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762 records · Page 4

A stable high-humidity bubbler design to supply steam for solid oxide electrolysis cells

A stable steam supply is required for the operation of solid oxide electrolysis cells. Heated water bubblers are the most common method due to the simplicity and inherent safety of the method, however, several design challenges hinder effective implementation. Here, a stable and validated bubbler design is presented, capable of achieving very high steam concentrations, relatively high flow rates, and continuous operation. A piping and instrumentation diagram and bill of materials are provided to enable easy duplication. Critical design parameters are discussed, including safety considerations and materials requirements, which are applicable to any bubbler design. The practical implementation of bubblers is also presented, including methods to prevent condensation instability and reduce backpressure to achieve a stable steam supply. The 3″ x 6″ (7.6 cm × 15.2 cm) bubbler achieves up to 98% steam balance hydrogen at 200 sccm and up to 1 slpm at 96% steam.

08 - HYDROGEN

Crustal Deformation and Gravitational Effects From Dynamic Ocean Mass Redistribution Impact Projected Sea‐Level Change

As the climate warms, associated changes in ocean dynamics will redistribute sea‐water mass within the ocean, contributing to relative sea‐level change. This mass redistribution will cause additional sea‐level changes due to gravitational self‐attraction, deformation of the solid Earth, and shifts in the Earth's rotation axis (GRD), which are not incorporated in sea‐level projections. Using CMIP6 climate model output, we quantify relative sea‐level changes induced by GRD from ocean‐dynamic mass loading through 2100. These effects act to amplify projected ocean‐dynamic sea‐level patterns, causing sea‐level rise in coastal regions, particularly along wide continental shelves and at high latitudes. On average, the magnitude of such GRD‐induced sea‐level change is equivalent to ∼15% of the signal due to dynamic ocean mass redistribution. Although our results show substantial inter‐model spread, they reveal that GRD‐induced relative sea‐level changes from ocean mass redistribution represent a non‐negligible component of regional sea‐level change and should be considered in projections.

58 GEOSCIENCES

Dark Energy Survey year 6 results: Magnification modeling and its impact on galaxy clustering and galaxy-galaxy lensing cosmology

Gravitational lensing magnification alters the observed spatial distribution of galaxies and must be accounted for to prevent biases in cosmological probes of the large-scale structure. We investigate its effects on the Dark Energy Survey Year 6 galaxy clustering and galaxy-galaxy lensing analyses using the fiducial lens (position tracer) sample M ag L im++. Magnification bias is parameterized by a coefficient that describes the response of the number of selected objects per unlensed area element to a change in the lensing convergence. We quantify this coefficient using the BALROG synthetic source injection catalog to account for the complexity of the selection function, and compare these results with simplified estimates. The resulting values of the magnification coefficients for each redshift bin are [3.16 ± 0.08, 2.76 ± 0.21, 4.09 ± 0.15, 4.42 ± 0.16, 4.90 ± 0.29, 4.83 ± 0.25]. Relative to Year 3, this analysis provides more precise and accurate magnification bias estimates through a larger BALROG area and reweighting to better match the data properties. Here, the cosmological results are robust when tested against various magnification parameter prior choices and also when adding cross-clustering between lens redshift bins. Neglecting magnification, however, introduces significant systematic shifts: relative to the fiducial analysis with Gaussian priors centered on the BALROG -derived estimates, we observe shifts of 1.37σ in S 8 and -0.84σ in Ω m (with cosmic shear included: -0.61σ in S 8 and -0.71σ in Ω m ), in agreement with findings from simulated data, demonstrating that magnification must be modeled to avoid biases. Freeing the magnification bias in lens bin 2 leads to unphysical negative values, further justifying its exclusion from the fiducial Year 6 analysis.

Cosmological parameters

Laser–plasma amplification of an ultrabroadband laser pulse to 0.3 TW

Producing on-target laser intensities much greater than 10 23 W cm −2 with current laser technologies is a roadblock to accessing new regimes of physics such as strong-field quantum electrodynamics. Laser–plasma amplifiers show promise to realize these intensities by augmenting the final amplifier and compressor in traditional chirped-pulse-amplification architectures with a plasma-based amplification and compression stage that operates at a much higher damage threshold. Here we demonstrate amplification of an ultrabroadband (>60 nm) pulse in a laser–plasma Raman amplifier. We directly amplified seed intensities up to 3.7 × 10 15 W cm −2 and measured efficiencies up to 8.7%. Single-shot SPIDER measurements show a factor-of-2 reduction in the amplified pulse duration with final powers up to 0.3 TW, a 10× improvement over previous results. Final pulse durations of 64 fs are measured. Energy transfers greater than 220 mJ from the picosecond pump into the seed result in a 30× energy amplification of a 7.6 mJ seed. These results set the stage for a compact plasma afterburner based on Raman amplification that could extend the scientific capability of existing petawatt-class laser facilities to enable experiments at the intensity frontier.

