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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 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Bio‐Inspired Cascade Photocatalysis on Fe Single‐Atom Carbon Nitride Upcycles Plastic Wastes for Effective Acetic Acid Production

Plastic imposes a critical threat to the environment, ecosystems, and human health because of the low utilization efficiency of plastics. Here, we demonstrate a sustainable, highly efficient cascade photocatalysis for upcycle plastics to value-added acetic acid using Fe single-atom catalysts (Fe@C 3 N 4 SAC) at ambient conditions. Inspired by Phanerochaete chrysosporium microbial, the defective Fe@C 3 N 4 SAC acts as a bifunctional cascade photocatalyst for both Fenton-like and CO 2 reduction reactions. During the reaction, hydroxyl radicals (*OH) form and subsequently oxidize plastics into CO 2 intermediates. These CO 2 intermediates are then photo-reduced to CH 3 COOH on the same catalyst via cascade photocatalysis. The mechanism is confirmed by in situ multimodal microscopy and spectroscopies, with density functional theory calculations. A state-of-art CH 3 COOH yield of 63.8 mg h −1 gcat −1 from PVC, 12.7 mg h −1 gcat −1 from PE, 5.4 mg h −1 gcat −1 from PET, and 5.3 mg h −1 gcat −1 from PP are directly obtained under AM1.5G solar irradiation and further validated under real sunlight (≈0.6 sun), achieving 5.6 mg h −1 gcat −1 from PET, using low-cost Fe@C 3 N 4 SAC in a sealed reactor by enhancing the photon transport and utilization efficiency. The techno-economic analysis shows it is promising to practically mitigate plastic based on broader social welfare assessments.

cascade photocatalysis↗
DOE OSTI2022

Catalyst and reactor design considerations for selective production of acids by oxidative cleavage of alkenes and unsaturated fatty acids with H 2 O 2

Oxidative cleavage of alkenes and unsaturated fatty acids with hydrogen peroxide gives an efficient and sustainable process to obtain mono- and di-acids for polymers and lubricants with fewer safety risks and less environmental impact than processes that utilize ozone or other inorganic oxidizers (e.g., permanganate, dichromate, etc.). Guided by insight into the mechanisms for competing reaction pathways (i.e., epoxidation of alkene on W–(η 2 -O 2 ) complexes vs. H 2 O 2 decomposition) and the apparent kinetics derived from kinetic experiments, here, we postulate that W-based heterogeneous catalysts can provide high performance and stable operations at low H 2 O 2 concentrations. Semi-batch reactors with continuous introduction of H 2 O 2 solutions offer the means to maintain low H 2 O 2 concentrations while providing sufficient quantities of H 2 O 2 to satisfy the reaction stoichiometry. We derived simple kinetic model equations for the epoxidation, ring-opening, oxidative cleavage, and oxidation steps and fit theses equations to batch experimental data to obtain kinetic parameters. Furthermore, this kinetic model describes the concentration profiles of reactant, oxidant, and products well as shown by agreement with experimental data. Further predictions of the optimal H 2 O 2 feed rate for semi-batch operation utilized by the proposed rate expressions and the reactor design equations suggest that low H 2 O 2 feed rate increases selectivity towards oxidative cleavage products and selective use of H 2 O 2 for oxidative cleavage pathway. Comparisons of oxidative cleavage of 4-octene in batch and semi-batch reactors show that semibatch reactors with optimized molar feed rates of H 2 O 2 increased oxidative cleavage product selectivities (76% to 99%; with an increase in butyric acid selectivity from 1% to 55%) and H 2 O 2 selectivity (3% to 30%). In addition, semibatch reaction conditions used avoid H 2 O 2 -mediated dissolution of W-atoms from the catalyst. Analysis of these findings suggest that solid oxide catalysts will be effective for continuous oxidative cleavage reactions if deployed within fixed-bed reactors that allow for distributed introduction of reactants and therefore low in situ concentrations of H 2 O 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2007

