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At least 1,603 records · Page 89
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Influence of Electrode Interfaces on the Stability of Perovskite Solar Cells: Reduced Degradation Using MoO x /Al for Hole Collection

We investigated and characterized the stability of the power output from methylammonium lead iodide perovskite photovoltaic devices produced with various hole-collecting anode configurations consisting of Au, Ag, MoOx/Au, MoOx/Ag, and MoOx/Al. The unencapsulated devices were operated under constant illumination and constant load conditions in laboratory ambient with periodic current-voltage testing. Although the initial efficiencies of devices were comparable across these configurations, the stability of these devices varied significantly due to subtle differences in the electrode structure. Specifically, we found that devices with MoOx/Al electrodes are more stable than devices with more conventional, and more costly, Au and Ag electrodes. We demonstrate that a thin MoOx layer inhibits decomposition of the perovskite films under illumination in ambient laboratory conditions and greater improvements in device stability are achieved specifically with MoOx/Al electrodes. We investigated the role of the MoOx interlayer in the MoOx/Al electrodes by exploring the effect of relative humidity and the MoOx interlayer thickness on the perovskite solar cell stability.

14 SOLAR ENERGY↗
DOE OSTI2024

Colloidal Dispersions of Sterically and Electrostatically Stabilized PbS Quantum Dots: Structure Factors, Second Virial Coefficients, and Film-Forming Properties

Electrostatically stabilized nanocrystals (NCs) and, in particular, quantum dots (QDs) hold promise for forming strongly coupled superlattices due to their compact and electronically conductive surface ligands. However, studies of the colloidal dispersion and interparticle interactions of electrostatically stabilized sub-10 nm NCs have been limited, hindering the optimization of their colloidal stability and self-assembly. In this study, we employed small-angle X-ray scattering (SAXS) experiments to investigate the interparticle interactions and arrangement of PbS QDs with thiostannate ligands (PbS-Sn2S64-) in polar solvents. The study reveals significant deviations from the ideal solution behavior in electrostatically stabilized QD dispersions. Our results demonstrate that PbS-Sn2S64- QDs exhibit long-range interactions within the solvent, in contrast to the short-range steric repulsion characteristic of PbS QDs with oleate ligands (PbS-OA). Introducing highly charged multivalent electrolytes screens electrostatic interactions between charged QDs, reducing the length scale of the repulsive interactions. Furthermore, we calculated the second virial (B2) coefficients from SAXS data, providing insights into how surface chemistry, solvent, and size influence pair potentials. Finally, we explore the influence of long-range interparticle interactions of PbS-Sn2S64- QDs on the morphology of films produced by drying or spin-coating colloidal solutions. The long-range repulsive term of PbS-Sn2S64- QDs promotes the formation of amorphous films, and screening the electrostatic repulsion by the addition of an electrolyte enables the formation of crystalline domains. These findings highlight the critical role of NC-NC interactions in tailoring the properties of functional materials made of colloidal NCs.

SAXS↗
DOE OSTI2015

Enhanced Luminescent Stability through Particle Interactions in Silicon Nanocrystal Aggregates

Close-packed assemblies of ligand-passivated colloidal nanocrystals can exhibit enhanced photoluminescent stability, but the origin of this effect is unclear. Here, we use experiment, simulation, and ab initio computation to examine the influence of interparticle interactions on the photoluminescent stability of silicon nanocrystal aggregates. The time-dependent photoluminescence emitted by structures ranging in size from a single quantum dot to agglomerates of more than a thousand is compared with Monte Carlo simulations of noninteracting ensembles using measured single-particle blinking data as input. In contrast to the behavior typically exhibited by the metal chalcogenides, the measured photoluminescent stability shows an enhancement with respect to the noninteracting scenario with increasing aggregate size. We model this behavior using time-dependent density functional theory calculations of energy transfer between neighboring nanocrystals as a function of nanocrystal size, separation, and the presence of charge and/or surface-passivation defects. In conclusion, our results suggest that rapid exciton transfer from “bright” nanocrystals to surface trap states in nearest-neighbors can efficiently fill such traps and enhance the stability of emission by promoting the radiative recombination of slowly diffusing excited electrons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Effects of Catalyst Processing on the Activity and Stability of Pt–Ni Nanoframe Electrocatalysts

