Contrasting role of antimony and bismuth dopants on the thermoelectric performance of lead selenide
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charge transport↗
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Thermal conductivity of bulk nanostructured lead telluride
Thermal conductivity of lead telluride with embedded nanoinclusions was examined using Monte Carlo simulations with intrinsic phonon transport properties obtained from first-principles-based lattice dynamics. The nanoinclusion/matrix interfaces were set to completely reflect phonons to model the maximum interface-phonon-scattering scenario. The simulations with the geometrical cross section and volume fraction of the nanoinclusions matched to those of the experiment show that the experiment has already reached the theoretical limit of thermal conductivity. The frequency-dependent analysis additionally identifies that the thermal conductivity reduction is dominantly attributed to scattering of low frequency phonons and demonstrates mutual adaptability of nanostructuring and local disordering.
36 MATERIALS SCIENCE↗
Observation of the dynamics leading to a conical intersection in dissociative electron attachment to water
Following prior work on the lower-energy resonances, we apply techniques of momentum imaging and ab initio scattering calculations to the process of dissociative electron attachment to water via the highest-energy {sup 2}B{sub 2} resonance. We focus on the H{sup -} anion fragment, which is produced via dynamics passing through and avoiding the conical intersection with the lower A{sub 1} state, leading to OH ({sup 2}{Pi}) and OH ({sup 2}{Sigma}), respectively. The momentum imaging technique, when combined with theoretical calculations on the attachment amplitude and dissociation dynamics, demonstrates that the angular distributions provide a signature of the location of the conical intersection in the space of nuclear configurations.
74 ATOMIC AND MOLECULAR PHYSICS↗
Next-to-leading order analysis of target mass corrections to structure functions and asymmetries
Not Available
Brady, L. T.↗
Axial couplings in heavy-hadron chiral perturbation theory at the next-to-leading order
Not Available
Detmold, William↗
Recycling of Lead Pastes from Spent Lead–Acid Batteries: Thermodynamic Constraints for Desulphurization
Lead–acid batteries are important to modern society because of their wide usage and low cost. The primary source for production of new lead–acid batteries is from recycling spent lead–acid batteries. In spent lead–acid batteries, lead is primarily present as lead pastes. In lead pastes, the dominant component is lead sulfate (PbSO 4 , mineral name anglesite) and lead oxide sulfate (PbO•PbSO 4 , mineral name lanarkite), which accounts for more than 60% of lead pastes. In the recycling process for lead–acid batteries, the desulphurization of lead sulfate is the key part to the overall process. In this work, the thermodynamic constraints for desulphurization via the hydrometallurgical route for recycling lead pastes are presented. The thermodynamic constraints are established according to the thermodynamic model that is applicable and important to recycling of lead pastes via hydrometallurgical routes in high ionic strength solutions that are expected to be in industrial processes. The thermodynamic database is based on the Pitzer equations for calculations of activity coefficients of aqueous species. The desulphurization of lead sulfates represented by PbSO 4 can be achieved through the following routes. (1) conversion to lead oxalate in oxalate-bearing solutions; (2) conversion to lead monoxide in alkaline solutions; and (3) conversion to lead carbonate in carbonate solutions. Among the above three routes, the conversion to lead oxalate is environmentally friendly and has a strong thermodynamic driving force. Oxalate-bearing solutions such as oxalic acid and potassium oxalate solutions will provide high activities of oxalate that are many orders of magnitude higher than those required for conversion of anglesite or lanarkite to lead oxalate, in accordance with the thermodynamic model established for the oxalate system. An additional advantage of the oxalate conversion route is that no additional reductant is needed to reduce lead dioxide to lead oxide or lead sulfate, as there is a strong thermodynamic force to convert lead dioxide directly to lead oxalate. As lanarkite is an important sulfate-bearing phase in lead pastes, this study evaluates the solubility constant for lanarkite regarding the following reaction, based on the solubility data, PbO•PbSO 4 + 2H + ⇌ 2Pb 2+ + SO 4 2– + H 2 O(l).