Catalytic Ignition and Upstream Reaction Propagation in a Platinum Tube

A challenge for catalytic combustion in monolithic reactors at elevated temperatures is the start-up or "light-off" from a cold initial condition. In this work, we demonstrate a concept called "back-end catalytic ignition that potentially can be utilized in the light-off of catalytic monoliths. An external downstream flame or Joule heating raises the temperature of a small portion of the catalyst near the outlet initiating a localized catalytic reaction that propagates upstream heating the entire channel. This work uses a transient numerical model to demonstrate "back-end" ignition within a single channel which can characterize the overall performance of a monolith. The paper presents comparisons to an experiment using a single non-adiabatic channel but the concept can be extended to the adiabatic monolith case. In the model, the time scales associated with solid heat-up are typically several orders of magnitude larger than the gas-phase and chemical kinetic time-scales. Therefore, the model assumes a quasi-steady gas-phase with respect to a transient solid. The gas phase is one-dimensional. Appropriate correlations, however, account for heat and mass transfer in a direction perpendicular to the flow. The thermally-thin solid includes axial conduction. The gas phase, however, does not include axial conduction due to the high Peclet number flows. The model includes both detailed gas-phase and catalytic surface reactions. The experiment utilizes a pure platinum circular channel oriented horizontally though which a CO/O2 mixture (equivalence ratios ranging from 0.6 to 0.9) flows at 2 m/s.

Struk, P. M.↗
DOE OSTI2021

Introducing a novel technique for measuring hydrogen crossover in membrane-based electrochemical cells

Hydrogen crossover that is the unwanted hydrogen permeation across the membrane driven by the difference of gas concentrations causes a critical concern of safety and efficiency for electrochemical cells, such as fuel cells and electrolyzer cells. Although the hydrogen crossover measurement in fuel cells that employ platinum based catalysts is simple and widely used in laboratory settings, it is questionable to apply existing limiting current method to water electrolyzer cells and alkaline exchange membrane (AEM) systems, which is due to the typical catalyst materials used and membrane properties, respectively. In this work, we demonstrate the operation of a compact and low-cost method of measuring hydrogen crossover that works for both AEM and proton exchange membrane (PEM) systems. The method entails a tandem configuration that utilizes an upstream crossover cell with a downstream cell in hydrogen pump configuration to measure the crossover in the cell of interest. We have successfully measured the hydrogen crossover with different membranes at various differential pressures. The developed method can be applied to catalyst-free membranes (both PEM and AEM) as well as PGM free catalyst containing cells. It will be a promising technique for measuring hydrogen crossover in-situ for a real operating membraned-based electrochemical cell or stack.

08 HYDROGEN↗
DOE OSTI2020

Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization

This study presented an approach to overcome diffusion limitation and imbalance between Brønsted and Lewis acidities that affect conversion and aromatic yield in alkane nonoxidative dehydroaromatization (DHA) conversion. Three different Ga-promoted ZSM-5 catalysts were synthesized for the ethane DHA reaction. The hierarchical galloaluminosilicate Meso-GaZSM-5 was prepared by the solid-state crystallization technique wherein Ga was introduced through the in situ synthesis process. The microporous galloaluminosilicate Micro-GaZSM-5 was synthesized by the hydrothermal technique wherein Ga was introduced in situ during zeolite formation. The hierarchically structured Ga-Meso-ZSM-5 was synthesized by the solid-state crystallization method, but the Ga was introduced by the incipient wetness method. Additional Pt was incorporated by the incipient wetness technique for all three catalysts to enhance the DHA activity. The solid-state crystallization technique created the hierarchical structure without using a template. With the in situ technique, Ga species replaced the Al framework, reducing the strong Brønsted acidity. Meanwhile, they created the extraframework GaO + , introducing the strong Lewis acid sites into catalysts. Due to better synergistic interaction between the oxidation state of metals, acidic properties, and catalyst porosity, Pt-Meso-GaZSM-5 showed higher C 2 H 6 conversion and aromatic selectivity. The improvement on diffusivity not only reduces the effect of channel blockage but also improves the utilization of active sites. As a result, this work sheds light on the direct, nonoxidative conversion of shale gas without going through the syngas route.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Enabling Multireference Calculations on Multimetallic Systems with Graphic Processing Units

Modeling multimetallic systems efficiently enables faster prediction of desirable chemical properties and the design of new materials. This work describes an initial implementation for performing multireference wave function method localized active-space self-consistent field (LASSCF) calculations through the use of multiple graphics processing units (GPUs) to accelerate time-to-solution. Density fitting is leveraged to reduce memory requirements, and we demonstrate the ability to fully utilize multi-GPU compute nodes. Performance improvements of 5–10x in total application runtime were observed in LASSCF calculations for multimetallic catalyst systems up to 1200 AOs and an active space of (22e,40o) using up to four NVIDIA A100 GPUs. Furthermore, written with performance portability in mind, a comparable performance is also observed in early runs on the Aurora exascale system using Intel Max Series GPUs.

