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DOE OSTI2024

Defect-Limited Mobility and Defect Thermochemistry in Mixed A-Cation Tin Perovskites: (CH3NH3)1-xCsxSnBr3

Hybrid organic-inorganic semiconductors crystallizing in the perovskite structure present a significant opportunity for realizing defect-tolerant semiconductors. In this work, we examine the solid solution, (CH3NH3)1-xCsxSnBr3, and identify the thermochemistry dictating the intrinsic carrier concentrations and how local structural distortions influences this electronic behavior. This family of compounds exhibits the expected systematic trend in decreasing optical gap with the cesium to methylammonium A-site mixing ratio, x, in the visible region. However, the carrier mobility, as determined from time-resolved microwave conductivity measurements, trends opposite to that expected from first-principles calculations combined with Boltzmann scattering theory calculations of the carrier mobility. We propose that this is a result of increasing carrier scattering with x in (CH3NH3)1-xCsxSnBr3 due to a significant increase in the carrier density with x. By examining the dependence of the carrier density as a function of x, we infer the compositional-dependence of the average enthalpy and nonconfigurational entropy per defect. While diffraction reveals a cubic aristotypic perovskite structure as a function of x at room temperature, the pair distribution functions obtained from synchrotron X-ray total scattering from these materials are better described by symmetry-adapted displacement modes of the Pm3m crystal structure, which we attribute to a large degree of anharmonic dynamics of the atom positions. This analysis shows that CH3NH3+-rich compositions retain mostly linear Sn-Br-Sn bonding environments through the displacements, while Cs+-rich compositions lead to more significantly bent Sn-Br-Sn environments. We propose that these bent bonding arrangements in Cs-rich compositions yield a higher propensity for defect formation. This also provides a rationale for carrier trapping that gives rise to anomalous microwave transients. Together, these results provide insight into the structure-dynamics-properties relationships in this highly anharmonic system with high amplitude atomic motions and low defect formation energies.

defect thermochemistry↗

DOE OSTI2026

The Next Stage for Smart Cities: Metrics to Spur an Evolution from Technology for Efficiency to Technology for People's Needs

The Smart Cities movement is about a decade old, energized by the USDOT Smart Cities grant that sparked cities to dream big. Now, 10 years later, and multitudes of conferences and papers later, the biggest question regarding Smart Cities is whether any progress has been made? Smart Cities forums are typically led by the technology sector, either telecommunications, internet access, or most recently artificial intelligence (AI) concerns. Each of these areas have grown and found new applications in the context of Smart Cities, however, these technology applications are just tools toward ends. Do digital communications and assistance enable or foster improved access to real, tactile, non-virtual goods and services such as transportation, food, housing, trash removal, health care, education, social interaction? These and other topics are not 'big tech', but are each critical to quality of life outcomes and are day-to-day necessities, comprising many of the touch points through which citizens interact with municipal agencies. Regarding Smart Cities, relationships have not been fully refined as to how best to merge the emerging generation of technology and related trends with more mundane but essential requirements of tactile services. How should municipal managers and operators bring the range of new technology tools (e.g. on-demand transit, automated vehicles, digital connectivity) to bear to improve functions serving real- physical- non-virtual needs? How do we make cities more efficient in providing access to services and opportunities for improved quality of life? This paper examines the current Smart City movement, emerging trends, and the need to put metrics with respect to the delivery, access, and provision of real-life needs. Using a few case studies of past, present, and projected future scenarios, this paper attempts to bring Smart Cities into the real cities domain, perhaps pushing the moniker away from 'Smart' to 'Efficient' - something that can be measured, counted, and assessed. Through the consideration of the next stage of the evolution of cities from 'Smart' to 'Efficient', the combined efforts and experience of multiple researchers at the NREL and their network of collaborators highlights the need for updates metrics that can be used to start guiding efforts toward productive initiatives to improve quality of life.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2026

The solubility of ErPO 4 and Er speciation in hydrothermal fluids at varying pH and salinity between 350 and 450 °C

