THE EFFECT OF CO SUB 2 ON PH IN CULTURE MEDIA FOR ALGAE
Effect of carbon dioxide on ph of algal culture media
ALGAE↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Carbon dioxide measuring systems for manned spacecraft.
Radiation absorption, infrared and ph in flight carbon dioxide measuring systems for manned spacecraft
MANNED SPACECRAFT↗
Van Slyke's buffer values for cell secretions.
Buffering capacity of substances liberated by Chlorella expressed in terms of van Slyke buffer index, noting changes in pH
BIOLOGICAL CELL↗
Properties of the induced acid phosphatase and of the constitutive acid phosphatase of Euglena.
Enzymatic activity and inhibition, thermal stability and electrophoretic properties of induced and constitutive acid phosphatases of Euglena gracilis
BACTERIA↗
Normal man and chronic hypercapnia - Metabolic aspects.
Chronic hypercapnia effects on pH level, Ca and P metabolism and electrolyte metabolism in normal sedentary man
HYPERCAPNIA↗
Application of selected methods of remote sensing for detecting carbonaceous water pollution
The use of aerial photography to determine the nature and extent of water pollution from carbonaceous materials is discussed. Flights were conducted over the Galveston Bay estuarine complex. Ground truth data were developed from field sampling of the waters in a region near the Houston Ship Channel. Tests conducted in the field were those for the following physical and chemical factors: (1) ph, (2) dissolved oxygen, (3) temperature, and (4) light penetration. Laboratory analyses to determine various properties of the water are described and the types of instruments used are identified. Results of the analyses are presented as charts and graphs.
Davis, E. M.↗
Olivine Dissolution and Formation of Secondary phases in Ultramafic Soils
Introduction: Olivine has been proposed as an indicator for the duration of water-rock interaction within Martian rocks and sediments [1-3]. The use of olivine as a mineralogical indicator for past aqueous alteration on Mars requires interpretation of a complex combination of factors including pH, temperature, and composition [5,6]. Here, we examine the persistence of natural olivine within terrestrial ultramafic soils (Fe/Mg-rich, Al-poor) developing under different climatic conditions and the incipient dissolution of emplaced forsterite (Fo) and fayalite (Fa) surfaces to investigate environmental effects on incipient olivine dissolution, olivine persistence in soils, and formation of secondary phases. Methods: Field Sites. We examined olivine weathering and secondary material formation in ultramafic soils at 6 sites in the Klamath Mountains (KM) of northern California with a mean annual temperature of ~12.8℃ and precipitation of ~55.7-95.4 cm/year [7], and soil pH of ~6.5-7.3; 4 sites in the Tablelands (TB) of Newfoundland, Canada with a mean annual temperature of <3.9℃ and precipitation of ~120.0 cm/year [8], and soil pH of ~7.7; and at 3 sites at Pickhandle Gulch (PG), Nevada with a mean annual temperature of ~14.4℃ and precipitation of ~14.1 cm/year [7], and soil pH of ~8.5. Sampling sites span an age range of ~12.1-50+ kya in the Klamath Mountains [9,10] and ~13-30 kya in the Tablelands [11]. Pickhandle Gulch sites are undated. Parent Material and Soil Analyses. Polished thin sections of bulk soil prepared by Wagner Petrographic, Inc were carbon-coated and analyzed on a JEOL 2100 SEM in back-scattered electron mode in the EMIL lab at UNLV and at the 13-ID-E synchrotron beamline at Argonne National Laboratory using µXRF, µXRD, and XAS. Soil and parent material samples were powdered in a Fritsch pulverisette and analyzed by XRD and soil by VNIR. Soil preparation is further described in [12]. Disk Preparation, Burial, and Collection. Fo disks were cut from a column prepared via hot-pressing and Fa disks by sintering synthetic fayalite powder, see [13] for detail. Disks were polished to a 0.25-micron level with diamond grit. Disks were buried in 3 KM soils, 4 TB soils, and 3 PG soils, collected after exactly 365 days, and washed gently with 100% reagent grade ethanol to remove potential adhered soil material. Weathered disks and soil samples were stored in a -20℃ freezer until analysis. Unaltered control disks prepared identically to the buried disks were stored at -20℃ for the duration of the experiment. Disk Analyses. One Fo and Fa disk from each climate zone was analyzed on a variable pressure Zeiss Supra 40VP SEM at Northern Arizona University. A separate Fo and Fa disk from each climate zone was analyzed by XPS using a Physical Electronics VersaProbe II at the Penn State Univ. Materials Characterization Lab after a Na-dodecyl sulfate wash and ozonation to remove carbon contamination as in [14]. VNIR measurements were conducted at Johnson Space Center using an ASD FieldSpec3 under ambient lab conditions on a separate Fo and Fa disk from each climate zone. One separate Fo and Fa control sample was analyzed for each technique for comparison with weathered samples. XPS uncertainty was determined from 5 repeat measurements on controls. Results: Bedrock and Soil Results Olivine is present in the parent material in the KM and TB. Olivine is found in ~12.1 ka KM soils but is absent from all older soils, while persisting into the oldest (>20 