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DOE OSTI2022

High Throughput Data-Driven Design of Laser-Crystallized 2D MoS 2 Chemical Sensors: A Demonstration for NO 2 Detection

High throughput characterization and processing techniques are becoming increasingly necessary to navigate multivariable, data-driven design challenges for sensors and electronic devices. For two-dimensional materials, device performance is highly dependent upon a vast array of material properties including the number of layers, lattice strain, carrier concentration, defect density, and grain structure. In this work, laser crystallization was used to locally pattern and transform hundreds of regions of amorphous MoS 2 thin films into 2D 2H-MoS 2 . Here a high throughput Raman spectroscopy approach was subsequently used to assess the process-dependent structural and compositional variations for each illuminated region, yielding over 6000 distinct nonresonant, resonant, and polarized Raman spectra. The rapid generation of a comprehensive library of structural and compositional data elucidated important trends between structure–property processing relationships involving laser-crystallized MoS 2 , including the relationships between grain size, grain orientation, and intrinsic strain. Moreover, extensive analysis of structure/property relationships allowed for intelligent design and evaluation of major contributions to device performance in MoS 2 chemical sensors. In particular, it is found that NO 2 sensor performance is strongly dependent on the orientation of the MoS 2 grains relative to the crystal plane.

36 MATERIALS SCIENCE↗

DOE OSTI2022

3D Bragg Coherent Diffraction Imaging of Extended Nanowires: Defect Formation in Highly Strained InGaAs Quantum Wells

InGaAs quantum wells embedded in GaAs nanowires can serve as compact near-infrared emitters for direct integration onto Si complementary metal oxide semiconductor technology. While the core–shell geometry in principle allows for a greater tuning of composition and emission, especially farther into the infrared, the practical limits of elastic strain accommodation in quantum wells on multifaceted nanowires have not been established. One barrier to progress is the difficulty of directly comparing the emission characteristics and the precise microstructure of a single nanowire. Here, in this study, we report an approach to correlating quantum well morphology, strain, defects, and emission to understand the limits of elastic strain accommodation in nanowire quantum wells specific to their geometry. We realize full 3D Bragg coherent diffraction imaging (BCDI) of intact quantum wells on vertically oriented epitaxial nanowires, which enables direct correlation with single-nanowire photoluminescence. By growing In 0.2 Ga 0.8 As quantum wells of distinct thicknesses on different facets of the same nanowire, we identified the critical thickness at which defects are nucleated. A correlation with a traditional transmission electron microscopy analysis confirms that BCDI can image the extended structure of defects. Finite element simulations of electron and hole states explain the emission characteristics arising from strained and partially relaxed regions. This approach, imaging the 3D strain and microstructure of intact nanowire core–shell structures with application-relevant dimensions, can aid the development of predictive models that enable the design of new compact infrared emitters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Metabolic Differentiation of Co-occurring Accumulibacter Clades Revealed through Genome-Resolved Metatranscriptomics

Natural microbial communities consist of closely related taxa that may exhibit phenotypic differences and inhabit distinct niches. However, connecting genetic diversity to ecological properties remains a challenge in microbial ecology due to the lack of pure cultures across the microbial tree of life. “Candidatus Accumulibacter phosphatis” (Accumulibacter) is a polyphosphate-accumulating organism that contributes to the enhanced biological phosphorus removal (EBPR) biotechnological process for removing excess phosphorus from wastewater and preventing eutrophication from downstream receiving waters. Distinct Accumulibacter clades often coexist in full-scale wastewater treatment plants and laboratory-scale enrichment bioreactors and have been hypothesized to inhabit distinct ecological niches. However, since individual strains of the Accumulibacter lineage have not been isolated in pure culture to date, these predictions have been made solely on genome-based comparisons and enrichments with varying strain compositions. Here, we used genome-resolved metagenomics and metatranscriptomics to explore the activity of coexisting Accumulibacter strains in an engineered bioreactor environment. We obtained four high-quality genomes of Accumulibacter strains that were present in the bioreactor ecosystem, one of which is a completely contiguous draft genome scaffolded with long Nanopore reads. We identified core and accessory genes to investigate how gene expression patterns differed among the dominating strains. Using this approach, we were able to identify putative pathways and functions that may confer distinct functions to Accumulibacter strains and provide key functional insights into this biotechnologically significant microbial lineage.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Sound velocities of iron-nickel (Fe90Ni10) alloy up to 8 GPa and 773 K: The effect of nickel on the elastic properties of bcc-iron at high P-T

