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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Self–Healing and Stretchable Molecular Ferroelectrics with High Expandability

The interplay between crystal ordering and stretchability is frequently encountered in contemporary materials science, particularly in the case of ferroelectrics. The inherent dilemma arises when these materials need to withstand repetitive mechanical deformations or stretching without sacrificing their crystal integrity, all while retaining their remarkable ferroelectric properties and even exhibiting self-healing capabilities. This complexity further presents a significant challenge in the design and engineering of mechanically rigid molecular ferroelectric crystals, particularly for applications where both precise crystalline structure and mechanical adaptability are crucial. In this study, the humidity-controlled expansion and contraction, dissolution, and recrystallization of a self-assembled molecular ferroelectric-in-hydrogel framework are reported. Self-healing ferroelectric-in-hydrogel networks exhibit a recyclable humidity-tailored ionic conductivity from 2.86 × 10 –6 to 1.36 × 10 –5 S cm –1 , facilitating the stretchable piezoelectric sensing. Additionally, the dynamic bond reforming interactions are observed, leading to the tailoring of Young's modulus from 452 to 170 MPa, maintaining ferroelectricity under a strain of 20% with a piezoelectric coefficient of 15.7 pC N –1 . Upon lattice contraction, the molecular contacts undergo reforming, leading to the restoration of stretchable ferroelectrics/piezoelectrics and paving the way for stretchable bioelectronics for full-body motion monitoring. The capabilities highlighted here open avenues for stretchable and self-healing ferroelectric-in-hydrogel bioelectronic technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Achieving Stable Molybdenum Oxide Cathodes for Aqueous Zinc-Ion Batteries in Water-in-Salt Electrolyte

A layered MoO 3 material with large interlayer spacing represents a promising cathode for aqueous rechargeable Zn-ion batteries (ARZIBs), but the implementation of this material is limited due to the intrinsically low conductivity and poor structural stability. A 30 m ZnCl 2 water-in-salt electrolyte (WISE) was introduced to a MoO 3 nanobelt cathode for the first time, significantly increasing the stability of MoO 3 cathodes compared to those in 3 M ZnSO 4 and 3 M ZnCl2 electrolyte. The Zn/MoO 3 cell in WISE unambiguously demonstrated significantly improved rate performance delivering 349, 253, and 222 mAh/g at 100, 500, and 1000 mA/g, denoting a 2×, and 12× capacity increase of those achieved in 3 M electrolytes at 500 and 1000 mA/g, respectively. A capacity retention rate of 73% was achieved after (dis)charging at 100 mA/g for 100 cycles, and no obvious capacity fading was observed at higher current densities of 500 mA/g and 2A/g. A compilation of structural and morphological characterization was systematically performed to provide insight into the mechanisms of the improved performance in ZnCl 2 WISE for the MoO3 cathode materials. Specifically, our data collectively suggested that the drastic fading in 3M electrolytes can be attributed to the parasitic surface deposits on Zn originated from Mo dissolution and H 2 formation due to Zn corrosion and hydrogen evolution reaction (HER), which were significantly suppressed in the ZnCl 2 WISE. The direct visualization of these side reactions was achieved for the first time in the Zn-MoO 3 system, using an in situ optoelectrochemical measurement.

25 ENERGY STORAGE↗
DOE OSTI2020

Membrane-Free Zn/MnO 2 Flow Battery for Large-Scale Energy Storage

The traditional Zn/MnO 2 battery has attracted great interest due to its low cost, high safety, high output voltage, and environmental friendliness. However, it remains a big challenge to achieve long-term stability, mainly owing to the poor reversibility of the cathode reaction. Different from previous studies where the cathode redox reaction of MnO 2 /MnOOH is in solid state with limited reversibility, in this work a new aqueous rechargeable Zn/MnO 2 flow battery is constructed with dissolution–precipitation reactions in both cathodes (Mn 2+ /MnO 2 ) and anodes (Zn 2+ /Zn), which allow mixing of anolyte and catholyte into only one electrolyte and remove the requirement for an ion selective membrane for cost reduction. Impressively, this new battery exhibits a high discharge voltage of ≈1.78 V, good rate capability (10C discharge), and excellent cycling stability (1000 cycles without decay) at the areal capacity ranging from 0.5 to 2 mAh cm -2 . More importantly, this battery can be readily enlarged to a bench scale flow cell of 1.2 Ah with good capacity retention of 89.7% at the 500th cycle, displaying great potential for large-scale energy storage.