25 ENERGY STORAGE↗
Plumbojarosite Remediation of Soil Affects Lead Speciation and Elemental Interactions in Soil and in Mice Tissues
Lead (Pb) contamination of soils is of global concern due to the devastating impacts of Pb exposure in children. Because early-life exposure to Pb has long-lasting health effects, reducing exposure in children is a critical public health goal that has intensified research on the conversion of soil Pb to low bioavailability phases. Recently, plumbojarosite (PLJ) conversion of highly available soil Pb was found to decrease Pb relative bioavailability (RBA <10%). However, there is sparse information concerning interactions between Pb and other elements when contaminated soil, pre- and post-remediation, is ingested and moves through the gastrointestinal tract (GIT). Addressing this may inform drivers of effective chemical remediation strategies. In this study, we utilize bulk and micro-focused Pb X-ray absorption spectroscopy to probe elemental interactions and Pb speciation in mouse diet, cecum, and feces samples following ingestion of contaminated soils pre- and post-PLJ treatment. RBA of treated soils was less than 1% with PLJ phases transiting the GIT with little absorption. In contrast, Pb associated with organics was predominantly found in the cecum. These results are consistent with transit of insoluble PLJ to feces following ingestion. The expanded understanding of Pb interactions during GIT transit complements our knowledge of elemental interactions with Pb that occur at higher levels of biological organization.
54 ENVIRONMENTAL SCIENCES↗
Examination of lead concentrations in new decorative enamel paints in four countries with different histories of activity in lead paint regulation
Paints with high lead concentrations (ppm) continue to be sold around the world in many developing countries and those with economies in transition representing a major preventable environmental health hazard that is being increased as the economies expand and paint consumption is increasing. Prior lead paint testing had been performed in Brazil and India and these countries were selected to examine the impact of a new regulatory limit in Brazil and the impact of efforts of non-governmental organizations and others to stop the use of lead compounds in manufacturing paints. Armenia and Kazakhstan, in Central Asia, were selected because no information on lead concentration in those regions was available, no regulatory activities were evident and non-governmental organizations in the IPEN network were available to participate. Another objective of this research was to evaluate the lead loading (µg/cm{sup 2}) limit determined by X-Ray Fluorescence (XRF) for areas on toys that are too small to obtain a sample of sufficient size for laboratory analysis. The lead concentrations in more than three-fourths of the paints from Armenia and Kazakhstan exceeded 90 ppm, the limit in the United States, and 600 ppm, the limit in Brazil. The percentages were about one-half as high in Brazil and India. The average concentration in paints purchased in Armenia, 25,000 ppm, is among the highest that has been previously reported, that in Kazakhstan, 15,700 ppm, and India, 16,600, about median. The average concentration in Brazil, 5600 ppm, is among the lowest observed. Paints in Brazil that contained an average of 36,000 ppm before the regulatory limit became effective were below detection (<9 ppm) in samples collected in the current study. The lack of any apparent public monitoring of paint lead content as part of regulatory enforcement makes it difficult to determine whether the regulation was a major factor contributing to the decline in lead use in these paints. Using data from the current study and those available from other studies 24 of 28 paints from major brands in India decreased from high concentrations to 90 ppm or lower. Since lead concentrations in golden yellow paints from these brands were found to decrease to ≤90 ppm, it is possible that all 28 of these paints now contain ≤90 ppm since yellow paints usually have the highest lead concentrations. Other brands in Brazil and India that have been analyzed only one time had lead concentrations up to 59,000 ppm and 134,000 ppm, respectively. Less than one-third of the paints had notations on their labels with information about lead content and these were sometimes inaccurate. The label from one brand indicating “no added lead” contained paint with 134,000 ppm lead, the highest found in this study. Three percent (3 of 98) of the paints with surface lead loading that did not exceed 2 µg/cm{sup 2}, the limit established by the Consumer Product Safety Improvement Act for small areas on toys, contained greater than 90 ppm lead and thus were false negatives. Of the new paint samples that contained ≤600 ppm, 88% contained ≤90 ppm. Of the samples that contained ≤90 ppm, 97% contained ≤45 ppm and 92% contained ≤15 ppm. Based on these data it appears to be technically feasible to manufacture paints containing ≤90 ppm and in many cases to produce paints that have lead concentrations that do not exceed 15 ppm. - Highlights: • Brazilian paints with high lead (avg. 36,000 ppm) contained <9 ppm after regulation. • Lead in major Indian paint brands decreased to low levels by efforts of NGOs/others. • Most paints with lead ≤600 ppm also are ≤90 ppm and many also ≤15 ppm. • At the CPSIA limit of 2 µg Pb/cm{sup 2} for small areas on toys, 3% exceeded 90 ppm lead. • Most paint brands in Armenia and Kazakhstan based/manufactured outside the country.