Sound velocities of iron and iron-based alloys at high pressure and high temperature are crucial for understanding the composition and structure of Earth’s and other telluric planetary cores. In this study, we performed ultrasonic interferometric measurements of both compressional (ν P ) and shear (ν S ) velocities on a polycrystalline body-centered-cubic (bcc)-Fe 90 Ni 10 up to 8 GPa and 773 K. The elastic moduli and their pressure and temperature derivatives are derived from least-square fits to third-order finite strain equations, yielding K S0 = 154.2(8) GPa, G 0 = 73.2(2) GPa, K' S0 = 4.6(2), G' 0 = 1.5(1), ∂K S /∂T = –0.028(1) GPa/K, and ∂G/∂T = –0.023(1) GPa/K. Furthermore, a comparison with literature data on bcc-Fe suggests that nickel not only decreases both P and S wave velocities but also weakens the temperature effects on the elastic moduli of Fe-Ni alloys.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Understanding Formation of Irradiation-Induced Defects through 4D-STEM, Electron Tomography, and WBDF-STEM

A major challenge in advancing nuclear materials for next-generation fission and proposed fusion reactors is to comprehensively understand the formation of irradiation-induced defects. Here it is essential to correlate the evolution of irradiation-induced defects and the degradation of mechanical properties, as they collectively dictate the material's lifespan and ensure nuclear safety. Scanning transmission electron microscopy (STEM) based techniques have emerged as indispensable tools for irradiation-induced defect characterization, offering high spatial resolution imaging and chemical analysis, such as electron energy loss spectroscopy (EELS) and energy dispersive X-ray spectroscopy (EDXS). These techniques have been effectively used to obtain an atomic-scale view of the defect structure. Recent advances in electron microscopy, particularly in 4D-STEM, offer detailed insight into microstructural evolution by capturing full 2D diffraction patterns at every pixel position. Using high-speed direct electron detectors, this technology generates a four-dimensional dataset, overcoming the limitations of traditional STEM imaging.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Rate-dependent strength and deformation heterogeneity of B4C-reinforced Al composite: Time-resolved imaging with synchrotron X-rays

Dynamic (up to 5500 s -1 ) and quasi-static compression tests are conducted on a 15 wt% B4C particle-reinforced Al (B 4 C/Al) composite. In situ, high-speed synchrotron X-ray phase contrast imaging and digital image correlation are employed to map mesoscale deformation fields at μm and μs scales. The bulk stress–strain curves show significant strain and strain-rate hardening under dynamic compression. The strain-rate sensitivity exponent is an order of magnitude higher at high strain rates (> 10 3 s -1 ) than that at low strain rates (< 10 -2 s -1 ). Strain field mapping demonstrates distinct compressive strain localizations for both quasi-static and dynamic loading. Nevertheless, compressive strain localizations appear denser in spacing under dynamic loading, owing to spontaneous dislocation nucleation in both weak and strong zones. This results in a higher density of geometrically necessary dislocations, which contributes to the higher strain and strain-rate hardening of B 4 C/Al under dynamic loading. Additionally, the ratio of the maximum local strain to the bulk average is 1.5, and the local strain-rate enhancement cannot explain the increased rate sensitivity of B 4 C/Al under dynamic loading. Therefore, the rate-dependent deformation heterogeneity dominates the strain-rate hardening of B 4 C/Al. Postmortem analyses help correlate deformation features to particle- and grain-scale microstructures, yielding consistent results with mesoscale strain fields.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Expanding the composition of polyhydroxyalkanoates produced by an industrial host: CRADA 505 [Abstract only]

The Agile BioFoundry (ABF) is a multi-national lab consortium funded by the Department of Energy’s Bioenergy Technologies Office that has developed a biofoundry that enables the rapid deployment of bioproducts into the market. Working with two ABF laboratory members (National Renewable Energy Laboratory (NREL) and Pacific Northwest National Laboratory (PNNL), Danimer will develop bacterial strains to produce PHAs with different compositions aimed at expanding Danimer’s product offerings. This project will enable the ABF to contribute to the development of a high-profile, commercial product that falls squarely in the DOE mission space and has strong potential to have meaningful benefit both to the US economy and the environment.