Algorithms↗
DOE OSTI2022

Copper(ii)-photocatalyzed decarboxylative oxygenation of carboxylic acids

Showcasing the concept of light-induced homolysis for the generation of radicals, the Cu II -photocatalyzed decarboxylative oxygenation of carboxylic acids with molecular oxygen as the terminal oxidant is described. Here, two Cu II -carboxylate complexes with different coordination geometries were synthesized and characterized by X-ray analysis, correlating their structure with their ability to initiate light-induced decarboxylations.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
NASA NTRS1997

A Chemical Approach to Carbon Dioxide Utilization on Mars

We describe several novel proposals for CO2 reduction through chemical, photochemical, and photoelectrochemical means. The approach involves coupled catalytic cycles to simultaneously produce oxygen and carbon monoxide. Efficient metal catalysts and photocatalysts are to be used for both halfreactions: (1) the reduction of CO2 to CO; and (2) the evolution of O2. Photolytic reduction of CO2 to CO and oxygen can occur under mild conditions using a series of recently synthesized trinuclear nickel catalysts. Nickel cluster catalysts hold great promise because of the proven ability of nickel cluster materials to catalyze the reduction of CO2 to CO.

Hepp, Aloysius F.↗
DOE OSTI2024

Cooperative Effects Drive Water Oxidation Catalysis in Cobalt Electrocatalysts through the Destabilization of Intermediates

A barrier to understanding the factors driving catalysis in the oxygen evolution reaction (OER) is understanding multiple over- lapping redox transitions in the OER catalysts. The complexity of these transitions obscure the relationship between the coverage of adsorbates and OER kinetics, leading to an experimental challenge in measuring activity descriptors, such as binding energies, as well as adsorbate interactions, which may destabilize intermediates and modulate their binding energies. Herein, we utilize a newly designed optical spectroelectrochemistry system to measure these phenomena in order to contrast the behavior of two electrocatalysts, cobalt oxyhydroxide (CoOOH) and cobalt-iron hexacyanoferrate (cobalt-iron Prussian blue, CoFe-PB). Three distinct optical spectra are observed in each catalyst, corresponding to three separate redox transitions, the last of which we show to be active for the OER using time-resolved spectroscopy and electrochemical mass spectroscopy. By combining predictions from density functional theory with parameters obtained from electroadsorption isotherms, we demonstrate that a destabilization of catalytic intermediates occurs with increasing coverage. In CoOOH, a strong (~0.34 eV/ monolayer) destabilization of a strongly bound catalytic intermediate is observed, leading to a potential offset between the accumulation of the intermediate and measurable O 2 evolution. We contrast these data to CoFe-PB, where catalytic intermediate generation and O 2 evolution onset coincide due to weaker binding and destabilization (~0.19 eV/monolayer). By considering a correlation between activation energy and binding strength, we suggest that such adsorbate driven destabilization may account for a significant fraction of the observed OER catalytic activity in both materials. Finally, we disentangle the effects of adsorbate interactions on state coverages and kinetics to show how adsorbate interactions determine the observed Tafel slopes. Crucially, the case of CoFe-PB shows that, even where interactions are weaker, adsorption remains non-Nernstian, which strongly influences the observed Tafel slope.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Iridium-Doped Nanosized Zn–Al Layered Double Hydroxides as Efficient Water Oxidation Catalysts