ka) TB soil (Figure 1). In both locations, olivine is found as cores surrounded by a serpentine rind (Figure 2). VNIR spectra from the analyzed soils possess strong OH-associated spectral features at ~2.33 µm indicating the presence of Mg-rich phyllosilicates as well as ferric-oxide features at ~0.92 µm in the KM (Figure 3). Primary crystalline silicate grains mostly incorporate Fe2+, while poorly crystalline weathering rinds are best fit by ferric oxide XAS standards (Figure 4). µXRF also shows that Fe and Ni concentrate in weathering rinds and Cr remains within interior silicate grains (Figure 4). Buried Sample Results All Fo surfaces exhibited formation of dissolution features including shallow pitting not observed on controls. Dissolution features were most visually widespread on the KM disk (Figure 5). Leaching of Mg from KM and TB Fo disks was evident from <1.6 Mg/Si ratios measured by XPS (Figure 6). Fe-rich precipitates in SEM (Figure 5) and Fe presence in XPS scans (Figure 6) indicate Fe deposition onto KM and TB Fo disk surfaces. The appearance of a spectral feature at 0.55 µm in the VNIR spectra from the TB Fo suggests this Fe is ferric (Figure 7). The PG Fo appears least altered, with minimal formation of dissolution features in SEM (Figure 5), a Mg/Si ratio inconsistent with leaching (~2) (Figure 6), and VNIR spectra almost identical to the control sample. Analysis of Fa surfaces is ongoing. The higher temperatures and more acidic pH in the KM soils likely drive the faster dissolution of the Fo disks described above. While the TB soils experience greater precipitation than in the KM, the cooler temperatures and more basic soil pH facilitate observable but more limited alteration. The dry climate and basic soil pH at PG lead to minimal dissolution of the PG disk surfaces.
A D Feldman↗
Leaching characteristics of calcium-based compounds in MSWI Residues: From the viewpoint of clogging risk
Highlights: • The leaching behavior of Ca-based compounds commonly in MSWI residues was studied. • pH is the crucial factor for calcium leaching process. • CaCO{sub 3} was the most sensitive to leaching temperature and Ca{sub 3}(PO{sub 4}){sub 2} was the least. • Ca leaching of MSWIBA and SAPCR attributed to CaCO{sub 3} and Ca{sub 3}(PO{sub 4}){sub 2} respectively. • Potential clogging ability of MSWI residues leachate in open air was calculated. - Abstract: Leachate collection system (LCS) clogging caused by calcium precipitation would be disadvantageous to landfill stability and operation. Meanwhile, calcium-based compounds are the main constituents in both municipal solid waste incineration bottom ash (MSWIBA) and stabilized air pollution control residues (SAPCR), which would increase the risk of LCS clogging once these calcium-rich residues were disposed in landfills. The leaching behaviors of calcium from the four compounds and municipal solid waste incineration (MSWI) residues were studied, and the influencing factors on leaching were discussed. The results showed that pH was the crucial factor in the calcium leaching process. CaCO{sub 3} and CaSiO{sub 3} began leaching when the leachate pH decreased to less than 7 and 10, respectively, while Ca{sub 3}(PO{sub 4}){sub 2} leached at pH < 12. CaSO{sub 4} could hardly dissolve in the experimental conditions. Moreover, the sequence of the leaching rate for the different calcium-based compounds is as follows: CaSiO{sub 3} > Ca{sub 3}(PO{sub 4}){sub 2} > CaCO{sub 3}. The calcium leaching from the MSWIBA and SAPCR separately started from pH < 7 and pH < 12, resulting from CaCO{sub 3} and Ca{sub 3}(PO{sub 4}){sub 2} leaching respectively, which was proven by the X-ray diffraction results. Based on the leaching characteristics of the different calcium compounds and the mineral phase of calcium in the incineration residues, simulated computation of their clogging potential was conducted, providing the theoretical basis for the risk assessment pertaining to LCS clogging in landfills.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Unearthing principal strengthening factors tuning the additive manufactured 15-5 PH stainless steel
Additive manufactured (AM) materials exhibit enhanced performance, while post-processing is essential to reinforce its properties. Controlling the tunable factors and the underlying strengthening mechanisms during the post-processing are a key to answering the calls from the industry and end users. We identified the principal strengthening factors that contribute to AM stainless steel under heat-treatment and weighed their importance. The as-built sample exhibited a unique microstructure with a heterogeneous grain size distribution, a small amount of retained austenite, high dislocation density, and dispersed oxide particles. The strengthening primarily by dislocation forest and additionally by heterogeneous grain size contributed to the as-built sample. Although aging slightly decreased dislocation strengthening, superior aging enhancement was achieved by Cu-precipitates. The solid-solutionizing not only increased the effective grain size but also reduced the dislocation density by eliminating the heterogeneous microstructure, which deteriorated the precipitation hardenability. Our findings shed light on the performance optimization of AM metals.