09 BIOMASS FUELS↗

DOE OSTI2026

Suppressing Phase Segregation and Improving Stability in Mixed-Halide Perovskites through Spinel Oxide-Directed Epitaxy

Mixed-cation mixed-halide perovskite compositions are essential for achieving the required bandgaps for high-efficiency multijunction photovoltaics, yet their stability remains limited by interfacial defects, phase segregation, and degradation. Here, we introduce spinel oxides as a new family of lattice-matched substrates that enable crystalline, phase-pure, compositionally-uniform, bromide-rich perovskite film growth. The effect of spinel oxides is two-fold: reducing defects at the bottom interface by templating film growth and inducing beneficial compressive strain through mismatch-dependent substrate-perovskite lattice coupling. Spinel oxide substrates facilitate growth of highly crystalline films and eliminate detrimental secondary phases across thicknesses. Using grazing incidence X-ray diffraction, X-ray fluorescence, cathodoluminescence–scanning electron microscopy, cryogenic photoluminescence, and density functional theory, we reveal that Mg-halide bonds at the bottom interface induce lattice mismatch-dependent compressive strain that suppresses halide segregation and further reduces defect formation. In addition, films grown on spinel oxides maintain over 87% of the perovskite phase after 12 h under 100% relative humidity, as monitored by in situ grazing incidence wide-angle X-ray scattering (GIWAXS), compared to less than 70% for control samples. This work extends lattice matching from vapor-deposited epitaxial semiconductors to solution-processed halide perovskites to establish a broadly applicable strategy for defect suppression, phase homogenization, and long-term stability. Based on the fundamental science explored here, we set the stage for the development of lattice-matched spinel oxide charge transport layers to be integrated into perovskite solar cells and other optoelectronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Doping- and Strain-Dependent Electrolyte-Gate-Induced Perovskite to Brownmillerite Transformation in Epitaxial La 1– x Sr x CoO 3–δ Films

Much recent attention has focused on the voltage-driven reversible topotactic transformation between the ferromagnetic metallic perovskite (P) SrCoO 3-δ and oxygen-vacancy-ordered antiferromagnetic insulating brownmillerite (BM) SrCoO 2.5 . This is emerging as a paradigmatic example of the power of electrochemical gating (using, e.g., ionic liquids/gels), the wide modulation of electronic, magnetic, and optical properties generating clear application potential. SrCoO 3 films are challenging with respect to stability, however, and there has been little exploration of alternate compositions. Here, we present the first study of ion-gel-gating-induced P. BM transformations across almost the entire La 1-x SrxCoO 3 phase diagram (0 ≤ x ≤ 0.70), under both tensile and compressive epitaxial strain. Electronic transport, magnetometry, and operando synchrotron X-ray diffraction establish that voltage-induced P → BM transformations are possible at essentially all x, including x ≤ 0.50, where both P and BM phases are highly stable. Under small compressive strain, the transformation threshold voltage decreases from approximately +2.7 V at x = 0 to negligible at x = 0.70. Both larger compressive strain and tensile strain induce further threshold voltage lowering, particularly at low x. The P → BM threshold voltage is thus tunable, via both composition and strain. At x = 0.50, voltage-controlled ferromagnetism, transport, and optical transmittance are then demonstrated, achieving Curie temperature and resistivity modulations of similar to 220 K and at least 5 orders of magnitude, respectively, and enabling estimation of the voltage-dependent Co valence. The results are analyzed in the context of doping- and strain-dependent oxygen vacancy formation energies and diffusion coefficients, establishing that it is thermodynamic factors, not kinetics, that underpin the decrease in the threshold voltage with x, that is, with increasing formal Co valence. These findings substantially advance the practical and mechanistic understanding of this voltage-driven transformation, with fundamental and technological implications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Observation of large Rashba spin–orbit coupling at room temperature in compositionally engineered perovskite single crystals and application in high performance photodetectors