The rare earth elements (REE) are important for the green-energy transition and can be incorporated into the REE phosphates, such as xenotime-(Y), which also hosts heavy REE (Tb– Lu). Xenotime-(Y) is a common accessory mineral in metamorphic rocks and a range of mineral deposits where it controls the mobility of heavy REE, however, the impact of high temperature aqueous fluids on the behavior of heavy REE is largely unknown. Thermodynamic modeling can be utilized as a tool to predict the mobility of REE in hydrothermal aqueous fluids, but must be supported by accurate experimental data. Here, we measured the solubility of endmember synthetic xenotime-structured ErPO4 in NaCl-HCl-NaOH-bearing aqueous solutions at 350 °C and water vapor saturation pressure, at 400 and at 450 °C and 500 bar using batch-type Inconel reactors. Erbium speciation was investigated as a function of pH from 2.8 to 8, where Er chloride species are predominant at acidic conditions (pH <3) and Er hydroxyl complexes are predominant at near- neutral to alkaline conditions (pH >3). At pH 7–9, the measured ErPO 4 solubility (-9.8 to -7.5 log m Er ) is up to 2.5 orders of magnitude lower than thermodynamic predictions (-9.4 to -6.7 log m Er ) using existing thermodynamic databases. At pH 2–3, the predicted ErPO 4 solubility is ~0.5 orders of magnitude higher at 350 °C and ~1 order of magnitude lower at 450 °C compared to experimentally measured Er concentrations. The thermodynamic properties of aqueous Er species were therefore revised in this study. The partial molal Gibbs energy of formation (Δ f G 0 T,P ) for aqueous Er hydroxyl and chloride species are optimized using GEMSFITS and the logarithmic formation constants (logβ n ( Cl,OH) ) were derived at each experimental temperature and pressure. The updated thermodynamic properties for Er hydroxyl species (Er(OH) +2 , Er(OH) 2 + , and Er(OH) 3 0 ) show that their stability shifts to more acidic conditions at and below 400 °C. The Er chloride species (ErCl +2 and ErCl 2 + ) show increased stability compared to Er hydroxyl species at temperatures of 450 °C and 0.01 mol/kg NaCl. The updated thermodynamic properties are implemented into the GEM-Selektor modeling package to investigate the mobility of Er in saline hydrothermal fluids in equilibrium with alkaline rocks. Importantly, the updated properties for Er hydroxyl species result in low Er solubility at rock equilibrated pH conditions due to an expanded hydroxyl predominance zone, but lower aqueous complex stability overall, whereas previous models suggest greater stability for aqueous Er species. Furthermore, ErPO 4 solubility increases with decreasing temperature due to the deprotonation of HCl, which increases the acidity of hydrothermal fluids and the availability of Cl - to complex with the REE. These simulations highlight how fluid-rock reaction and temperature affect the mobility of REE in hydrothermal ore-forming systems.

58 GEOSCIENCES↗

DOE OSTI2026

Corrected Moments in Antenna Coordinates (CMAC) Technical Report

Various corrections are needed in order to extract the best value of the measurements from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility’s scanning precipitation radars. The Corrected Moments in Antenna Coordinates (CMAC) Value-Added Product provides an application chain for providing radar moments that are corrected for artifacts such as aliasing, attenuation, multi-trip echoes, and beam blockage. This technical report provides details on the entire process of correcting the ARM scanning precipitation radar data using CMAC. CMAC has been used at multiple ARM sites and ARM Mobile Facility deployments including the Tracking Aerosol Convection Interactions Experiment (TRACER), Cloud, Aerosol, and Complex Terrain Interactions (CACTI), and the Surface Atmosphere Integrated Laboratory (SAIL).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Development and implementation of high-throughput proteomic and metabolomics assays by using advanced chromatographic and mass spectrometric systems (CRADA Final Report)