36 MATERIALS SCIENCE↗
Organic-to-Aqueous Phase Transfer of Cadmium Chalcogenide Quantum Dots Using a Sulfur-Free Ligand for Enhanced Photoluminescence and Oxidative Stability
This article describes a procedure for transferring colloidal CdS and CdSe quantum dots (QDs) from organic solvents to water by exchanging their native hydrophobic ligands for phosphonopropionic acid (PPA) ligands, which bind to the QD surface through the phosphonate group. This method, which uses dimethylformamide as an intermediate transfer solvent, was developed in order to produce high-quality water soluble QDs with neither a sulfur-containing ligand nor a polymer encapsulation layer, both of which have disadvantages in applications of QDs to photocatalysis and biological imaging. CdS (CdSe) QDs were transferred to water with a 43% (48%) yield using PPA. The photoluminescence (PL) quantum yield for PPA-capped CdSe QDs is larger than that for QDs capped with the analogous sulfur-containing ligand, mercaptopropionic acid (MPA), by a factor of four at pH 7, and by up to a factor of 100 under basic conditions. The MPA ligands within MPA-capped QDs oxidize at E ox ~ +1.7 V vs. SCE, whereas cyclic voltammograms of PPA-capped QDs show no discerible oxidation peaks at applied potentials up to +2.5 V vs. SCE. The PPA-capped QDs are chemically and colloidally stable for at least five days in the dark, even in the presence of O 2 , and are stable when continuously illuminated for five days, when oxygen is excluded and a sacrificial reductant is present to capture photogenerated holes.
36 MATERIALS SCIENCE↗
Building a genome-based understanding of bacterial pH preferences
The environmental preferences of many microbes remain undetermined. This is the case for bacterial pH preferences, which can be difficult to predict a priori despite the importance of pH as a factor structuring bacterial communities in many systems. We compiled data on bacterial distributions from five datasets spanning pH gradients in soil and freshwater systems (1470 samples), quantified the pH preferences of bacterial taxa across these datasets, and compiled genomic data from representative bacterial taxa. While taxonomic and phylogenetic information were generally poor predictors of bacterial pH preferences, we identified genes consistently associated with pH preference across environments. We then developed and validated a machine learning model to estimate bacterial pH preferences from genomic information alone, a model that could aid in the selection of microbial inoculants, improve species distribution models, or help design effective cultivation strategies. More generally, we demonstrate the value of combining biogeographic and genomic data to infer and predict the environmental preferences of diverse bacterial taxa.