Indirect absorption extended below the direct transition edge and increase in carrier lifetime derived from Rashba spin–orbit coupling may advance the optoelectronic applications of metal halide perovskites. Spin-orbit coupling in halide perovskites is due to the presence of heavy elements in their structure. However, when these materials lack an inversion symmetry, for example by the application of strain, spin–orbit coupling becomes odd in the electron’s momentum giving rise to a splitting in the electronic energy bands. Here we report on the observation of a large Rashba splitting of 117 meV at room temperature, as predicted by relativistic first-principles calculations, in halide perovskite single crystals through a facile compositional engineering approach. Partial substitution of organic cations by rubidium in single crystals induces significant indirect absorption and dual peak photoluminescence as a result of a large Rashba splitting. We measured circularly polarized photoluminescence and magneto-photoluminescence in perovskite films printed by single crystals as well as magneto-electroluminescence and magneto-photocurrent in spin-LEDs based on perovskite single crystals. They indicated significant spin-momentum locking due to the large Rashba effect. A hybrid perovskite single crystal photodetector achieved record figures of merit, including detectivity of more than 1.3 × 10 18 Jones which represents a three orders of magnitude improvement compared to the to date record. Furthermore, these findings show that facile compositional engineering of perovskite single crystals holds great promise for further advancing the optoelectronic properties of existing materials.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Surface smoothing for laser powder-bed Ti-6Al-4V by a transient liquid phase

Surface roughness is the primary driver of fatigue for additively manufactured metals. To address surface roughness, this work introduces a new method to smooth features beyond line-of-sight without material removal. The method applies a coating that triggers local surface remelting by activating a eutectic reaction during heat treatment. The associated liquid phase then wets and isothermally solidifies into a smoother surface. For Ti-6Al-4V fabricated with laser powder bed fusion, samples with and without TLP smoothing (using a Cu coating) were characterized with a suite of techniques, including mechanical testing, electron backscatter diffraction, synchrotron X-ray tomography, and fractography. TLP smoothing reduced surface roughness by 80% and amplified compressive residual stress at the surface by about 50%. With statistically equivalent virtual microstructures, crystal plasticity scrutinized the roles of phases, porosity, and surface roughness. Although the tensile strain-to-failure was reduced to 1% strain, the TLP smoothing process increased high-cycle fatigue strength by about 20% compared to control samples, pointing to future opportunities to optimize the new process through various coating compositions and heat treatment schedules. Overall, this work establishes a new paradigm for treating surfaces of materials for smoothness and compressive residual stress.

Additive manufacturing↗

DOE OSTI2026

Evaluating the Transport Mechanism for Lignocellulosic Inhibitors in Zymomonas mobilis

The conversion of lignocellulosic biomass to biofuels and bioproducts is limited by small inhibitory molecules generated during the pretreatment process. The diverse compounds within the cell wall hydrolysate including aldehydes, carboxylic acids, phenolics, and alcohols inhibit microbial growth by disrupting microbial membranes. Although Zymomonas mobilis combines high ethanol productivity with hopanoid-rich membranes that confer solvent tolerance, hydrolysate compounds still inhibit microbial growth. One proposed mitigation strategy is to pump these molecules out through active transport processes, reducing direct toxicity. However, if passive permeation rates are high, active transport would create a futile cycle where the exported molecules diffuse back in, creating a net drag on fitness. To investigate this hypothesis, we measure the passive permeation for thirty-three lignocellulose derived compounds using atomistic molecular dynamics simulations with enhanced sampling. Permeability coefficients determined spanned more than eight orders of magnitude driven largely by the balance between hydrophobicity and polarity. Hydrophobic inhibitors such as aromatic acids, aldehydes, and short chain alcohols readily partitioned into the membrane and showed high permeability consistent with rapid passive influx and strong toxicity. Most polar molecules have lower but still appreciable permeation rates, with only the most polar sugars having low permeabilities. By integrating these predictions together with hydrolysate composition information, we find that most of these molecules are so permeable that futile cycles where passive permeation overwhelms efflux is highly likely. These findings provide a predictive framework for strain engineering, highlighting that, for highly permeable inhibitors, reducing extracellular inhibitor concentrations through hydrolysate detoxification, pretreatment optimization, or dilution may be necessary to mitigate futile cycling and improve microbial productivity in industrial biorefineries.