Shaw, J. L. [Univ. of Rochester, NY (United States

Role of Amorphous Chains in Nanoplastic Formation from Semicrystalline Polymers

Semicrystalline polymers, e.g., polyethylene terephthalate (PET), release micro- (100 nm to 1 mm) and nanoplastics (up to 100 nm) [MNPL] when they are degraded under quiescent conditions. However, the exact molecular mechanisms leading to material fragmentation into MNPL are unknown. Here, we monitor the evolution of chain molecular weight and the MNPL production kinetics during hydrolysis of PET pellets. We find that only ~0.6% of the amorphous phase ester bonds are hydrolyzed at the onset of MNPL release. Then, by combining a random scission model with measured amorphous spacings, we estimate that only ~15% of the stress transmitters in the amorphous phase, namely, bridges and entangled loops, have failed by this point. Thus, spontaneous fragmentation of the semicrystalline nanostructure occurs despite significant intercrystalline connectivity. We resolve this apparent contradiction by proposing that fragmentation can only occur when progressive tie-chain scission causes the material to undergo the ductile/brittle transition. Mechanistically, we speculate that the internal stresses responsible for material fragmentation are caused by processing (i.e., residual stresses) and/or sample densification induced by chemi-crystallization. We discuss additional factors that may affect our analysis and thus require further investigation, such as skin-core effects, preferential degradation of stress transmitters and/or recrystallization processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

In situ studies on heavy ion irradiation and partial oxidation induced stacking faults and nanograins in tungsten nanolaminates

Understanding the microstructural evolution of tungsten (W) under extreme irradiation environments is critical for its application as a plasma-facing material in future fusion reactors. Heavy ion irradiation study offers expedited damage accumulation and thus allows irradiation tolerance property prediction in a short period of time. In this study we explore in situ Kr ion irradiation of W nanolaminates at 800 °C and uncover a complex interplay of irradiation-induced transformations, including the emergence of stacking faults, nanograin formation, and generation of thickened grain boundaries defined as GB regions with the thickness of up to 15 nm. High-resolution transmission electron microscopy studies reveal the formation of extended planar faults and a metastable hexagonal close-packed (hcp) phase within the body-centered cubic (bcc) matrix. These structural transitions are facilitated by irradiation-induced shear. They are further stabilized by the presence of oxygen, which promotes stacking fault formation and vacancy trapping. Elevated temperatures enhance defect mobility, enabling dynamic recrystallization into ultrafine grains and the thickening of GBs due to defect absorption and impurity segregation. These findings unravel non-equilibrium phase transformation pathways in heavy ion irradiated W and highlight the critical role of impurity-mediated defect dynamics in governing its radiation tolerance properties.

Wazeer, Adil [Purdue University]

Dynamics of Radiation Damage Buildup in Ultrathin Hexagonal Boron Nitride Films under Ion Bombardment

Two-dimensional hexagonal boron nitride (hBN) is attractive for several emerging applications. Ion bombardment can be used to modify the hBN properties. However, the understanding of radiation damage buildup in hBN remains limited. Here, we investigate the effects of the dose rate and ion mass on radiation damage buildup by studying 40 nm-thick hBN films bombarded at room temperature with 500 keV 4 He, 15 N, 40 Ar, and 129 Xe ions and comparing with results for ion bombardment of polycrystalline hBN ceramics. Raman spectroscopy is used to quantify damage buildup, and transmission electron microscopy is used for microstructural analysis. Experiments are complemented by molecular dynamics simulations of the formation and evolution of point defects. Lighter ions are found to be more efficient at disordering hBN than heavier ions. This observation points to a critical role of intracascade defect processes. In contrast, a negligible dose rate effect observed suggests limited intercascade defect dynamic annealing processes for these irradiation conditions. These findings provide a fundamental basis for hBN defect engineering.