Layered double hydroxides (LDHs) are an ideal platform to host catalytic metal centers for water oxidation (WO) owing to the high accessibility of water to the interlayer region, which makes all centers potentially reachable and activated. In this paper, we report the syntheses of three iridium-doped zinc–aluminum LDHs (Ir-LDHs) nanomaterials (1–3, with about 80 nm of planar size and a thickness of 8 nm as derived by field emission scanning electron microscopy and powder X-ray diffraction studies, respectively), carried out in the confined aqueous environment of reverse micelles, through a very simple and versatile procedure. These materials exhibit excellent catalytic performances in WO driven by NaIO 4 at neutral pH and 25 °C, with an iridium content as low as 0.5 mol % (~0.8 wt %), leading to quantitative oxygen yields (based on utilized NaIO 4 , turnover number up to ~10,000). Nanomaterials 1–3 display the highest ever reported turnover frequency values (up to 402 min –1 ) for any heterogeneous and heterogenized catalyst, comparable only to those of the most efficient molecular iridium catalysts, tested under similar reaction conditions. The boost in activity can be traced to the increased surface area and pore volume (>5 times and 1 order of magnitude, respectively, higher than those of micrometric materials of size 0.3–1 μm) estimated for the nanosized particles, which guarantee higher noble metal accessibility. X-ray absorption spectroscopy (XAS) studies suggest that 1–3 nanomaterials, as-prepared and after catalysis, contain a mixture of isolated, single octahedral Ir(III) sites, with no evidence of Ir–Ir scattering from second-nearest neighbors, excluding the presence of IrO 2 nanoparticles. The combination of the results obtained from XAS, elemental analysis, and ionic chromatography strongly suggests that iridium is embedded in the brucite-like structure of LDHs, having four hydroxyls and two chlorides as first neighbors. These results demonstrate that nanometric LDHs can be successfully exploited to engineer efficient WOCs, minimizing the amount of iridium used, consistent with the principle of the noble-metal atom economy.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Engineering the electronic and strained interface for high activity of PdM core @Pt monolayer electrocatalysts for oxygen reduction reaction

Alloyed nanoparticles with core-shell structures provide a favorable model to modulate interfacial interaction and surface structures at the atomic level, which is important for designing electrocatalysts with high activity and durability. Herein, core-shell structured Pd 3 M@Pt/C nanoparticles with binary PdM alloy cores (M = Fe, Ni, and Co) and a monolayer Pt shell were successfully synthesized with diverse interfaces. Among these, Pd 3 Fe@Pt/C exhibited the best oxygen reduction reaction catalytic performance, roughly 5.4 times more than that of the commercial Pt/C catalyst used as reference. The significantly enhanced activity is attributed to the combined effects of strain engineering, interfacial electron transfer, and improved Pt utilization. Density functional theory simulations and extended X-ray absorption fine structure analysis revealed that engineering the alloy core with moderate lattice mismatch and alloy composition (Pd 3 Fe) optimizes the surface oxygen adsorption energy, thereby rendering excellent electrocatalytic activity. Finally, future researches may use this study as a guide on the construction of highly effective core-shell electrocatalysts for various energy conversions and other applications.

25 ENERGY STORAGE↗
DOE OSTI2024

First-Principles Insights into the Thermodynamics of Variable-Temperature Ammonia Synthesis on Transition-Metal-Doped Cu (100) and (111)

Ammonia (NH 3 ) is one of the most produced chemicals worldwide. NH 3 synthesis predominantly utilizes the Haber–Bosch (HB) process, requiring high temperatures and pressures. Despite significant process advances, ample opportunity remains for improving the rate, selectivity, catalyst stability, and energy efficiency. Inspired by a recently developed programmable heating and quenching (PHQ) technique, we present in this paper a first-principles screening of candidate single-atom alloy catalysts generated from doping (111) and (100) surfaces of copper (Cu), an ineffective HB catalyst in its pure form. We predict the thermodynamics of two rate-limiting reactions, N 2 dissociative adsorption and the final hydrogenation step leading up to NH 3 release, at 400 and 900 K. Thermodynamically, the former reaction is favored at low temperatures, while the latter is favored at high temperatures. Vanadium-, chromium-, and molybdenum-doped Cu surfaces, due to intermediate M–N covalent bonding character, emerge as appealing candidate catalysts for PHQ NH 3 synthesis, as they balance the thermodynamics of the above-mentioned reaction steps at their respective optimal temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