25 ENERGY STORAGE↗
DOE OSTI2024

A Green, Fire–Retarding Ether Solvent for Sustainable High–Voltage Li–Ion Batteries at Standard Salt Concentration

Lithium-ion batteries (LIBs) are increasingly encouraged to enhance their environmental friendliness and safety while maintaining optimal energy density and cost-effectiveness. Although various electrolytes using greener and safer glyme solvents have been reported, the low charge voltage (usually lower than 4.0 V vs Li/Li + ) restricts the energy density of LIBs. Herein, tetraglyme, a less-toxic, non-volatile, and non-flammable ether solvent, is exploited to build safer and greener LIBs. It is demonstrated that ether electrolytes, at a standard salt concentration (1 m), can be reversibly cycled to 4.5 V vs Li/Li + . Anchored with Boron-rich cathode-electrolyte interphase (CEI) and mitigated current collector corrosion, the LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode delivers competitive cyclability versus commercial carbonate electrolytes when charged to 4.5 V. Synchrotron spectroscopic and imaging analyses show that the tetraglyme electrolyte can sufficiently suppress the overcharge behavior associated with the high-voltage electrolyte decomposition, which is advantageous over previously reported glyme electrolytes. The new electrolyte also enables minimal transition metal dissolution and deposition. NMC811||hard carbon full cell delivers excellent cycling stability at C/3 with a high average Coulombic efficiency of 99.77%. In conclusion, this work reports an oxidation-resilient tetraglyme electrolyte with record-high 4.5 V stability and enlightens further applications of glyme solvents for sustainable LIBs by designing Boron-rich interphases.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Impacts of Dissolved Ni 2+ on the Solid Electrolyte Interphase on a Graphite Anode

Transition metal (e.g. Ni) ions dissolved from layered-structured Ni-rich cathodes can migrate to the anode side and accelerate the failure of lithium-ion batteries. The investigations of the impact and distribution of Ni species on the solid electrolyte interphase (SEI) on the anode are crucial to understand the failure mechanism. Herein, we used time-of-flight secondary ion mass spectroscopy (TOF-SIMS) coupled with multivariate curve resolution (MCR) analysis to intuitively characterize the distribution of Ni species in the SEI. We find that the SEI on the graphite electrode using an EC-based electrolyte exhibits a multi-stratum structure. During accelerated aging of the LiNi 0.88 Co 0.08 Mn 0.04 O 2 /graphite full cell, the dissolution of Ni aggravates significantly upon cycling. A strong correlation between the dissolved-Ni and organic species in the SEI on graphite is illustrated. Here, the ion-exchange reaction between Ni 2+ and Li + ions in the SEI is demonstrated to be the main reason for the increase of SEI resistivity.

25 ENERGY STORAGE↗
DOE OSTI2023

Electrolyte Engineering Stabilizes Photoanodes Decorated with Molecular Catalysts

Molecular catalysts are promising oxygen evolution promoters in conjunction with photoanodes for solar water splitting. Maintaining the stability of both photoabsorber and cocatalyst is still a prime challenge, with many efforts tackling this issue through sophisticated material designs. Such approaches often mask the importance of the electrode-electrolyte interface and overlook easily tunable system parameters, such as the electrolyte environment, to improve efficiency. We provide a systematic study on the activity-stability relationship of a prominent Fe 2 O 3 photoanode modified with Ir molecular catalysts using in situ mass spectroscopy. After gaining detailed insights into the dissolution behavior of the Ir cocatalyst, a comprehensive pH study is conducted to probe the impact of the electrolyte on the performance. An inverse trend in Fe and Ir stability is found, with the best activity-stability synergy obtained at pH 9.7. The results bring awareness to the overall photostability and electrolyte engineering when advancing catalysts for solar water splitting.