Zymomonas mobilis↗

DOE OSTI2024

Chapter 7.1: Microalgae

Microalgae is a unique biomass resource that does not need to compete for land and water with other biomass feedstocks because it can be cultivated on low-quality unencumbered land using noncompetitive water types including saline and wastewater. It is included as a complementary resource alongside other biomass feedstocks reported in this study, albeit at higher biomass production costs reflective of more capital-intensive farming operations than typical for terrestrial biomass. Higher biomass costs can be offset by the potential to produce value-added coproducts unique to compositional constituents of microalgae. Relative to BT16, this chapter reflects the latest analysis from the 2022 Algae Harmonization Update, which uses the latest parameterized and high-performing saline algal strain, second-generation carbon capture of point-source waste CO2 and high-pressure pipeline transport resolved to specific point-source types, saline water sourcing up to 40,000 mg/L total dissolved solids for source and makeup water salinity, blowdown water treatment and recycle, and brine disposal handling. National-scale algal biomass availability potential was calculated at 152 million tons/yr ash-free dry weight (AFDW) (191 million tons/yr dry weight) at an average biomass productivity of 26.2 g/m2 -day AFDW (about 50 tons/acre/yr dry weight).1 The algal biomass was cultivated on 3.9 million acres of multi-criteria screened and potentially available land for CONUS and fixed 268 million tons of waste CO2 based on biomass uptake. The algae biomass can be produced at an average MBSP of $674/ton AFDW ($536/ton dry weight) in 2020 dollars,2 corresponding to a total energy potential of 3.3 quads/yr at an average MBSP of $31.2/MMBtu (higher-heating-value [HHV] basis).

algae↗

DOE OSTI2025

Blending Compostable Plastics for Packaging Applications

Non-sustainable packaging materials (polymers) are a large portion of the increasing amount of plastic waste that become environmental pollutants. While many biodegradable or compostable polymers have been developed in recent years, most fail to compete with the non-sustainable polymers dominating the market, due to lack of certain desired properties, such as thermal (high melt temperature) and mechanical (high ductility) performance. For example, the popular compostable polymer polylactic acid (PLLA) has a high melt temperature but is very brittle. Another polymer, poly(d-valerolactone) (PVL) demonstrates great ductility but has a very low melt temperature. By blending PLLA and PVL, there is an opportunity to create a new biodegradable material with synergistic desired properties for packaging applications. In this study, we produce several (9) physical blends of PVL and PLLA with varying compositions of the two polymers while applying three different materials to make them more compatible (compatibilizers). We test the success of compatibilization by scanning electron microscopy (SEM), mechanic testing (strain at break) and differential scanning calorimetry (melting temperature). Overall, we highlight several promising materials with high compatibility and desired thermomechanical properties for sustainable packaging. Ideally, these materials could help mitigate future plastic pollution in Colorado and beyond.

blending↗

DOE OSTI2020

Structure and good piezoelectric performance in the complex system of Pb[(Zn,Ni)Nb]O 3 –Pb[(In,Yb)Nb]O 3 –Pb(Zr,Hf,Ti)O 3

High-performance piezoelectrics are always demanded for the high-end application. In this study, a complex piezoelectric system of 0.49Pb(Zn 1/2 Ni 1/2 ) 1/3 Nb 2/3 O 3 – x Pb(In 1/2 Yb 1/2 ) 1/2 Nb 1/2 O 3 –(0.51 – x )Pb(Zr 1/2 Hf 1/2 ) 0.1 Ti 0.9 O 3 (0.16 ≤ x ≤ 0.23) was fabricated through the solid-state method. The structure, ferroelectric, piezoelectric, and dielectric properties were investigated. The optimum piezoelectric coefficient d 33 of 761 pC/N, high Curie temperature of 169 °C, dielectric permittivity ( ε r ) of 4557, and electromechanical coupling coefficient ( k p ) of 63% were found at the morphotropic phase boundary composition of x = 0.19, which are superior to other complex piezoelectric materials. In particular, a significant large-signal d 33 * of 913 pm/V and low strain hysteresis (6%) was obtained in the temperature range of 20–170 °C. Temperature-dependent x-ray diffraction (XRD) has demonstrated that good temperature stability is put down to the structure stability. The agreement between the calculated lattice strain from in situ high-energy synchrotron XRD data and the macroscopic measurements suggests that the large lattice strain has a dominant contribution to the high piezoelectric response. The high piezoelectric performance and good temperature stability makes it potential for application.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Hidden diversity: Transcriptomic and photosynthetic variation among common ‘wild type’ Chlamydomonas strains