The Radical Atom: Mechanosynthetic 3D Printing of an Atomically Precise SPM Tip

This research effort sought to overcome current limitations in scanning probe-based atomic manipulation to enable atomically precise manufacturing (APM). Previous theoretical and experimental works on atom by atom and molecule by molecule fabrication of precise structures are limited to essentially to two-dimensions. APM will enable a paradigm shift in 21st century manufacturing practices in which every single atom in a electronic chip, device or machine can be placed in an exact and predefined position in three-dimensions. By providing a general method for generating reproducible SPM tip structure, this project will drive forward the entire field of atomically precise scanning probe microscopy, opening the door to positional control of nearly arbitrary covalent chemistry. Such control could, for example, be used in applications such as novel 2.5 or 3D microchip fabrication. The creation of a unique manufacturing method through APM has the potential to impact technologies at the theoretical limits of performance, weight, and utility including: solid-state quantum and spintronic computing systems, high efficiency optical antenna, solar power systems, defect engineered materials and extremely efficient catalysts. Although this experiment focused on pick-and-place non-scalable APM, the better understanding of the chemistry is crucial to the eventual goal of scalable APM. To place individual atoms into a specified location is a seminal aspiration of researchers and engineers in the many fields and may have early premium applications in medical devices and microelectronics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Au/Pt Bimetallic Nanowires with Stepped Pt Sites for Enhanced C–C Cleavage in C2+ Alcohol Electro-oxidation Reactions

Efficient C–C bond cleavage and oxidation of alcohols to CO 2 is the key to developing highly efficient alcohol fuel cells for renewable energy applications. In this work, we report the synthesis of core/shell Au/Pt nanowires (NWs) with stepped Pt clusters deposited along the ultrathin (2.3 nm) stepped Au NWs as an active catalyst to effectively oxidize alcohols to CO 2 . The catalytic oxidation reaction is dependent on the Au/Pt ratios, and the Au 1.0 /Pt 0.2 NWs have the largest percentage (~75%) of stepped Au/Pt sites and show the highest activity for ethanol electro-oxidation, reaching an unprecedented 196.9 A/mg Pt (32.5 A/mg Pt+Au ). This NW catalyst is also active in catalyzing the oxidation of other primary alcohols, such as methanol, n-propanol, and ethylene glycol. In situ X-ray absorption spectroscopy and infrared spectroscopy are used to characterize the catalyst structure and to identify key reaction intermediates, providing concrete evidence that the synergy between the low-coordinated Pt sites and the stepped Au NWs is essential to catalyze the alcohol oxidation reaction, which is further supported by DFT calculations that the C–C bond cleavage is indeed enhanced on the undercoordinated Pt–Au surface. Here, our study provides important evidence that a core/shell structure with stepped core/shell sites is essential to enhance electrochemical oxidation of alcohols and will also be central to understanding electro-oxidation reactions and to the future development of highly efficient direct alcohol fuel cells for renewable energy applications.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2021

A Nanocrystal Catalyst Incorporating a Surface Bound Transition Metal to Induce Photocatalytic Sequential Electron Transfer Events

Heterogeneous photocatalysis is less common but can provide unique avenues for inducing novel chemical transformations and can also be utilized for energy transductions, i.e., the energy in the photons can be captured in chemical bonds. Here, we developed a novel heterogeneous photocatalytic system that employs a lead-halide perovskite nanocrystal (NC) to capture photons and direct photogenerated holes to a surface bound transition metal Cu-site, resulting in a N–N heterocyclization reaction. The reaction starts from surface coordinated diamine substrates and requires two subsequent photo-oxidation events per reaction cycle. We establish a photocatalytic pathway that incorporates sequential inner sphere electron transfer events, photons absorbed by the NC generate holes that are sequentially funneled to the Cu-surface site to perform the reaction. The photocatalyst is readily prepared via a controlled cation-exchange reaction and provides new opportunities in photodriven heterogeneous catalysis.