14 SOLAR ENERGY↗
DOE OSTI2022

Integration of Highly Luminescent Lead Halide Perovskite Nanocrystals on Transparent Lead Halide Nanowire Waveguides through Morphological Transformation and Spontaneous Growth in Water

The integration of highly luminescent CsPbBr 3 quantum dots on nanowire waveguides has enormous potential applications in nanophotonics, optical sensing and quantum communications. On the other hand, CsPb 2 Br 5 nanowires have also attracted a lot of attention due to their unique water stability and controversial luminescent property. Here we first report the growth of CsPbBr 3 nanocrystals on CsPb 2 Br 5 nanowires by simply immersing CsPbBr 3 powder into pure water, CsPbBr 3-γ X γ (X = Cl, I) nanocrystals on CsPb 2 Br 5-γ X γ nanowires are then synthesized for tunable light sources. Systematic structure and morphology studies, including in-situ monitoring, revealed that CsPbBr 3 powder was first converted to CsPb 2 Br 5 microplatelets in water, followed by a morphological transformation from CsPb 2 Br 5 microplatelets to nanowires, which is a kinetic dissolution-recrystallization process controlled by electrolytic dissociation and supersaturation of CsPb 2 Br 5 . CsPbB r3 nanocrystals are spontaneously formed on CsPb 2 Br 5 nanowires when nanowires are collected from the aqueous solution. Raman spectroscopy, combined photoluminescence and SEM imaging confirm that the bright emission originates from CsPbBr 3-γ X γ nanocrystals while CsPb 2 Br 5-γ X γ nanowires are transparent waveguides. In conclusion, the intimate integration of nanoscale light sources with a nanowire waveguide is demonstrated through the observation of the wave guiding of light from nanocrystals and Fabry-Perot interference modes of the nanowire cavity.

42 ENGINEERING↗
DOE OSTI2022

Assessing Long-Term Cycling Stability of Single-Crystal Versus Polycrystalline Nickel-Rich NCM in Pouch Cells with 6 mAh cm -2 Electrodes

Lithium-ion batteries based on single-crystal LiNi1-x-yCoxMnyO2 (NCM, 1-x-y ≥ 0.6) cathode materials are gaining increasing attention due to their improved structural stability resulting in superior cycle life compared to batteries based on polycrystalline NCM. However, an in-depth understanding of the less pronounced degradation mechanism of single-crystal NCM is still lacking. Here, a detailed postmortem study is presented, comparing pouch cells with single-crystal versus polycrystalline LiNi 0.60 Co 0.20 Mn 0.20 O 2 (NCM622) cathodes after 1375 dis-/charge cycles against graphite anodes. The thickness of the cation-disordered layer forming in the near-surface region of the cathode particles does not differ significantly between single-crystal and polycrystalline particles, while cracking is pronounced for polycrystalline particles, but practically absent for single-crystal particles. Transition metal dissolution as quantified by time-of-flight mass spectrometry on the surface of the cycled graphite anode is much reduced for single-crystal NCM622. Similarly, CO 2 gas evolution during the first two cycles as quantified by electrochemical mass spectrometry is much reduced for single-crystal NCM622. Benefitting from these advantages, graphite/single-crystal NMC622 pouch cells are demonstrated with a cathode areal capacity of 6 mAh cm -2 with an excellent capacity retention of 83% after 3000 cycles to 4.2 V, emphasizing the potential of single-crystalline NCM622 as cathode material for next-generation lithium-ion batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optimizing Hybrid-Phase IrO2 Catalysts with Ti for Enhanced Oxygen Evolution Reaction for Proton Exchange Membrane Water Electrolysis