2D materials

Aragonite saturation horizon variability along North Pacific seamounts and implications for deep-sea coral reefs

The 2014 discovery of living deep-sea coral reefs along the Northwest Hawaiian Islands (NWHI) and lower Emperor Seamount Chain (ESC), despite the North Pacific’s shallow aragonite saturation horizon (ASH) and high CaCO3 dissolution rates, underscores the need to understand the local seawater chemistry that allows these reefs to persist. We investigated seawater carbonate chemistry using discrete samples along the NWHI and ESC from two cruises ~1 year apart (08/26/21 – 09/26/21, 09/09/22 – 10/24/22). Across the two cruises, ASH depth difference ranged from 15 to 77 m. Since the Pacific ASH shoals by 1–2 m yr?¹, this long-term trend cannot explain the magnitude of ASH change observed between cruises. Temperature-salinity plots similarly indicate no major shifts in intermediate water masses that could account for these changes. Instead, ASH depth variability was primarily governed by localized biogeochemical processes, namely changes in intermediate water respiration and CaCO3 dissolution. Indicators for dissolution (TA*) and respiration (AOU) suggest changes in ASH depth were driven by changes in dissolution at the northern- and southern-most sites, whereas respiration exerted stronger control at central sites. Combining 2021 and 2022 data with data from 2014 – 2019 (excluding 2018) revealed high interannual ASH variability, by as much as >200 m at one site. Deep-sea coral reefs across the NWHI and ESC currently reside close to the ASH depth and likely experience seasonal and interannual shifts between under- and supersaturation. As ocean acidification progresses however, persistent exposure to undersaturated seawater could further threaten these critical deep-sea ecosystems.

coral reefs

Precise Modeling of a Complex Solenoidal Magnetic Field Using a Combination of Analytic Functions and a PINN

We demonstrate an iterative approach to modeling a sparsely measured magnetic field in a large-bore solenoid. This approach uses a hybrid of traditional and machine learning techniques. The traditional technique is a linear least-squares fit using a series solution to Laplace's equation, while the machine learning technique involves the training of a physics-informed neural network (PINN) on the least-squares fit residuals. We use a newly defined activation function "DELTAsnake," a modification to the snake activation function proposed by Ziyin et al. that allows for stronger curvature and non-monotonicity. The combined model approximately obeys Maxwell's equations to a level sufficient for producing high quality physics simulations and analysis. Our approach is applied to a highly realistic calculation of the expected magnetic field in the Mu2e experiment's Detector Solenoid which includes a simple model for the expected statistical measurement uncertainties. Using ten toy measurement simulations, we demonstrate the capabilities of our model in comparison to the least-squares method alone; the least-squares method alone results in a reduced chi-squared statistic of ${2.15 \pm 0.01}$, while our approach improves the reduced chi-square to ${1.034 \pm 0.005}$. Furthermore, for an average toy simulation, we show that the range of the RMS of the three field component residuals reduces from ${0.07-0.37}$ Gauss to ${0.05-0.07}$ Gauss. We find that this novel method is robust against a realistic systematic uncertainty deriving from Hall probe calibration bias and can be used to significantly reduce the number of measurements required to achieve an accurate model.

Kampa, Cole [Caltech] (ORCID:0000000192972920)

SPT clusters with DES and HST weak lensing. II. Cosmological constraints from the abundance of massive halos

We present cosmological constraints from the abundance of galaxy clusters selected via the thermal Sunyaev-Zel’dovich (SZ) effect in South Pole Telescope (SPT) data with a simultaneous mass calibration using weak gravitational lensing data from the Dark Energy Survey (DES) and the Hubble Space Telescope (HST). The cluster sample is constructed from the combined SPT-SZ, SPTpol ECS, and SPTpol 500d surveys, and comprises 1,005 confirmed clusters in the redshift range 0.25–1.78 over a total sky area of 5200 deg 2 . We use DES Year 3 weak-lensing data for 688 clusters with redshifts 𝑧 < 0.95 and HST weak-lensing data for 39 clusters with 0.6 < 𝑧 < 1.7. The weak-lensing measurements enable robust mass measurements of sample clusters and allow us to empirically constrain the SZ observable-mass relation without having to make strong assumptions about, e.g., the hydrodynamical state of the clusters. For a flat Λ⁢ CDM cosmology, and marginalizing over the sum of massive neutrinos, we measure Ω m = 0.286 ± 0.032, 𝜎 8 = 0.817 ± 0.026, and the parameter combination 𝜎 8 ⁢(Ω m /0.3) 0.25 = 0.805 ± 0.016. Our measurement of 𝑆 8 ≡ 𝜎 8 ⁢$\sqrt{Ω_{m}/0.3}$ = 0.795 ± 0.029 and the constraint from Planck CMB anisotropies (2018 TT, TE, EE+lowE) differ by 1.1⁢𝜎. In combination with that Planck dataset, we place a 95% upper limit on the sum of neutrino masses ∑𝑚 𝜈 < 0.18 eV. When additionally allowing the dark energy equation of state parameter 𝑤 to vary, we obtain 𝑤 = −1.45 ± 0.31 from our cluster-based analysis. In combination with Planck data, we measure 𝑤 =−1.3⁢4$^{+0.22}_{−0.15}$, or a 2.2⁢𝜎 difference with a cosmological constant. We use the cluster abundance to measure 𝜎8 in five redshift bins between 0.25 and 1.8, and we find the results to be consistent with structure growth as predicted by the Λ⁢ CDM model fit to Planck primary CMB data.