59 BASIC BIOLOGICAL SCIENCES↗
Development of a CO 2 Chemical Sensor for Downhole CO 2 Monitoring in Carbon Sequestration
Geologic storage of carbon dioxide (CO 2 ) has been proposed as a viable means for reducing anthropogenic CO 2 emissions. The means for geological sequestration of CO 2 is injection of supercritical CO 2 underground, which requires the CO 2 to remain either supercritical, or in solution in the water/brine present in the underground formation. However, there are aspects of geologic sequestration that need further study, particularly in regards to safety. To date, none of the geologic sequestration locations have been tested for storage integrity under the changing stress conditions that apply to the sequestration of very large amounts of CO 2 . Establishing environmental safety and addressing public concerns require widespread monitoring of the process in the deep subsurface. In addition, studies of subsurface carbon sequestration such as flow simulations, models of underground reactions and transports require a comprehensive monitoring process to accurately characterize and understand the storage process. Real-time information about underground CO 2 movement and concentration change is highly helpful for: (1) better understanding the uncertainties present in CO 2 geologic storage; (2) improvement of simulation models; and (3) evaluation of the feasibility of geologic CO 2 storage. Current methods to monitor underground CO 2 storage include seismic, geoelectric, isotope and tracer methods, and fluid sampling analysis. However, these methods commonly resulted low resolution, high cost, and the inability to monitor continuously over the long time scales of the CO 2 storage process. A preferred way of monitoring in-situ underground CO 2 migration is to continuous measure CO 2 concentration change in brine during the carbon storage process. An approach to obtain the real time information on CO 2 concentration change in formation solution is highly demanded in carbon storage to understand the CO 2 migration subsurface and to answer the public safety problem. The objective of the study is to develop a downhole CO 2 sensor that can in-situ, continuously monitor CO 2 concentration change in deep saline. The sensor is a Severinghaus-type CO 2 sensor with small size, which renders it can be embedded in monitoring well casing or integrated with pressure/temperature transducers, enabling the development of “smart” wells. The studies included: (1) prepare and characterize metal-oxide electrodes. Test the electrodes response to pH change. Investigate different ions and brine concentration effects on the electrode’s performance. Study the stability of the electrode in brine solution; (2) fabricate a downhole CO 2 sensor with the metal-oxide electrodes prepared in the laboratory. Test the performance of the CO 2 sensor in brine solutions. Study high pressure effects on the performance of the sensor; (3) design and conduct CO 2 /brine coreflooding experiments with the CO2 sensor. Monitor CO 2 movement along the core and test the performance of the sensor in coreflooding tests. Develop a data acquisition system that can digitize the sensor’s output voltage. Our completed research has resulted in deep understanding of downhole CO 2 sensor development and CO 2 monitoring in CO 2 storage process. The developed downhole CO 2 sensor included a metal-oxide electrode, a gas-permeable membrane, a porous steel cup, and a bicarbonate-based internal electrolyte solution. Iridium oxide-based electrode was prepared and used for preparation the CO 2 sensor. The prepared iridium oxide-based electrode displayed a linearly response to pH change. Different factors such as different ions and ions concentration, temperature, and pressure effects on the electrode performance on pH response were investigated. The results indicated that the electrode exhibited a good performance even in high salt concentration of produced water. To improve the electrode performance under high pressure, IrO 2 nanoparticles with the particle size in the range of 1-2 nm were prepared and electrodeposited on stainless steel substrate by cyclic voltammetry. It was observed that the thin film of iridium oxide was formed on the substrate surface and such iridium oxide-based electrode displayed excellent performance under high pressure for longer term. A downhole CO 2 sensor with the iridium oxide-based electrode was prepared. The working principle of the CO 2 sensor is based on the measurement of the pH change of the internal electrolyte solution caused by the hydrolysis of CO 2 and then determination of the CO 2 concentration in water. The prepared downhole CO 2 sensor had the size of diameter of 0.7 in. and length of 1.5 in. The sensor was tested under the pressures of 500 psi, 2,000 psi, and 3,000 psi. A linear correlation was observed between the sensor potential change and dissolved CO 2 concentration in water. The response time of the CO 2 sensor was in the range of 60-100 minutes. Further tests indicated that the CO 2 sensor exhibited good reproducibility under high pressure. A CO 2 /brine coreflooding system was constructed to simulate the real-world CO 2 storage process. The prepared downhole CO 2 sensor was loaded in the system to monitor CO 2 movement during CO 2 /brine coreflooding test. The results indicated that the sensor could detect CO 2 movement in the tests. Further studies showed that the sensor could be recovered by brine flooding after CO 2 /brine flushed the core. The results of the coreflooding tests demonstrated that the sensor had potential application for CO 2 monitoring in carbon sequestration. A data acquisition system for the downhoe CO 2 sensor was developed and coded. The system converted the sensor output signal into digital data and transported the data from downhole to wellhead surface. The data acquisition system was tested and evaluated in the laboratory with the prepared sensor for data collection.