To realize a sustainable energy transition, water electrolysis-particularly proton exchange membrane water electrolysis (PEMWE)-holds significant promise. However, practical deployment is hindered by the cost and instability of the anode catalyst, IrO2. Recent studies indicate that tuning the Ir-O bond distance, via doping or composite formation, is key to enhancing the oxygen evolution reaction (OER) performance of IrO2-based electrocatalysts. Herein, a hybrid-phase Ti-incorporated IrO2 electrocatalyst is developed, exhibiting outstanding OER activity (298.8 mV at 100 mA cm-2) and stability over 25 h. This improvement originates from asymmetric interatomic interactions introduced by Ti, as revealed by combined experimental X-ray analyses and theoretical modeling. Ti incorporation induces tensile strain along the z-axis in IrO2 motifs, effectively reducing the average Ir-O bond distance and thereby enhancing OER activity. In situ X-ray absorption spectroscopy further confirms that at 1.5 V (vs. RHE), the elongated Ir-O bond facilitates -OOH* intermediate formation while suppressing Ir dissolution, contributing to superior stability. These findings underscore the critical role of Ir-O bond engineering in balancing activity and durability, offering strategic insights for the rational design of high-performance OER catalysts for renewable energy technologies.

08 HYDROGEN↗
DOE OSTI2017

Stratigraphic and structural controls on groundwater flow in an outcropping fossil fan delta: the case of Sant Llorenç del Munt range (NE Spain)

Hydrogeological models of mountain regions present the opportunity to understand the role of geological factors on groundwater resources. The effects of sedimentary facies and fracture distribution on groundwater flow and resource exploitation studied in the ancient fan delta of Sant Llorenç de Munt (central Catalonia, Spain) by integrating geological field observations (using sequence stratigraphy methods) and hydrogeological data (pumping tests, hydrochemistry and environmental isotopes). A comprehensive analysis of data portrays the massif as a single unit, constituted by different compartments determined by specific layers and sets of fractures. Two distinct flow systems—local and regional—are identified based on pumping test analysis as well as hydrochemical and isotopic data. Drawdown curves derived from pumping tests indicate that the behavior of the saturated layers, whose main porosity is given by the fracture network, corresponds to a confined aquifer. Pumping tests also reflect a double porosity within the system and the occurrence of impervious boundaries that support a compartmentalized model for the whole aquifer system. Hydrochemical data and associated spatial evolution show the result of water–rock interaction along the flow lines. Concentration of magnesium, derived from dolomite dissolution, is a tracer of the flow-path along distinct stratigraphic units. Water stable isotopes indicate that evaporation (near a 5% loss) occurs in a thick unsaturated zone within the massif before infiltration reaches the water table. The hydrogeological analysis of this outcropping system provides a methodology for the conceptualization of groundwater flow in similar buried systems where logging and hydrogeological information are scarce.

58 GEOSCIENCES↗
DOE OSTI2018

Fingerprinting groundwater salinity sources in the Gulf Coast Aquifer System, USA

Understanding groundwater salinity sources in the Gulf Coast Aquifer System (GCAS) is a critical issue due to depletion of fresh groundwater and concerns for potential seawater intrusion. The study objective was to assess sources of groundwater salinity in the GCAS using ∼1,400 chemical analyses and ∼90 isotopic analyses along nine well transects in the Texas Gulf Coast, USA. Salinity increases from northeast (median total dissolved solids (TDS) 340 mg/L) to southwest (median TDS 1,160 mg/L), which inversely correlates with the precipitation distribution pattern (1,370– 600 mm/yr, respectively). Molar Cl/Br ratios (median 540–600), depleted δ{sup 2}H and δ{sup 18}O (−24.7‰, −4.5‰) relative to seawater (Cl/Br ∼655 and δ{sup 2}H, δ{sup 18}O 0‰, 0‰, respectively), and elevated {sup 36}Cl/Cl ratios (∼100), suggest precipitation enriched with marine aerosols as the dominant salinity source. Mass balance estimates suggest that marine aerosols could adequately explain salt loading over the large expanse of the GCAS. Evapotranspiration enrichment to the southwest is supported by elevated chloride concentrations in soil profiles and higher δ{sup 18}O. Secondary salinity sources include dissolution of salt domes or upwelling brines from geopressured zones along growth faults, mainly near the coast in the northeast. The regional extent and large quantities of brackish water have the potential to support moderate-sized desalination plants in this location. These results have important implications for groundwater management, suggesting a current lack of regional seawater intrusion and a suitable source of relatively low TDS water for desalination.