79 ASTRONOMY AND ASTROPHYSICS

Acute Exposure to Aerosolized Nanoplastics Modulates Redox-Linked Immune Responses in Human Airway Epithelium

Micro- and nanoplastics (MPs and NPs) are pervasive environmental pollutants detected in aquatic ecosystems, with emerging evidence suggesting their presence in airborne particles generated by water body motion. Inhalation exposure to airborne MPs and NPs remains understudied despite documented links between occupational exposure to these particles and adverse respiratory outcomes, including airway inflammation, oxidative stress, and chronic respiratory diseases. This study explored the effects of acute NP exposure on a fully differentiated 3D human airway epithelial model derived from 14 healthy donors. Airway epithelium was exposed to aerosolized 50 nm polystyrene NPs at concentrations ranging from 2.5 to 2500 µg/mL for three minutes per day over three days. Functional assays revealed no significant alterations in tissue integrity, cell survival, mucociliary clearance, or cilia beat frequency, suggesting intact epithelial function post-exposure. However, cytokine and chemokine profiling identified a significant five-fold increase in CCL3 (MIP-1α), a neutrophilic chemoattractant, in NP-exposed samples compared to controls. This was corroborated by increased neutrophil chemotaxis in response to conditioned media from NP-exposed tissues, indicating a pro-inflammatory neutrophilic response. Conversely, levels of interleukins (IL-21, IL-2, IL-15), CXCL10, and TGF-β were significantly reduced, suggesting immunomodulatory effects that may impair adaptive immune responses and tissue repair mechanisms. These findings demonstrate that short-term exposure to NP-containing aerosols induces a distinct pro-inflammatory response in airway epithelium, characterized by enhanced neutrophil recruitment and reduced secretion of key immune modulators. These findings underscore the potential for aerosolized NPs to induce oxidative and inflammatory stress, raising concerns about their long-term impact on respiratory health and redox regulation.

Biochemistry & Molecular Biology

Nonlinear reversal of photoexcitation on the attosecond time scale improves ultrafast X-ray diffraction images

The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.

Ulmer, Anatoli [Universität Hamburg (Germany)] (OR

Tunable high Néel temperature and large anomalous Hall response in antiferromagnetic Weyl semimetal Mn 3 Sn 1− x Ga x thin films

Antiferromagnetic Weyl semimetals based on Mn 3 X(X = Ge, Sn, Ga) kagome compounds exhibit the same ferromagnetic-like responses, including anomalous Hall, Nernst, and magneto-optical effects, as recently discussed for altermagnets. Driven by the Berry curvature due to Weyl fermions, these materials show a disproportionately large magnitude of electromagnetic effects even in the absence of large magnetization. For applications it is crucial to realize these responses in a wide range of temperatures both below and above 300 K. While stoichiometric Mn 3 X materials do not offer optimal performance, we show that Mn 3 Sn 1−x Ga x sputtered films with a variable composition offers a tunable Néel temperature, T N ≈ 425 ± 6–500 ± 15 K, which is crucial for device applications, together with a large tunable anomalous Hall effect. Our thin film growth method enables continuous and precise control over the film composition between x = 0 and x = 1. Through a detailed magnetization and Hall transport, we establish the magnetic phase diagram for the hexagonal Mn 3 Sn 1−x Ga x . Our results reveal an enhanced T N and antichiral magnetic phase in Ga-doped Mn 3 Sn and an enhanced anomalous Hall magnitude in Sn-doped Mn 3 Ga compared to their stoichiometric undoped forms. Our work demonstrates a route to optimize the technologically relevant antiferromagnets for various applications.

