric matrix as a minimum volume-change and dendrite-free lithium metal anode

Lithium metal is the ideal anode for the next generation of high-energy-density batteries. Nevertheless, dendrite growth, side reactions and infinite relative volume change have prevented it from practical applications. Here, we demonstrate a promising metallic lithium anode design by infusing molten lithium into a polymeric matrix. The electrospun polyimide employed is stable against highly reactive molten lithium and, via a conformal layer of zinc oxide coating to render the surface lithiophilic, molten lithium can be drawn into the matrix, affording a nano-porous lithium electrode. Importantly, the polymeric backbone enables uniform lithium stripping/plating, which successfully confines lithium within the matrix, realizing minimum volume change and effective dendrite suppression. The porous electrode reduces the effective current density; thus, flat voltage profiles and stable cycling of more than 100 cycles is achieved even at a high current density of 5 mA cm -2 in both carbonate and ether electrolyte. Furthermore, the advantages of the porous, polymeric matrix provide important insights into the design principles of lithium metal anodes.

36 MATERIALS SCIENCE↗