58 GEOSCIENCES↗
DOE OSTI2017

Hydrochemical and isotopic characteristics of groundwater in the northeastern Tennger Desert, northern China

Groundwater is typically the only water source in arid regions, and its circulation processes should be better understood for rational resource exploitation. Stable isotopes and major ions were investigated in the northeastern Tengger Desert, northern China, to gain insights into groundwater recharge and evolution. In the northern mountains, Quaternary unconsolidated sediments, exposed only in valleys between hills, form the main aquifer, which is mainly made of aeolian sand and gravel. Most of the mountain groundwater samples plot along the local meteoric water line (LMWL), with a more depleted signature compared to summer precipitation, suggesting that mountain groundwater was recharged by local precipitation during winter. Most of the groundwater was fresh, with total dissolved solids less than 1 g/L; dominant ions are Na{sup +}, SO{sub 4}{sup 2−} and Cl{sup −}, and all mineral saturation indices are less than zero. Evaporation, dissolution and cation exchange are the major hydrogeochemical processes. In the southern plains, however, the main aquifers are sandstone. The linear regression line of δD and δ{sup 18}O of groundwater parallels the LMWL but the intercept is lower, indicating that groundwater in the plains has been recharged by ancient precipitation rather than modern. Both calcite and dolomite phases in the plains groundwater are close to saturation, while gypsum and halite can still be dissolved into the groundwater. Different recharge mechanisms occur in the northern mountains and the southern plains, and the hydraulic connection between them is weak. Because of the limited recharge, groundwater exploitation should be limited as much as possible.

58 GEOSCIENCES↗
DOE OSTI2018

Groundwater mixing and mineralization processes in a mountain–oasis–desert basin, northwest China: hydrogeochemistry and environmental tracer indicators

Hydrogeochemistry and environmental tracers ({sup 2}H, {sup 18}O, {sup 87}Sr/{sup 86}Sr) in precipitation, river and reservoir water, and groundwater have been used to determine groundwater recharge sources, and to identify mixing characteristics and mineralization processes in the Manas River Basin (MRB), which is a typical mountain–oasis–desert ecosystem in arid northwest China. The oasis component is artificial (irrigation). Groundwater with enriched stable isotope content originates from local precipitation and surface-water leakage in the piedmont alluvial–oasis plain. Groundwater with more depleted isotopes in the north oasis plain and desert is recharged by lateral flow from the adjacent mountains, for which recharge is associated with high altitude and/or paleo-water infiltrating during a period of much colder climate. Little evaporation and isotope exchange between groundwater and rock and soil minerals occurred in the mountain, piedmont and oasis plain. Groundwater δ{sup 2}H and δ{sup 18}O values show more homogeneous values along the groundwater flow direction and with well depths, indicating inter-aquifer mixing processes. A regional contrast of groundwater allows the {sup 87}Sr/{sup 86}Sr ratios and δ{sup 18}O values to be useful in a combination with Cl, Na, Mg, Ca and Sr concentrations to distinguish the groundwater mixing characteristics. Two main processes are identified: groundwater lateral-flow mixing and river leakage in the piedmont alluvial–oasis plain, and vertical mixing in the north oasis plain and the desert. The {sup 87}Sr/{sup 86}Sr ratios and selected ion ratios reveal that carbonate dissolution and mixing with silicate from the southern mountain area are primarily controlling the strontium isotope hydrogeochemistry.