Magnetic properties and materials

Four Years of Type Ia Supernovae Observed by TESS: Early-time Light-curve Shapes and Constraints on Companion Interaction Models

Abstract We present 307 type Ia supernova (SN) light curves from the first 4 yr of the Transiting Exoplanet Survey Satellite mission. We use this sample to characterize the shapes of the early-time light curves, measure the rise times from first light to peak, and search for companion star interactions. Using simulations, we show that light curves must have noise <10% of the peak flux to avoid biases in the early-time light-curve shape, restricting our quantitative analysis to 74 light curves. We find that the mean power-law index t β 1 of the early-time light curves isβ 1 = 1.93 ± 0.57, and the mean rise time to peak is 15.7 ± 3.5 days. The underlying population distribution forβ 1 may instead consist of a Gaussian component with mean 2.29, width 0.34, and a long tail extending to values less than 1.0. We find that the data can rarely distinguish between models with and without companion interaction models. Nevertheless, we find three high-quality light curves that tentatively prefer the addition of a companion interaction model, but the statistical evidence for the companion interactions is not robust. We also find two SNe that disfavor the addition of a companion interaction model to a curved power-law model. Taking the 74 SNe together, we calculate 3σupper limits on the presence of companion signatures to control for orientation effects that can hide companions in individual light curves. Our results rule out common progenitor systems with companions having Roche lobe radii >31R ⊙ (separations >5.7 × 10 12 cm, 99.9% confidence level) and disfavor companions having Roche lobe radii >10R ⊙ (separations >1.9 × 10 12 cm, 95% confidence level). Lastly, we discuss the implications of our results for the intrinsic fraction of single degenerate progenitor systems.

Astronomy & Astrophysics

Single particle – MC-ICP-MS for isotopic analysis of uranium particles

Single particle – multi-collector – inductively coupled plasma – mass spectrometry (SP-MC-ICP-MS) was employed to measure a suspension of 1 µm U3O8 particles (∼1.3 pg total U/particle) to determine their individual isotopic compositions of 234U/238U, 235U/238U, and 236U/238U. The effects of different detector combinations for 235U and 238U, including secondary electron multipliers (SEM) and Faraday detectors (1011 and 1013 Ω amplifiers), were explored for accuracy and precision optimization on the observed 235U/238U. The minor isotopic ratios (i.e., 234U/238U and 236U/238U) were analyzed such that the 234U and 236U were monitored on SEM detectors and the 238U was monitored on a Faraday (1011 Ω) detector. Various integration times (5, 10, 25, and 50 ms) were investigated in all detector configurations to gain a better understanding of their impact on sensitivity, accuracy, and precision. For 235U/238U ratios of 1 µm U3O8 particles, a dual Faraday detector measurement with 1011 Ω was the optimal choice; measurement of 1021 particles yielded an average 235U/238U ratio of 0.00170 (14), a −1.8% relative difference (% RD) from the reference value. The minor isotopic compositions were determined to be 0.0000070 (14) and 0.0000758 (48) for the 234U/238U and 236U/238U, respectively. These measurements correspond to <8% and <1% RD from their reference value for the 234U/238U and 236U/238U, respectively. SP-MC-ICP-MS was also able to provide insight into measurement sensitivity. In these individual particles, merely 15 and 165 atto-grams (ag) of 234U and 236U were present (calculated). Initial limits of detection for SP-MC-ICP-MS were determined to be ∼1.0 ag (when measured via SEM detectors). This valuable approach is applicable to areas including nuclear forensics, nuclear safeguards, and geochemical analysis, which require high-precision measurements of uranium within micron-sized particles.