54 ENVIRONMENTAL SCIENCES↗
Surface dust wipes are the best predictors of blood leads in young children with elevated blood lead levels
Background: As part of the only national survey of lead in Australian children, which was undertaken in 1996, lead isotopic and lead concentration measurements were obtained from children from 24 dwellings whose blood lead levels were ≥15 µg/dL in an attempt to determine the source(s) of their elevated blood lead. Comparisons were made with data for six children with lower blood lead levels (<10 µg/dL). Methods: Thermal ionisation and isotope dilution mass spectrometry were used to determine high precision lead isotopic ratios ({sup 208}Pb/{sup 206}Pb, {sup 207}Pb/{sup 206}Pb and {sup 206}Pb/{sup 204}Pb) and lead concentrations in blood, dust from floor wipes, soil, drinking water and paint (where available). Evaluation of associations between blood and the environmental samples was based on the analysis of individual cases, and Pearson correlations and multiple regression analyses based on the whole dataset. Results and discussion: The correlations showed an association for isotopic ratios in blood and wipes (r=0.52, 95% CI 0.19–0.74), blood and soil (r=0.33, 95% CI −0.05–0.62), and blood and paint (r=0.56, 95% CI 0.09–0.83). The regression analyses indicated that the only statistically significant relationship for blood isotopic ratios was with dust wipes (B=0.65, 95% CI 0.35–0.95); there were no significant associations for lead concentrations in blood and environmental samples. There is a strong isotopic correlation of soils and house dust (r=0.53, 95% CI 0.20–0.75) indicative of a common source(s) for lead in soil and house dust. In contrast, as with the regression analyses, no such association is present for bulk lead concentrations (r=−0.003, 95% CI −0.37–0.36), the most common approach employed in source investigations. In evaluation of the isotopic results on a case by case basis, the strongest associations were for dust wipes and blood. -- Highlights: • Children with elevated blood lead ≥15 µg/dL compared with a group with <10 µg/dL. • High precision lead isotopic ratios in blood, house dust wipes, soil, water, paint. • Associations for isotopic measures of blood and dust, blood and soil, blood and paint. • Regressions gave significance for isotopic measures of blood/dust and dust/soil.
54 ENVIRONMENTAL SCIENCES↗
Formation and Aggregation of Lead Phosphate Particles: Implications for Lead Immobilization in Water Supply Systems
Phosphate is commonly added to drinking water to inhibit lead release from lead service lines and lead-containing materials in premise plumbing. Phosphate addition promotes the formation of lead phosphate particles, and their aggregation behaviors may affect their transport in pipes. In this work, lead phosphate formation and aggregation were studied under varied aqueous conditions typical of water supply systems. Under high aqueous PO 4 /Pb molar ratios (>1), phosphate adsorption made the particles more negatively charged. Therefore, enhanced stability of lead phosphate particles was observed, suggesting that although addition of excess phosphate can lower the dissolved lead concentrations in tap water, it may increase concentrations of particulate lead. Adsorption of divalent cations (Ca 2+ and Mg 2+ ) onto lead phosphate particles neutralized their negative surface charges and promoted their aggregation at pH 7, indicating that phosphate addition for lead immobilization may be more efficient in harder waters. The presence of natural organic matter (NOM, ≥ 0.05 mg C/L humic acid and ≥ 0.5 mg C/L fulvic acid) retarded particle aggregation at pH 7. Consequently, removal of organic carbon during water treatment to lower the formation of disinfection-byproducts (DBPs) may have the additional benefit of minimizing the mobility of lead-containing particles. This study provided insight into fundamental mechanisms controlling lead phosphate aggregation. Such understanding is helpful to understand the observed trends of total lead in water after phosphate addition in both field and pilot-scale lead pipe studies. Also, it can help optimize lead immobilization by better controlling the water chemistry during phosphate addition.
54 ENVIRONMENTAL SCIENCES↗
SU-E-P-09: Radiation Transmission Measurements and Evaluation of Diagnostic Lead-Based and Lead-Free Aprons
Purpose: This study was conducted to ensure that various lead shield apron manufacturers provided accurate attenuation factors regardless of whether the apron was made of lead-based or lead-free equivalent material. Methods: A calibrated ionization survey meter was placed at chest height and 36 cm horizontally away from a solid water phantom on a simulator couch. Measurements were done with or without apron. Radiation field was set to 24cmx24cm with the phantom at 100cm source-to-surface distance. Irradiation time was set for 1 minute at voltages of 60, 80, 100 and 120 kVp. Current was set at 6mA. Results: Between 60 kVp and 120 kVp, the transmission through 0.50 mm of lead-based apron was between 1.0% and 6.5% with a mean value of 3.2% and a standard deviation (s.d.) of 1.4%. The transmissions through the 0.50 mm lead-free aprons were 1.0 % to 12.0% with a mean value of 6.1% and s.d. of 2.6%. At 120 kVp, the transmission value was 6.5% for 0.50 mm lead-based apron and 11.1% to 12.0% for 0.50 mm lead-free aprons. The radiation transmissions at 80 kVp, measured in two different 0.5 mm lead-free aprons, were 4.3% each. However, only 1.4% transmission was found through the lead-based apron. Overall, the radiation transmitted through the lead-based apron was 1/3 transmission of lead-free at 80kVp, and half value of lead-free aprons at 100 and 120 kVp. Conclusion: Even though lead-based and lead-free aprons all claimed to have the same lead equivalent thickness, the transmission might not be the same. The precaution was needed to exercise diligence in quality assurance program to assure adequate protection to staff who wear it during diagnostic procedures. The requirement for aprons not only should be in certain thickness to meet state regulation but also to keep reasonably achievable low exposure with the accurate labeling from manufacturers.