58 GEOSCIENCES↗
DOE OSTI2018

Characterization of a fluvial aquifer at a range of depths and scales: the Triassic St Bees Sandstone Formation, Cumbria, UK

Fluvial sedimentary successions represent porous media that host groundwater and geothermal resources. Additionally, they overlie crystalline rocks hosting nuclear waste repositories in rift settings. The permeability characteristics of an arenaceous fluvial succession, the Triassic St Bees Sandstone Formation in England (UK), are described, from core-plug to well-test scale up to ~1 km depth. Within such lithified successions, dissolution associated with the circulation of meteoric water results in increased permeability (K~10{sup −1}–10{sup 0} m/day) to depths of at least 150 m below ground level (BGL) in aquifer systems that are subject to rapid groundwater circulation. Thus, contaminant transport is likely to occur at relatively high rates. In a deeper investigation (> 150 m depth), where the aquifer has not been subjected to rapid groundwater circulation, well-test-scale hydraulic conductivity is lower, decreasing from K~10{sup −2} m/day at 150–400 m BGL to 10{sup −3} m/day down-dip at ~1 km BGL, where the pore fluid is hypersaline. Here, pore-scale permeability becomes progressively dominant with increasing lithostatic load. Notably, this work investigates a sandstone aquifer of fluvial origin at investigation depths consistent with highly enthalpy geothermal reservoirs (~0.7–1.1 km). At such depths, intergranular flow dominates in unfaulted areas with only minor contribution by bedding plane fractures. However, extensional faults represent preferential flow pathways, due to presence of high connective open fractures. Therefore, such faults may (1) drive nuclear waste contaminants towards the highly permeable shallow (< 150 m BGL) zone of the aquifer, and (2) influence fluid recovery in geothermal fields.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Hydrogeological and hydrochemical investigation of groundwater using environmental isotopes ({sup 18}O, {sup 2}H, {sup 3}H, {sup 14}C) and chemical tracers: a case study of the intermediate aquifer, Sfax, southeastern Tunisia

Major element concentrations and stable (δ{sup 18}O and δ{sup 2}H) and radiogenic ({sup 3}H and {sup 14}C) isotopes in groundwater have proved useful tracers for understanding the geochemical processes that control groundwater mineralization and for identifying recharge sources in the semi-arid region of Sfax (southeastern Tunisia). Major-ion chemical data indicate that the origins of the salinity in the groundwater are the water–rock interactions, mainly the dissolution of evaporitic minerals, as well as the cation exchange with clay minerals. The δ{sup 18}O and δ{sup 2}H relationships suggest variations in groundwater recharge mechanisms. Strong evaporation during recharge with limited rapid water infiltration is evident in the groundwater of the intermediate aquifer. The mixing with old groundwater in some areas explains the low stable isotope values of some groundwater samples. Groundwaters from the intermediate aquifer are classified into two main water types: Ca-Na-SO{sub 4} and Ca-Na-Cl-SO{sub 4}. The high nitrate concentrations suggest an anthropogenic source of nitrogen contamination caused by intensive agricultural activities in the area. The stable isotopic signatures reveal three water groups: non-evaporated waters that indicate recharge by recent infiltrated water; evaporated waters that are characterized by relatively enriched δ{sup 18}O and δ{sup 2}H contents; and mixed groundwater (old/recent) or ancient groundwater, characterized by their depleted isotopic composition. Tritium data support the existence of recent limited recharge; however, other low tritium values are indicative of pre-nuclear recharge and/or mixing between pre-nuclear and contemporaneous recharge. The carbon-14 activities indicate that the groundwaters were mostly recharged under different climatic conditions during the cooler periods of the late Pleistocene and Holocene.

58 GEOSCIENCES↗
DOE OSTI2018

The integrated impacts of natural processes and human activities on groundwater salinization in the coastal aquifers of Beihai, southern China