The unicellular green alga Chlamydomonas reinhardtii is a widely studied reference organism, particularly in photosynthesis research. It employs photoprotective mechanisms, such as state transitions (ST) and non-photochemical quenching (NPQ), to cope with rapid light changes. Most widely used strains share a recent common ancestor yet differ by up to ~50 000 nuclear variants—genetic diversity that is often overlooked. Even among ‘wild type’ strains, we document significant phenotypic differences, such as pigment accumulation, and nutrient utilization. To elucidate the basis for this variation, we compared transcriptomes and physiological traits of seven commonly used laboratory strains, including the reference strain and the CLiP mutant library parental strain. Despite identical growth conditions, ~40% of genes were differentially expressed between strains. Most of these differences are attributable to changes that have accrued during laboratory propagation, and adverse conditions may have driven transcriptomic drift. At the physiological level, we catalog the range of strain-dependent responses related to photosynthesis and high light (HL) acclimation. Specifically, (i) all strains develop NPQ upon HL exposure, but to various degrees, (ii) they show a substantial variation in ST capacity, and (iii) they regulate the composition of the photosynthetic apparatus differently. We find that NPQ levels do not correlate with LHCSR3 expression, suggesting an additional layer of NPQ regulation. STs are constantly activated and independent of growth light intensities. Overall, our findings highlight significant strain-to-strain differences in virtually all photosynthetic parameters, emphasizing the importance of careful strain selection in future research endeavors.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Effect of laminae count and manufacturing methods on mechanical properties of thin‐ply woven composites

Abstract Thin‐ply woven composites exhibit exceptional mechanical performance by delaying the onset of damage, making them suitable for high‐performance structural applications. This study outlines the impact of manufacturing techniques (vacuum bagging and hot pressing), ply count, and fiber waviness on the mechanical properties of aromatic thermosetting copolyester/carbon‐fiber (ATSP/CF) composites. The analysis encompasses several different ply counts, evaluating their effects on the in‐plane elastic modulus (0°–90°) and tensile strength. Results demonstrate that reducing the waviness (or crimp) ratio significantly enhances the in‐plane elastic modulus, with improvements up to 188%, highlighting the importance of fiber alignment. Vacuum bagging produced ply thicknesses from 128 to 58 μm for 1–36 plies, with in‐plane elastic moduli from 30.3 to 87.2 GPa, and 4‐ and 8‐ply samples showed approximately 40% higher stiffness than those made by hot pressing. ATSP resin with high thermal stability (up to 400°C) and recyclability was used. Furthermore, this study highlights the microstructural enhancements achieved through vacuum bagging, as revealed by scanning electron and optical microscopy, and micro‐computed tomography imaging. This paper provides insights into damage mitigation and achieving enhanced mechanical properties by controlling fiber waviness using vacuum bagging and higher ply count in thin‐ply ATSP/CF composites. Highlights Crimp ratio reduction enhances elastic in‐plane elastic modulus up to 188%. Vacuum bagging increases modulus over the hot pressing manufacturing method by 40%. Lowering thickness‐per‐ply increases failure strain from 0.8% to 1.2%. Explored the performance of a novel ATSP matrix with high recyclability and thermal stability.

Kushwaha, Shashank [The Grainger College of Engine↗

DOE OSTI2021

Alloying–realloying enabled high durability for Pt–Pd-3d-transition metal nanoparticle fuel cell catalysts

Abstract Alloying noble metals with non-noble metals enables high activity while reducing the cost of electrocatalysts in fuel cells. However, under fuel cell operating conditions, state-of-the-art oxygen reduction reaction alloy catalysts either feature high atomic percentages of noble metals (>70%) with limited durability or show poor durability when lower percentages of noble metals (<50%) are used. Here, we demonstrate a highly-durable alloy catalyst derived by alloying PtPd (<50%) with 3d-transition metals (Cu, Ni or Co) in ternary compositions. The origin of the high durability is probed by in-situ/operando high-energy synchrotron X-ray diffraction coupled with pair distribution function analysis of atomic phase structures and strains, revealing an important role of realloying in the compressively-strained single-phase alloy state despite the occurrence of dealloying. The implication of the finding, a striking departure from previous perceptions of phase-segregated noble metal skin or complete dealloying of non-noble metals, is the fulfilling of the promise of alloy catalysts for mass commercialization of fuel cells.

25 ENERGY STORAGE↗