Pt-based alloys have shown great promise as cathodic catalysts for cost-effective proton exchange membrane fuel cells. Post-synthesis treatment has been recognized as a critical step to improve the catalytic performance of Pt-based alloys. Here we present the effects of catalyst processing on the catalytic behavior of Pt-Ni nanoframe electrocatalysts in oxygen reduction reaction. The Pt-Ni nanoframes were made by corroding Ni-rich phase from solid rhombic dodecahedral particles. Three different corrosion procedures were compared. Among them, electrochemical corrosion led to the highest initial specific activity (1.35 mA cm -2 at 0.95 VRHE) by retaining more Ni in the nanoframes. However, the high activity gradually went down in a subsequent stability test due to continuous Ni loss and concomitant surface reconstruction. On the other hand, the best stability was achieved by a more aggressive corrosion using oxidative nitric acid. Although the initial activity was compromised, this procedure imparted a less-defective surface and thus the specific activity dropped by only 7% over 30,000 potential cycles. These results indicate a delicate trade-off between the activity and stability of Pt-Ni nanoframe electrocatalysts. The obtained understandings on how to balance the activity-stability trade-off via catalyst processing can be generalized to other Pt-based alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Growth of Carbon Nanotubes Using Mixed-Metal Catalysts That Include Heavy Refractory Metals as Catalyst Stabilizers

Here, we report new findings from studies of a novel technique to augment the growth of CNTs. In this method, the catalytic metals used for CNT growth are combined with high-melting-point heavy refractory metals, which serve to stabilize the metal catalyst nanoparticles, from which the CNTs nucleate and grow. Our study investigates the combination of an iron catalyst with tungsten and osmium refractory stabilizers. We find that both tungsten and osmium enhance the lifetime of the iron catalyst particles by a factor of approximately two. Tungsten stabilizer resulted in production of CNTs longer by a factor of 1.25 compared to those produced using a pure iron catalyst, while the osmium stabilizer did not significantly affect the ultimate length of the CNTs due to the decreased CNT growth rate with a combined Fe/Os catalyst. These results suggest a possible new route toward producing CNTs with lengths sufficient for materials applications.

Park, Wonjung [Univ. of Tampa, FL (United States)]↗
DOE OSTI2016

Bio-oil Stabilization by Hydrogenation over Reduced Metal Catalysts at Low Temperatures

Biomass fast pyrolysis integrated with bio-oil upgrading represents a very attractive approach for converting biomass to hydrocarbon transportation fuels. However, the thermal and chemical instability of bio-oils presents significant problems when they are being upgraded, and development of effective approaches for stabilizing bio-oils is critical to the success of the technology. Catalytic hydrogenation to remove reactive species in bio-oil has been considered as one of the most efficient ways to stabilize bio-oil. This paper provides a fundamental understanding of hydrogenation of actual bio-oils over a Ru/TiO2 catalyst under conditions relevant to practical bio-oil hydrotreating processes. Bio-oil feed stocks, bio-oils hydrogenated to different extents, and catalysts have been characterized to provide insights into the chemical and physical properties of these samples and to understand the correlation of the properties with the composition of the bio-oil and catalysts. The results indicated hydrogenation of various components of the bio-oil, including sugars, aldehydes, ketones, alkenes, aromatics, and carboxylic acids, over the Ru/TiO2 catalyst and 120 to 160oC. Hydrogenation of these species significantly changed the chemical and physical properties of the bio-oil and overall improved its thermal stability, especially by reducing the carbonyl content, which represented the content of the most reactive species (i.e., sugar, aldehydes, and ketones). The change of content of each component in response to increasing hydrogen additions suggests the following bio-oil hydrogenation reaction sequence: sugar conversion to sugar alcohols, followed by ketone and aldehyde conversion to alcohols, followed by alkene and aromatic hydrogenation, and then followed by carboxylic acid hydrogenation to alcohols. Hydrogenation of bio-oil samples with different sulfur contents or inorganic material contents suggested that sulfur poisoning of the reduced Ru metal catalysts was significant during hydrogenation; however, the inorganics at low concentrations had minimal impact at short times on stream, indicating that sulfur poisoning was the primary deactivation mode for the bio-oil hydrogenation catalyst. Reducing the sulfur content in bio-oil could significantly increase the lifetime of the hydrogenation catalyst used. The knowledge gained during this work will allow rational design of more effective catalysts and processes for stabilizing and upgrading bio-oils.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Rutile-Deposited Pt–Pd clusters: A Hypothesis Regarding the Stability at 50/50 Ratio