The mission of this CRADA with Agilent was to couple powerful MS platforms (QQQ, IM-QTOFMS) with Agilent’s novel Ultra-High-Performance Liquid Chromatography (UHPLC) fast metabolomic workflows and perform ABF Machine Learning (ML) to generated datasets. Agilent transferred UHPLC methods to PNNL and LBNL and methods were implemented and demonstrated in both labs, achieving total acquisition times of < 10 min. Metabolites analyzed using Agilent’s shared methods included metabolites from central carbon metabolism, common across hosts, and metabolites unique to engineered strains. Standards were acquired in an UHPLC-Drift Tube Ion Mobility Mass Spectrometer (DTIMS) system for the first time within the context of ABF and methods were optimized based on Agilent’s protocols. Samples from ABF hosts Pseudomonas putida, Aspergillus pseudoterreus, Aspergillus niger and Rhodosporidium toruloides were analyzed using the UHPLC-DTIMS platform for a total of 276 runs. A data analysis workflow compatible with the Experimental Data Depot (EDD) and completely shareable was developed for the acquired UHPLC-DTIMS data. Samples were analyzed using a Data Independent Acquisition Approach (DIA), which for most of the standards provided more transitions therefore increasing detection confidence. Using the data acquired by PNNL, LBNL, and Agilent’s specifications from previous ML projects, SNL applied an ensemble ML strategy to pick the best performing model for automated LC-method selection. Finally, with the contribution of the participant labs and Agilent, SNL developed an Automated Method Selection (AMS) software tool to predict the best liquid chromatography method for analysis of any new molecules of interest. Samples with novel pathways and new metabolite targets of interest are generated at a high pace in the ABF. Overall, the project advanced rapid metabolomics by combining liquid chromatography, ion mobility spectrometry, and data-independent mass spectrometry with machine learning. This multidimensional approach uses retention time, collision cross-section, precursor mass, and fragment-ion information to distinguish chemically similar metabolites that can be difficult to resolve using conventional liquid- or gas-chromatography methods. The resulting workflow also provided automated metabolite-identification error estimates, addressing a recognized need for statistical confidence measures in metabolomics.

Petzold, Christopher [Lawrence Berkeley National L↗

DOE OSTI2026

The solubility and speciation of REE phosphate endmembers (CePO 4 and YPO 4 ) in Cl-rich aqueous fluids from 350 to 450 °C and implications for natural systems

The rare earth elements (REE) are important metals used increasingly in advanced technologies. Within the crust, the elements Ce and Y are commonly more abundant compared to other lanthanides and comprise important end-member constituents of REE-bearing minerals. Specifically, Ce is part of the light (L) REE which have larger ionic radii than the heavy (H) REE, which are grouped together with Y. These differences in ionic radius can lead to important physico-chemical trends within the lanthanide group. Despite a recent increase in experimental and thermodynamic data for the REE at high temperature and pressure, there is still a significant lack of these data at supercritical conditions. In this study we conducted batch-type experiments to measure the solubility of REE phosphates (CePO 4 and YPO 4 ) at varying starting pH (1.5–10), and salinity (0.01–1.4 mol/kg NaCl) at 350 and P sat , and from 400 to 450 °C at 700 bar. Results show that the solubility of Ce (33–0.14 ppb) is generally higher than Y (13–0.13 ppb) and that Ce complexes more strongly with both chloride and hydroxyl ligands compared to Y. The solubilities of both REE phosphates are highly pH-dependent and, to a lesser extent, depend on salinity at the studied conditions. The solubility data from this study were implemented into the GEMSFITS program to optimize the thermodynamic properties of Ce and Y hydroxyl and chloride species. The updated standard partial molal Gibbs energies of formation (Δ f G 0 T,P ) are used within the experimental temperature and pressure range to accurately predict the CePO 4 and YPO 4 solubility and Ce and Y speciation behavior. Based on the updated thermodynamic properties we also provide formation constants (log β n Cl,OH ) for Ce and Y hydroxyl and chloride species. Updated thermodynamic properties are applied to model REE-apatite dissolution and REE mobility based on the Pea Ridge iron oxide apatite deposit in Missouri, USA. The apatite dissolution model replicates natural observations including the replacement of monazite and xenotime after apatite and is an example of the utility of the new thermodynamic constants applied to supercritical crustal fluids. Furthermore, the findings of this study advance the predictive capabilities of geochemical models, our understanding of the behavior of individual REE, and permit modeling the overarching fractionation trends between LREE and HREE in supercritical crustal fluids.