36 MATERIALS SCIENCE↗
Reassessment of caustic scrubbing for radioiodine capture during UNF processing
The effective removal of iodine-129 from gaseous emissions during used nuclear fuel processing is critical for minimizing environmental contamination and ensuring environmental regulatory compliance. Recent research has focused on optimizing process air, scrubber conditions, and integrating complementary techniques, such as solid sorbents as a polishing step, to improve iodine capture efficiency. The efficiency of a caustic scrubber is influenced by several factors, such as pH, temperature, gas–liquid contact time, and the presence of oxidants, yet the existing literature tends not to consider how these factors might interact or change in importance with process scaling. This perspective advocates for reconsidering how to mitigate many of these factors, especially in view of the transition from laboratory bench to pilot scale and beyond. This paper reviews the principles, operational parameters, and advancements in caustic aqueous scrubbing for radioiodine mitigation, aims to direct the next scientific pursuit of this technology, and inform environmental decision-making.
Ngelale, Randy [Oak Ridge National Laboratory (ORN↗
Highly Rectifying Fluidic Diodes Based on Asymmetric Layer-by-Layer Nanofilms on Nanochannel Membranes
Nanochannel-based fluidic diodes display ion selectivity and ion-current rectification (ICR), which may prove important in energy harvesting and biosensors. This paper reports asymmetric functionalization of the outer surface of a flexible nanochannel polymer membrane to create fluidic diodes that give ICR. Layer-by-layer (LbL) adsorption with cross-linking of only the underlying part of the polyelectrolyte nanofilm leads to a porosity step across the film. The combination of a high effective surface-charge density and the porosity step in the film leads to a remarkable maximum ICR factor of ~200 with a pH gradient across the film. Incorporation of pH-sensitive polyelectrolyte components enables the ICR factor to increase an order of magnitude on going from pH 8 to pH 3. Furthermore, the coated membrane shows excellent anion-selectivity. Thus, LbL adsorption with partial cross-linking provides a simple method for creating coated nanochannel membranes that serve as pH-responsive ionic diodes for potential chemical/biosensors.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Leaching characteristics of toxic constituents from coal fly ash mixed soils under the influence of pH
Highlights: • The impact of pH on the leaching of elements and metals from fly ash mixed soils. • Generally Ca, Cd, Mg, and Sr follows a cationic leaching pattern. • The leaching of As and Se shows an oxyanionic leaching pattern. • The leaching behavior of elements does not change based on material type. • Different fly ash types show different abilities in immobilizing trace elements. - Abstract: Leaching behaviors of Arsenic (As), Barium (Ba), Calcium (Ca), Cadmium (Cd), Magnesium (Mg), Selenium (Se), and Strontium (Sr) from soil alone, coal fly ash alone, and soil-coal fly ash mixtures, were studied at a pH range of 2–14 via pH-dependent leaching tests. Seven different types of soils and coal fly ashes were tested. Results of this study indicated that Ca, Cd, Mg, and Sr showed cationic leaching pattern while As and Se generally follows an oxyanionic leaching pattern. On the other hand, leaching of Ba presented amphoteric-like leaching pattern but less pH-dependent. In spite of different types and composition of soil and coal fly ash investigated, the study reveals the similarity in leaching behavior as a function of pH for a given element from soil, coal fly ash, and soil-coal fly ash mixtures. The similarity is most likely due to similar controlling mechanisms (e.g., solubility, sorption, and solid-solution formation) and similar controlling factors (e.g., leachate pH and redox conditions). This offers the opportunity to transfer knowledge of coal fly ash that has been extensively characterized and studied to soil stabilized with coal fly ash. It is speculated that unburned carbon in off-specification coal fly ashes may provide sorption sites for Cd resulting in a reduction in concentration of these elements in leachate from soil-coal fly ash mixture. Class C fly ash provides sufficient CaO to initiate the pozzolanic reaction yielding hydrated cement products that oxyanions, including As and Se, can be incorporated into.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Lactic Acid is Elevated in Idiopathic Pulmonary Fibrosis and Induces Myofibroblast Differentiation Via pH-Dependent Activation of Transforming Growth Factor-β
Rationale: Idiopathic pulmonary fibrosis (IPF) is a complex disease for which the pathogenesis is poorly understood. In this study, we identified lactic acid as a metabolite that is elevated in the lung tissue of patients with IPF. Objectives: This study examines the effect of lactic acid on myofibroblast differentiation and pulmonary fibrosis. Methods:We used metabolomic analysis to examine cellular metabolism in lung tissuefrom patients with IPFanddeterminedthe effects of lactic acid and lactate dehydrogenase-5 (LDH5) overexpression on myofibroblast differentiation and transforming growth factor (TGF)-b activation in vitro. Measurements and Main Results: Lactic acid concentrations from healthy and IPF lung tissue were determined by nuclear magnetic resonance spectroscopy; a-smooth muscle actin, calponin, and LDH5 expression were assessed by Western blot of cell culture lysates. Lactic acid and LDH5 were significantly elevated in IPF lung tissue compared with controls. Physiologic concentrations of lactic acid induced myofibroblast differentiation via activation of TGF-b. TGF-b induced expression of LDH5 via hypoxia-inducible factor 1a (HIF1a). Importantly, overexpression of both HIF1a and LDH5 in human lung fibroblasts induced myofibroblast differentiation and synergized with low dose TGF-b to induce differentiation. Furthermore, inhibition of both HIF1a and LDH5 inhibited TGF-b–induced myofibroblast differentiation. Conclusions: We have identified the metabolite lactic acid as an important mediator of myofibroblast differentiation via a pHdependent activation of TGF-b. We propose that the metabolic milieu of the lung, and potentially other tissues, is an important driving force behind myofibroblast differentiation and potentially the initiation and progression of fibrotic disorders.