Mixed Pt–Pd clusters deposited on oxides have been of great interest to catalysis. Clusters containing Pt and Pd in roughly equal proportions were found to be unusually stable against sintering, one of the major mechanisms of catalyst deactivation. After aging of such catalysts, the 50/50 Pt–Pd and Pd–O clusters appeared to be the two most prevalent phases. The reason for the enhanced stability of these equally proportioned clusters has remained unclear. In the following, sintering of mixed Pt–Pd clusters on TiO2(110) for various initial atomic concentrations of Pt and Pd and at a range of catalytically relevant temperatures was simulated. It is confirmed that equally mixed clusters have the relatively highest survival rate. Surprisingly, subnanoclusters containing Pt and Pd in all proportions have very similar geometries and chemical bonding, revealing no apparent explanation for favoring the 1:1 Pt/Pd ratio. However, it was discovered that at high temperatures, the 50/50 clusters have considerably more thermally accessible isomers than clusters containing Pt and Pd in other proportions. Hence, one of the reasons for stability is entropic stabilization. Electrostatics also plays a key role as a subtle charge redistribution, and a shift of electron density to the slightly more electronegative Pt results in the partially charged atoms being further stabilized by intracluster Coulomb attraction; this effect is greatest for 1:1 mixtures.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2022

Entropy Stabilization Effects and Ion Migration in 3D “Hollow” Halide Perovskites

A recently discovered new family of 3D halide perovskites with the general formula (A) 1–x (en) x (Pb) 1–0.7x (X) 3–0.4x (A = MA, FA; X = Br, I; MA = methylammonium, FA = formamidinium, en = ethylenediammonium) is referred to as “hollow” perovskites owing to extensive Pb and X vacancies created on incorporation of en cations in the 3D network. The “hollow” motif allows fine tuning of optical, electronic, and transport properties and bestowing good environmental stability proportional to en loading. To shed light on the origin of the apparent stability of these materials, we performed detailed thermochemical studies, using room temperature solution calorimetry combined with density functional theory simulations on three different families of “hollow” perovskites namely en/FAPbI 3 , en/MAPbI 3 , and en/FAPbBr 3 . We found that the bromide perovskites are more energetically stable compared to iodide perovskites in the FA-based hollow compounds, as shown by the measured enthalpies of formation and the calculated formation energies. The least stable FAPbI 3 gains stability on incorporation of the en cation, whereas FAPbBr 3 becomes less stable with en loading. This behavior is attributed to the difference in the 3D cage size in the bromide and iodide perovskites. Configurational entropy, which arises from randomly distributed cation and anion vacancies, plays a significant role in stabilizing these “hollow” perovskite structures despite small differences in their formation enthalpies. With the increased vacancy defect population, we have also examined halide ion migration in the FA-based “hollow” perovskites and found that the migration energy barriers become smaller with the increasing en content.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Local Cation-Ordered Superlattice Stabilizing Ni-Rich Single-Crystalline Cathodes