58 GEOSCIENCES↗

DOE OSTI2025

Evaluating Direct and Indirect Influence on EV Charging Stations Across the US

The adoption of new technology for electric vehicles (EV) and mobility applications can bring underappreciated vulnerabilities to the power grid. One area of potential fraud and adversarial influence is through the business ecosystem of startups that own and deploy EV technology. Yet, there are no models or analyses that map the network of organizations and people that have direct and indirect influence over technologies currently deployed in the grid. To fill this gap, we develop a multilayer network model to measure direct and indirect influence on EV charging stations. First, we create and adversarial socio-technical network (ASTN) model via a data fusion pipeline for different US regions of interest (ROI). Then, we develop an integrated ASTN for Chicago, Los Angeles, New York, and Philadelphia. We rank EV charging companies direct influence within each geographic region as well as indirect influence via social network analysis. While some companies have strong direct and indirect influence (i.e., ChargePoint) others show a mismatch between their influence over charging stations and their position within the social network. For example, Tesla has strong direct influence on stations and weak indirect influence over competitors. In contrast, 7Charge has weak direct influence over stations, but strong indirect influence over competitors.

29 - ENERGY PLANNING, POLICY AND ECONOMY↗

DOE OSTI2026

Non-Invasive Electrode Impedance Estimation for Optimized Charge Profile Parameterization of Lithium-Ion Batteries

This work presents a non-invasive method for parameterizing a physically motivated equivalent circuit model of lithium-ion batteries using operando electrochemical impedance spectroscopy and time-domain data. The proposed model consists exclusively of linear circuit elements, enabling computationally efficient simulation and real-time implementation on battery management system chips. By integrating frequency- and time-domain measurements, the model accurately estimates internal states such as the negative electrode potential, achieving a root mean square error of 12.3 mV during fast charging validation. Parameterization requires only rate tests with sinusoidal perturbations at three different ambient temperatures, making the approach experimentally accessible. The model reveals key insights into battery behavior, including rate-dependent overpotentials primarily governed by charge transfer kinetics at the positive electrode, and temperature-dependent impedance contributions from both charge transfer and solid-state diffusion processes. Validation using reference electrodes confirms the model’s ability to detect lithium plating onset and reproduce impedance behavior across a wide range of operating conditions. The approach enables in situ optimization of fast charging profiles and lays the foundation for future extensions incorporating aging effects and plating dynamics.

25 ENERGY STORAGE↗

DOE OSTI2024

UV-Vis spectrophotometric determination of rare earth elements (REE) speciation at near-neutral to alkaline pH. Part I: m-cresol purple properties from 25-75 °C and Er hydrolysis

The speciation and mobility of rare earth elements (REE) strongly depends on pH which controls the formation of charged aqueous hydroxyl species. The latter potentially play an important role in controlling heavy REE adsorption on clay minerals in near-neutral to alkaline waters such as in regolith-hosted REE mineral deposits. However, accurate REE hydrolysis constants are needed for developing geochemical models that can predict the role of these charged species in natural systems. Here, we develop a robust experimental UV-Vis spectrophotometric method using m-cresol purple to determine in situ pH from 25 to 75 °C. This method is used to derive the average ligand number and hydrolysis constants of erbium (Er) at 25 °C in aqueous solutions with low ionic strength (≤ 0.001 mol/L) at pH from ~7 to 9.5 and in the presence of Er concentrations from 0 to 0.057 mM. The average ligand number ranges between 1 and 3 indicating that Er(OH) 2+ , Er(OH) 2 + and Er(OH) 3 0 control speciation in the experiments. The logarithm of the Er hydrolysis constants (log*β n ° , n= 1 to 3) derived at infinite dilution for the reaction Er 3+ + nH 2 O = Er(OH) n 3-n + nH + are: *β 1 ° = –7.22 ± 0.10, *β 2 ° = –14.52 ± 0.08, *β 3 ° = –23.24 ± 0.04. Implementation of these experimental data into a geochemical model indicates that the Er(OH) 2 + and Er(OH) 3 0 species are both stable in a much wider pH range than previously predicted. Consequently, the positively charged REE hydroxyl complexes can potentially control the fractionation of light vs. heavy REE via adsorption as observed in the formation of certain regolith-hosted REE deposits.