Salinization in coastal aquifers is usually related to both seawater intrusion and water–rock interaction. The results of chemical and isotopic methods were combined to identify the origin and processes of groundwater salinization in Daguansha area of Beihai, southern China. The concentrations of the major ions that dominate in seawater (Cl{sup −}, Na{sup +}, Ca{sup 2+}, Mg{sup 2+} and SO{sub 4}{sup 2–}), as well as the isotopic content and ratios ({sup 2}H, {sup 18}O, {sup 87}Sr/{sup 86}Sr and {sup 13}C), suggest that the salinization occurring in the aquifer of the coastal plain is related to seawater and that the prevailing hydrochemical processes are evaporation, mixing, dissolution and ion exchange. For the unconfined aquifer, groundwater salinization has occurred in an area that is significantly influenced by land-based sea farming. The integrated impacts of seawater intrusion from the Beibuwan Gulf and infiltration of seawater from the culture ponds are identified in the shallowest confined aquifer (I) in the middle of the area (site BBW2). Leakage from this polluted confined aquifer causes the salinization of groundwater in the underlying confined aquifer (II). At the coastal monitoring site (BBW3), confined aquifer I and lower confined aquifer II are heavily contaminated by seawater intrusion. The weak connectivity between the upper aquifers, and the seaward movement of freshwater, prevents saltwater from encroaching the deepest confined aquifer (III). A conceptual model is presented. Above all, understanding of the origin and processes of groundwater salinization will provide essential information for the planning and sustainable management of groundwater resources in this region.

58 GEOSCIENCES↗
DOE OSTI2017

Association with pedogenic iron and aluminum: effects on soil organic carbon storage and stability in four temperate forest soils

Soil organic carbon (SOC) can be stabilized via association with iron (Fe) and aluminum (Al) minerals. Fe and Al can be strong predictors of SOC storage and turnover in soils with relatively high extractable metals content and moderately acidic to circumneutral pH. Here we test whether pedogenic Fe and Al influence SOC content and turnover in soils with low Fe and Al content and acidic pH. In soils from four sites spanning three soil orders, we quantified the amount of Fe and Al in operationally-defined poorly crystalline and organically-complexed phases using selective chemical dissolution applied to the soil fraction containing mineral-associated carbon. We evaluated the correlations of Fe and Al concentrations, mean annual precipitation (MAP), mean annual temperature (MAT), and pH with SOC content and 14C-based turnover times. We found that poorly crystalline Fe and Al content predicted SOC turnover times (p < 0.0001) consistent with findings of previous studies, while organically-complexed Fe and Al content was a better predictor of SOC concentration (p < 0.0001). Greater site-level MAP (p < 0.0001) and colder site-level MAT (p < 0.0001) were correlated with longer SOC turnover times but were not correlated with SOC content. Our results suggest that poorly crystalline Fe and Al effectively slow the turnover of SOC in these acidic soils, even when their combined content in the soil is less than 2% by mass. However, in the strongly acidic Spodosol, organo-metal complexes tended to be less stable resulting in a more actively cycling mineral-associated SOC pool.

14C↗
DOE OSTI2018

Nanosized low-temperature phases of titanium(IV) oxide with anatase and η-phase structures: composition, structure, and photocatalytic properties

Nanosized low-temperature modifications of titanium(IV) oxide with the anatase and η-phase (TiO{sub 2–x}•mH{sub 2}O) structures were prepared by the sulfate method (pH <3) and for the first time characterized by a complex of methods (X-ray diffractometry, scanning electron microscopy, IR spectroscopy, Raman spectroscopy, differential scanning calorimetry, low-temperature sorption capacity of samples to nitrogen, and differentiating dissolution). The physicochemical properties of the modifications were compared. Differences in compositions of the surface and volumes of the samples, compositions and structures of the phases (structure of η-phase is superstructure to anatase), and microstructure elements (sizes of crystallites, nanoparticles, and specific surface area; volume of nano- and ultrananopores) were revealed. The region of η-phase stability was found in the coordinates of temperature (T = 50–95 °C) and hydrolysis duration (τ = 10–80 min) and temperature (T≤200 °C) and annealing duration (τ <6 h). The distinctions in the thermal behavior of the nanosized anatase and η-phase were studied. The photocatalytic activity (PCA) is determined by the physicochemical characteristics of the samples and phases and also by the composition and structure of the decomposed substrate. In the case of difenoxazole, the PCA is affected by the compositions of the samples, phases, and surface (the presence of OH groups) and specific surface area, whereas the composition of the samples and specific surface area affect the PCA in the case of thiamethoxam.

77 NANOSCIENCE AND NANOTECHNOLOGY↗