Ni-rich single-crystalline cathodes are pivotal for advancing lithium-ion battery technology due to their high energy density and mechanical stability. However, Ni-rich single-crystalline particles face intrinsic structural heterogeneity due to excessively high sintering temperature required to shape micron-sized morphologies─typically over 150 °C above the polycrystalline optimum, leading to rapid electrochemical decay and unsatisfied rate performance that hinder their practical application. Here, in this work, we propose a lithium-deficient presintering strategy to synthesize cation-ordered single-crystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 (S-NCM83), effectively minimizing lattice chemical heterogeneity and defect formation. The resulting cation-ordered percolation network enhances the structural stability of the bulk, reduces the energy barrier for Li + migration, and stabilizes Li + diffusion pathways. Consequently, S-NCM83 demonstrates significantly improved cycling stability across various operating temperatures and achieves exceptional rate performance, delivering 206 mAh g –1 at 0.1 C and 170 mAh g –1 at 5 C, without requiring surface coatings or doping. This work introduces a universal strategy to address the long-standing structural instability issues in single-crystalline cathodes, paving the way for simplified and scalable approaches to long-life and high-energy lithium-ion batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Single-Electron Transfer Stabilizes Metastable Alane in a Bipyridine-Functionalized MOF Nanopore

Nanoconfinement of metastable hydrides such as alane (AlH 3 ) in functionalized porous frameworks represents a promising yet largely untapped strategy for high-capacity energy storage. Despite its potential, the underlying mechanisms responsible for the thermodynamic stabilization of metastable hydrides are poorly understood. Here, in this study, concepts from solution Lewis acid–base chemistry were applied to a crystalline metal–organic framework (MOF) to stabilize AlH 3 . The long-range order and synthetically versatile pore chemistry enabled us to reveal the intimate details of the hydride-host interactions. Powder X-ray diffraction (PXRD) of AlH 3 -infiltrated UiO-67bpy (Zr 6 O 4 (OH) 4 (bpydc) 6 ; bpydc 2– = 2,2′-bipyridine-5,5′-dicarboxylate) confirms that the framework maintains its crystallinity up to 250 °C and is stable under 70 MPa H 2 pressure. We find that thermodynamic stabilization arises from coupled single-electron and hydrogen-atom transfer from AlH 3 to bipyridine-containing linkers. Electron paramagnetic resonance detects a bipyridyl radical with an anisotropic g-tensor (g values of 2.00132, 2.00215, and 2.00275), consistent with Bader charge analysis predicting 0.82 e – transferred from the hydride to the MOF. These findings establish critical structure–property relationships underpinning AlH 3 stabilization and suggest general strategies for tuning the thermodynamics and kinetics of metastable materials.

Shivanna, Mohana [Sandia National Laboratories (SN↗
DOE OSTI2017

Stabilizing CuPd Nanoparticles via CuPd Coupling to WO 2.72 Nanorods in Electrochemical Oxidation of Formic Acid

Stabilizing a 3d-transition metal component M from an MPd alloy structure in an acidic environment is key to the enhancement of MPd catalysis for various reactions. Here we show a strategy to stabilize Cu in 5 nm CuPd nanoparticles (NPs) by coupling the CuPd NPs with perovskite-type WO 2.72 nanorods (NRs). The CuPd NPs are prepared by controlled diffusion of Cu into Pd NPs and the coupled CuPd/WO 2.72 are synthesized by growing WO 2.72 NRs in the presence of CuPd NPs. The CuPd/WO 2.72 can stabilize Cu in 0.1 M HClO4 solution and, as a result, they show Cu, Pd composition dependent activity for the electrochemical oxidation of formic acid in 0.1 M HClO 4 + 0.1 M HCOOH. Among three different CuPd/WO 2.72 studied, the Cu 48 Pd 52 /WO 2.72 is the most efficient catalyst with its mass activity reaching 2086 mA/mgPd in a broad potential range of 0.40 to 0.80 V (vs. RHE) and staying at this value after the 12 h chronoamperometry test at 0.40 V. The synthesis can be extended to obtain other MPd/WO 2.72 (M = Fe, Co, Ni), making it possible to study MPd-WO 2.72 interactions and MPd stabilization on enhancing MPd catalysis for various chemical reactions.