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

The Reactivity and Structural Dynamics of Supported Metal Nanoclusters Using Electron Microscopy, in-situ X-Ray Spectroscopy, Electronic Structure Theories, and Molecular Dynamics Simulations

This research will provide new methods to determine the structures and compositions of heterogeneous catalysts as they exist in reaction conditions. The new tools will make it possible to understand how extremely small material structures—ones in a size range spanning from single atoms to larger polyatomic clusters—make it possible to carry out highly selective chemical transformations required to synthesize useful materials as well as for efficient energy production and utilization. The tools will make it possible to see how the atomic structures of catalytic materials evolve over time under the conditions of their use, and in this way provide understandings to guide the design of new energy-efficient catalysts. The work will make it possible to answer long standing questions that include the following. How does catalyst structure help guide molecules along specific reaction pathways? What are the important intermediates involved in these transformations? How do the structures and reactivity of catalytic materials, as well as the chemistry of their interfaces, vary with reaction conditions? Is it possible to develop new catalytic materials using new knowledge of the active structures and reaction mechanisms? The work will provide heretofore unavailable experimental tools that can be applied in advanced programs of research addressing such questions.

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

Design of a bifunctional TEMPO-tertiary amine mesoporous silica catalyst for the three-step cascade synthesis of a chromene derivative

A key challenge is design of materials and processes whereby competing reagents or conditions do not harm the multi-step sequence, thus allowing for more efficient chemical synthesis with elimination of work-up and separation steps. In this work, a three-step reaction cascade is performed using a porous bifunctional dimethylpropylamine-TEMPO-MCM41 catalyst, converting the commodity chemicals benzyl alcohol, sodium hypochlorite, and malononitrile to a biologically active anti-cancer, and anti-malarial 2-amino-chromene derivative. The cascade first utilizes a TEMPO-catalyzed oxidation of benzyl alcohol to benzaldehyde with NaOCl as the terminal oxidant. This is followed by a two-step, dual base catalyzed Knoevenagel condensation with malononitrile followed by a Michael addition with lawsone. Optimal conditions converting benzyl alcohol to 2-amino-5,10-dioxo-4-phenyl-5,10-dihydro-4H-benzo[g]chromene-3-carbonitrile include the delayed addition of malononitrile and lawsone during the three-step reaction sequence, which results in a 2-amino-chromene yield of over 80%. The importance of stepwise reagent addition is rationalized due to the unfavorable adsorption of acidic lawsone on the surface-grafted base catalyst. Tertiary Brønsted base sites of dimethylpropylamine outperform the more Lewis basic primary propylamine functionalized catalyst. This work outlines a simple and effective method for generating mesoporous materials with two types of active sites via co-condensation and thiol-ene coupling procedures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Scalable Metal Phosphides as a Dual-Function Catalyst and Lithium–Metal Stabilizer for Lithium–Sulfur Batteries

Although lithium-sulfur batteries are a promising approach for achieving high energy density, their commercial viability is limited by poor sulfur redox kinetics, polysulfide shuttling, and lithium metal instability. To resolve these issues concurrently, we utilize titanium phosphides (TiP x ) as dual-function materials to catalyze the sulfur redox kinetics at the cathode and stabilize the lithium metal at the anode. Importantly, these phosphides are synthesized via a facile, highly scalable one-step mechanochemical ball-milling process that does not generate toxic phosphine gas as a byproduct, making it more viable compared to traditional synthesis routes. At the cathode, we find that higher phosphorus contents in the phosphide as in TiP 2 leads to superior redox kinetics and reduced polysulfide shuttling due to improved polysulfide adsorption ability. Meanwhile, at the anode, TiP 2 acts as a lithiophilic seed in a 3-dimensional carbonaceous host that can be lithiated to form a Li-TiP 2 /C composite. This composite alleviates the volume changes of lithium metal while utilizing TiP 2 to form a more favorable solid-electrolyte interface (SEI). Full coin cells employing TiP 2 in the cathode and anode were assembled with a sulfur loading of 4 mg cm -2 and a negative to positive capacity (N/P) ratio of 6. After 50 cycles, the TiP 2 full cells retain a higher capacity of 643 mA h g -1 compared to 422 mA h g -1 for the conventional cell, despite the higher N/P ratio of 12 for the conventional cell. Altogether, we showcase the viability of employing metal phosphides as catalysts in practical lithium-sulfur batteries.

25 ENERGY STORAGE↗