58 GEOSCIENCES↗

DOE OSTI2025

Research, Development and Demonstration of Advanced Vehicle Technologies in Clean Motor Fuels (CRADA Final Report)

NREL/DOE has been funding research, development, and demonstration (RD&D) projects to facilitate the deployment of alternative fuels into the marketplace in order to achieve three objectives: 1) enhance the reduction of mobile source emissions in California and the U.S.; 2) increase U.S. competitiveness and economic prosperity; and 3) preserve the environment through the reduction of emissions and toxins from the motor vehicle population. The Lewis-Presley Air Quality Management Act requires the South Coast Air Quality Management District to establish a program to encourage participation in projects to increase the utilization of clean-burning fuels. The parties seek to collaborate on a joint RD&D project to perform a field test on a small vehicle fleet operating on Fischer-Tropsch synthetic diesel fuel. Recently the 106th U.S. Congress designated "gas-to-liquid" (GTL) transportation fuels that are produced from domestic products as alternative fuels under the Energy Policy Act of 1992 (EPACT). Niche markets could develop quickly for these fuel products, perhaps especially for the use of Fischer-Tropsch synthetic fuels in centrally fueled vehicle fleets in California. NREL and its project partners from the U.S. Department of Energy and West Virginia University have recently conducted what we believe to be the first-ever controlled tests of Fischer-Tropsch synthetic fuels in heavy vehicles. These tests have shown that Fischer-Tropsch fuels can be substituted in unmodified trucks and buses without any detectable loss in drivability and performance. Compared to a California diesel fuel baseline, neat Shell Fischer-Tropsch fuel emitted about 12% lower NOx and 24% lower particulate matter over a five-mile driving route while maintaining the same fuel economy on an energy equivalent basis. Whereas these exhaust emissions reductions from these previous studies have been impressive, far greater exhaust emissions reductions can be achieved if the vehicles are retrofitted with emissions control technologies that are enabled by Fischer-Tropsch fuels. For this program, a test fleet would be selected and retrofitted with continuously regenerating traps (CRT’s) or diesel particulate filters (DPF's). The University of West Virginia, under a separate subcontract to SCAQMD will have the responsibility to test and measure the emissions from the test fleet of vehicles.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2025

Studying Aerosol, Clouds, and Air Quality in the Coastal Urban Environment of Southeastern Texas

A multi-agency succession of field campaigns was conducted in southeastern Texas during July 2021 through October 2022 to study the complex interactions of aerosols, clouds and air pollution in the coastal urban environment. As part of the Tracking Aerosol Convection interactions Experiment (TRACER), the TRACER- Air Quality (TAQ) campaign the Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) and the Convective Cloud Urban Boundary Layer Experiment (CUBE), a combination of ground-based supersites and mobile laboratories, shipborne measurements and aircraft-based instrumentation were deployed. These diverse platforms collected high-resolution data to characterize the aerosol microphysics and chemistry, cloud and precipitation micro- and macro-physical properties, environmental thermodynamics and air quality-relevant constituents that are being used in follow-on analysis and modeling activities. We present the overall deployment setups, a summary of the campaign conditions and a sampling of early research results related to: (a) aerosol precursors in the urban environment, (b) influences of local meteorology on air pollution, (c) detailed observations of the sea breeze circulation, (d) retrieved supersaturation in convective updrafts, (e) characterizing the convective updraft lifecycle, (f) variability in lightning characteristics of convective storms and (g) urban influences on surface energy fluxes. The work concludes with discussion of future research activities highlighted by the TRACER model-intercomparison project to explore the representation of aerosol-convective interactions in high-resolution simulations.

54 ENVIRONMENTAL SCIENCES↗