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

Phase Control on Surface for the Stabilization of High Energy Cathode Materials of Lithium Ion Batteries

The development of high energy electrode materials for lithium ion batteries is challenged by their inherent instabilities, which become more aggravated as the energy densities continue to climb, accordingly causing increasing concerns on battery safety and reliability. Here, taking the high voltage cathode of LiNi 0.5 Mn 1.5 O 4 as an example, we demonstrate a protocol to stabilize this cathode through a systematic phase modulating on its particle surface. We are able to transfer the spinel surface into a 30 nm shell composed of two functional phases including a rock-salt one and a layered one. The former is electrochemically inert for surface stabilization while the latter is designated to provide necessary electrochemical activity. The precise synthesis control enables us to tune the ratio of these two phases, and achieve an optimized balance between improved stability against structural degradation without sacrificing its capacity. This study highlights the critical importance of well-tailored surface phase property for the cathode stabilization of high energy lithium ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2014

Activity–Stability Trends for the Oxygen Evolution Reaction on Monometallic Oxides in Acidic Environments

In the present study, we used a surface-science approach to establish a functional link between activity and stability of monometallic oxides during the OER in acidic media. We found that the most active oxides (Au< >Pt>Ir>Ru>>Os) materials. We suggest that the relationships between stability and activity are controlled by both the nobility of oxides as well as by the density of surface defects. This functionality is governed by the nature of metal cations and the potential transformation of stable metal cation with a valance state of n= +4 to unstable metal cation with n > +4. A practical consequence of such a close relationship between activity and stability is that the best materials for the OER should balance stability and activity in such a way that the dissolution rate is neither too fast nor too slow.

Danilovic, Nemanja↗
DOE OSTI2018

Mineralogical Controls on Frictional Strength, Stability, and Shear Permeability Evolution of Fractures

Massive fluid injection into the subsurface can induce microearthquakes by reactivating preexisting faults or fractures as seismic or aseismic slip. Such seismic or aseismic shear deformationsmay result in different modes of permeability evolution. Previous experimental studies have explored frictional stability-permeability relationships of carbonate-rich and phyllosilicate-rich samples under shear, suggesting that friction-permeability relationship may be primarily controlled by fracture minerals. We examine this relationship and identify the role of mineralogy (i.e., tectosilicate, carbonate, and phyllosilicate content) using direct-shear experiments on smooth saw-cut fractures of natural rocks and sintered fractures with distinct mineralogical compositions. These results indicate that the friction-permeability relationship is controlled by mineralogy. Frictional strength and permeability change upon reactivation decrease with phyllosilicate content but increase with tectosilicate content. In contrast, the reverse trend is observed for frictional stability (a-b). However, the permeability change decreases with carbonate content while both frictional strength and stability increase. The permeability change always decreases with an increase in frictional stability. This relationship implies a new mechanical-hydrochemical coupling loop via a linkage of frictional properties, mineralogy, and permeability.

58 GEOSCIENCES↗
DOE OSTI2019

Ensemble Shear Strength, Stability, and Permeability of Mixed Mineralogy Fault Gouge Recovered From 3D Granular Models

We conduct numerical shear experiments on mixtures of quartz and talc gouge using a three-dimensional (3D) distinct element model. A modified slip-weakening constitutive law is applied at contacts. We perform velocity-stepping experiments on both uniform and layered mixtures of quartz and talc analogs. We separately vary the proportion of talc in the uniform mixtures and talc layer thickness in the layered mixtures. Shear displacements are cycled through velocities of 1 and 10 μm/s. We follow the resulting evolution of ensemble shear strength, slip stability, and permeability of the gouge mixture and explore the mesoscopic mechanisms. Simulation results show that talc has a strong weakening effect on shear strength—a thin shear-parallel layer of talc (three particles wide) can induce significant weakening. However, the model offsets laboratory-derived strong weakening effects of talc observed in uniform mixtures, implying the governing mechanisms may be the shear localization effect of talc, which is enhanced by its natural platy shape or preimposed layered structure. Ensemble stability (a – b ) can be enhanced by increasing talc content in uniform talc-quartz mixtures. Reactivation-induced permeability increase is amplified with increased quartz content before the maturation of shear localization. Postmaturation permeability enhances on velocity upsteps and diminishes on velocity downsteps. Talc enhances compaction at velocity downsteps, potentially reducing fault permeability. Evolution trends of stability relating to the composition and structure of the fault gouge are straightforwardly obtained from the 3D simulation. Local friction evolution indicates that talc preferentially organizes and localizes in the shear zone, dominating the shear strength and frictional stability of faults