Manard, Benjamin [ORNL] (ORCID:0000000207400627)

Integration of ultra-low coverage whole-genome sequences for reconstructing the evolutionary history of Galapagos giant tortoises

Genomic data from contemporary and historical samples often need to be coupled for evolutionary reconstructions of multitaxon complexes. However, the genetic data recovered from historical samples may result only in ultra-low coverage whole-genome sequences (ulcWGS; <0.15× depth), leading to inaccurate evolutionary inferences given a preponderance of missing data. Using the Galapagos giant tortoise radiation as a study system (Chelonoidis spp., composed of 13 extant and four extinct lineages), we assembled a novel methodological pipeline that removes potential noise introduced by the missing data and enhances the evolutionary signal from ulcWGS samples. We leveraged existing tools for phylogenomic placement (EPA-ng), population genomic structure (smartsnp) and admixture (Admixfrog, NGSadmix) to demonstrate that the evolutionary history of samples can be uncovered with sequencing depths as low as 0.008–0.139×. Importantly, these approaches do not use genotype imputation of the ulcWGS samples, which would require extensive reference datasets. Our application to two cases of extinct lineages of Galapagos giant tortoises, with and without references from the same lineage, demonstrates the general value of the approach. We confirm where the extinct lineages from San Cristóbal and Santa Fe islands fit into the Galapagos giant tortoise radiation, and that these lineages were evolutionarily distinct entities.

ancient DNA

Heat exposure and maternal stress: evidence from the GRAPHS pregnancy cohort in Ghana

Heat exposure has been linked to psychosocial stress, an established antecedent of perinatal depression; however, evidence on heat-related stress during pregnancy in sub-Saharan Africa remains limited. We analyzed psychosocial stress scores and covariate data from the Ghana Randomized Air Pollution and Health Study, linking daily maximum and minimum shaded wet bulb globe temperature (WBGT) metrics to participants’ stress scores derived from the Crisis in Family Systems-Revised Life Events Questionnaire. We evaluated associations using ordinal logistic regression of pregnancy-average and trimester-average exposures and distributed lag non-linear models (DLNMs) to assess time-varying associations across gestation. Higher average maximum WBGT exposure across pregnancy was associated with increased odds of higher psychosocial stress; each 1 °C increase in maximum WBGT was associated with 64% higher odds of belonging to a higher stress category (OR = 1.64; 95% CI = 1.17–2.31; p = 0.0040). In trimester-average models, higher first-trimester maximum WBGT was also associated with higher stress (OR = 1.44; 95% CI = 1.15–1.81; p = 0.0014). DLNMs suggested that relatively cooler daily maximum WBGT values (25th percentile) were associated with decreased odds of stress in early pregnancy, whereas extreme daily maximum WBGT values (99th percentile) showed a pattern consistent with increased odds of stress in mid-to-late gestation. These findings highlight gestational windows in which heat exposure may influence stress, emphasizing the need for further research into underlying mechanisms and effective interventions to protect maternal mental health in heat-vulnerable settings.

White, Lewis [Columbia University] (ORCID:00090005

Electrolyte-Induced Restructuring of Acid-Stable Oxygen Evolution Catalysts

Crystalline metal oxide catalysts operating under oxygen evolution reaction (OER) conditions invariably restructure, resulting in active sites with hydroxo/oxo species in an amorphous environment. An increase in the population of terminal hydroxo/oxo species (i.e., edge sites) facilitates proton-coupled electron-transfer (PCET) kinetics for oxygen generation and thus improves catalyst competency. While amorphous films benefit from a greater density of active sites, they suffer from diminished charge transport as compared to that of extended crystalline lattices. Managing this amorphous–crystalline dichotomy is essential when designing OER catalysts, which we highlight with the examination of electrodeposited PbO x materials, which historically are very poor OER catalysts. Along these lines, the presence of phosphate during PbO x electrodeposition truncates the growth of an extended lattice owing to its strong bonding to oxide surfaces to afford an amorphous catalyst film (A-PbO x ) with significant charge-transfer resistance (138 ± 42 Ω) and poor OER kinetics (420 ± 105 mV dec –1 Tafel slope). Conversely, electrodeposition of Pb 2+ in the presence of less coordinating electrolytes such as nitrate affords crystalline β-PbO2 with improved charge-transfer resistance (42.6 ± 1.1 Ω), though still poor OER kinetics (134 ± 36 mV dec –1 Tafel slope). By operating amorphous A-PbOx in less coordinating electrolytes, however, a new partially crystalline material can be generated (μc-PbO x ) with further reduced charge-transfer resistance (33.0 ± 1.4 Ω) and improved OER kinetics (70 ± 15 mV dec –1 Tafel slope). The enhanced OER activity of μc-PbO x is the result of coupling the high edge-site population of an amorphous PbOx phase with crystalline-like charge transport properties. Finally, the ability to use an electrolyte to induce OER activity in an inactive amorphous form of PbO x highlights the benefits of optimizing the amorphous–crystalline phase compositions in the design of active OER catalysts.

catalysts