Environmental Molecular Sciences Laboratory↗
The Effect of pH and Time on the Extractability and Speciation of Uranium(VI) Sorbed to SiO2
The effect of pH and contact time on uranium extractability from quartz surfaces was investigated using either acidic or carbonate (CARB) extraction solutions, time-delayed spikes of different U isotopes (i.e., 238U and 233U), and liquid helium temperature time-resolved laser-induced fluorescence spectroscopy (LHeT TRLFS). Quartz powders were reacted with 238U(VI) bearing solutions that were equilibrated with atmospheric CO2 at pH 6, 7, and 8. After a 42 day equilibration period with 238U(VI), the suspensions were spiked with 233U(VI) and reacted for an additional 7 days. Sorbed U was then extracted with either dilute nitric acid or CARB. For the CARB extraction there was a systematic decrease in extraction efficiency for both isotopes from pH 6 to 8. This was mimicked by less desorption of 238U, after the 233U spike, from pH 6 to 8. Further, the efficiency of 233U extraction was consistently greater than that of 238U, indicating a strong temporal component to the strength of U association with the surface that was accentuated with increasing pH. LHeT TRLFS revealed a strong correlation between carbonate extraction efficiency and differences in sorbed U speciation as a function of pH. In contrast, the acid extraction was consistently more efficient than the CARB extraction, with a smaller dependence on both pH and aging time. Collectively, the observations show that aging and pH are critical factors in determining the form and strength of uranium-silica interactions.
54 ENVIRONMENTAL SCIENCES↗
Electron Mobility and Trapping in Ferrihydrite Nanoparticles
Iron is the most abundant transition metal in the Earth's crust, and naturally occurring iron oxide minerals play a commanding role in environmental redox reactions. Although iron oxide redox reactions are well studied, their precise mechanisms are not fully understood. Recent work has shown that these involve electron transfer pathways within the solid, suggesting that overall reaction rates could be dependent on electron mobility. Initial ultrafast spectroscopy studies of iron oxide nanoparticles sensitized by fluorescein derivatives supported a model for electron mobility based on polaronic hopping of electron charge carriers between iron sites, but the constitutive relationships between hopping mobilities and interfacial charge transfer processes has remained obscured. We developed a coarse-grained lattice Monte Carlo model to simulate the collective mobilities and lifetimes of these photoinjected electrons with respect to recombination with adsorbed dye molecules for the essential nanophase ferrihydrite, and tested predictions made by the simulations using pump-probe spectroscopy. We acquired optical transient absorption spectra as a function of particle size and under a variety of solution conditions, and used cryogenic transmission electron microscopy to determine the aggregation state of the nanoparticles. We observed biphasic electron recombination kinetics over timescales that spanned picoseconds to microseconds, the slower regime of which was fit with a stretched exponential decay function. The recombination rates were weakly affected by nanoparticle size and aggregation state, suspension pH, and the injection of multiple electrons per nanoparticle. We conclude that electron mobility indeed limits the rate of interfacial electron transfer in these systems with the slowest processes relating to escape from deep traps, the presence of which outweighs the influence of environmental factors such as pH-dependent surface charge.
77 NANOSCIENCE AND NANOTECHNOLOGY↗