58 GEOSCIENCES↗
DOE OSTI2019

The Role of Mineral Composition on the Frictional and Stability Properties of Powdered Reservoir Rocks

The growing hazard of induced seismicity driven by the boom in unconventional resources exploitation is strongly linked to fault activation. We perform laboratory measurements on simulated fault gouges comprising powdered reservoir rocks from major oil and gas production sites in China, to probe the control of mineral composition on fault friction and stability responses during reservoir stimulation. Double direct shear experiments were conducted on gouges with phyllosilicate content ranging from 0 to 30 wt.% and grain sizes <150 μm, at constant normal stresses of 10–40 MPa and conditions of room temperature and water saturation. The velocity step and slide-hold-slide sequences were employed to evaluate frictional stability and static healing, respectively. Results indicate that the mineralogy of the gouges exhibit a strong control on the frictional strength, stability, and healing. Phyllosilicate-rich samples show lower frictional strength μ and higher values of (a – b ), promoting stable sliding. For the gouges studied, the frictional strength decreases monotonically with increasing phyllosilicate content, and a transition from velocity weakening to velocity strengthening behavior is evident at 15 wt.% phyllosilicates. Intermediate healing rates are common in gouges with higher content of phyllosilicates, with high healing rates predominantly in phyllosilicate-poor gouges. As an indispensable component in reservoir rocks, the carbonates are shown to affect both the frictional stability and healing response. These findings can have important implications for understanding the effects of mineralogy on fault behavior and induced seismic potential in geoengineering activities, particularly in reservoirs in China.

58 GEOSCIENCES↗
DOE OSTI2026

Soil Organic Matter Stabilization by Polyvalent Cations in a Buried Alkaline Soil

Buried paleosols can store large quantities of organic carbon (C), much of which persists for millennia due to isolation from surface processes that promote decomposition. Subsoil organic matter (SOM) persistence is often enhanced by mineral associations and ionic conditions—particularly high clay content and polyvalent cations—that limit microbial degradation and leaching. However, the vulnerability of these deep C stocks under erosion or environmental change remains poorly understood. This study investigates controls on SOM stabilization in the Brady paleosol and overlying modern soils across contrasting geomorphic settings in the Great Plains of Nebraska where Late Quaternary loess deposition and erosion created a sequence of buried and exposed paleosols. We sampled soils along burial and erosional toposequences and analyzed their physicochemical properties and radiocarbon‐based persistence of occluded particulate organic matter (oPOM) and mineral fractions (MF). Brady paleosol showed greater persistence (lower Fm) of oPOM and MF than modern soils, particularly under burial. This was linked to higher silt and clay content, elevated electrical conductivity, and increased exchangeable calcium and magnesium content, supporting roles for organo‐mineral interactions, flocculation, and carbonate cementation. In modern soils, SOM persistence and C content were more strongly tied to pH and cation exchange capacity. Erosional exposure reduced SOM stability and promoted geochemical convergence toward modern surface soils. These findings show that burial enhances SOM persistence via multiple stabilization mechanisms, while erosion increases subsoil C vulnerability. Our results underscore the importance of geomorphic and geochemical context in predicting soil C stability under environmental change.

Environmental sciences↗
DOE OSTI2017

Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion

Design of cost-effective electrocatalysts with enhanced stability and activity is of paramount importance for the next generation of energy conversion systems, including fuel cells and electrolyzers. However, electrocatalytic materials generally improve one of these properties at the expense of the other. Here, using Density Functional Theory calculations and electrochemical surface science measurements, we explore atomic-level features of ultrathin (hydroxy)oxide films on transition metal substrates and demonstrate that these films exhibit both excellent stability and activity for electrocatalytic applications. The films adopt structures with stabilities that significantly exceed bulk Pourbaix limits, including stoichiometries not found in bulk and properties that are tunable by controlling voltage, film composition, and substrate identity. Using nickel (hydroxy)oxide/Pt(111) as an example, we further show how the films enhance activity for hydrogen evolution through a bifunctional effect. Finally, the results suggest design principles for a new class of electrocatalysts with simultaneously enhanced stability and activity for energy conversion.

36 MATERIALS SCIENCE↗