07 ISOTOPE AND RADIATION SOURCES↗
Prevalence of elevated blood lead levels among pregnant women and sources of lead exposure in rural Bangladesh: A case control study
Highlights: • Prenatal blood lead levels and lead sources are assessed in rural Bangladesh. • Elevated blood lead levels are found among pregnant women. • Multiple possible sources of lead are identified; all related to food. • Future lead prevention studies should investigate food storage and production. Prenatal and early childhood lead exposures impair cognitive development. We aimed to evaluate the prevalence of elevated blood lead levels (BLLs) among pregnant women in rural Bangladesh and to identify sources of lead exposure. We analyzed the BLLs of 430 pregnant women randomly selected from rural communities in central Bangladesh. Fifty-seven cases were selected with the highest BLLs, ≥ 7 μg/dL, and 59 controls were selected with the lowest BLLs, < 2 μg/dL. An exposure questionnaire was administered and soil, rice, turmeric, water, traditional medicine, agrochemical, and can samples were analyzed for lead contamination. Of all 430 women, 132 (31%) had BLLs > 5 μg/dL. Most women with elevated BLLs were spatially clustered. Cases were 2.6 times more likely than controls to consume food from a can (95% CI 1.0–6.3, p = 0.04); 3.6 times more likely to use Basudin, a specific brand of pesticide (95% CI 1.6–7.9, p = 0.002); 3.6 times more likely to use Rifit, a specific brand of herbicide (95% CI 1.7–7.9, p = 0.001); 2.9 times more likely to report using any herbicides (95% CI 1.2–7.3, p = 0.02); and 3.3 times more likely to grind rice (95% CI 1.3–8.4, p = 0.01). Five out of 28 food storage cans were lead-soldered. However, there was minimal physical evidence of lead contamination from 382 agrochemical samples and 129 ground and unground rice samples. Among 17 turmeric samples, one contained excessive lead (265 μg/g) and chromium (49 μg/g). Overall, we found evidence of elevated BLLs and multiple possible sources of lead exposure in rural Bangladesh. Further research should explicate and develop interventions to interrupt these pathways.
54 ENVIRONMENTAL SCIENCES↗
In situ investigation of the formation and metastability of formamidinium lead tri-iodide perovskite solar cells
Organic–inorganic perovskites have emerged as an important class of next generation solar cells due to their remarkably low cost, band gap, and sub-900 nm absorption onset. Here, we show a series of in situ observations inside electron microscopes and X-ray diffractometers under device-relevant synthesis conditions focused on revealing the crystallization process of the formamidinium lead-triiodide perovskite at the optimum temperature of 175 °C. Direct in situ observations of the structure and chemistry over relevant spatial, temporal, and temperature scales enabled identification of key perovskite formation and degradation mechanisms related to grain evolution and interface chemistry. The lead composition was observed to fluctuate at grain boundaries, indicating a mobile lead-containing species, a process found to be partially reversible at a key temperature of 175 °C. Using low energy electron microscopy and valence electron energy loss spectroscopy, lead is found to be bonded in the grain interior with iodine in a tetrahedral configuration. At the grain boundaries, the binding energy associated with lead is consequently shifted by nearly 2 eV and a doublet peak is resolved due presumably to a greater degree of hybridization and the potential for several different bonding configurations. At the grain boundaries there is adsorption of hydrogen and OH¯ ions as a result of residual water vapor trapped as a non-crystalline material during formation. Lastly, insights into the relevant formation and decomposition reactions of formamidinium lead iodide at low to high temperatures, observed metastabilities, and relationship with the photovoltaic performance were obtained and used to optimize device processing resulting in conversion efficiencies of up to 17.09% within the stability period of the devices.
14 SOLAR ENERGY↗
Modeling of Blood Lead Levels in Astronauts Exposed to Lead from Microgravity-Accelerated Bone Loss
Human exposure to lead has been associated with toxicity to multiple organ systems. Studies of various population groups with relatively low blood lead concentrations (<10 μg/dL) have indicated associations of blood lead level with lower cognitive test scores in children, later onset of puberty in girls, and increased blood pressure and cardiovascular mortality rates in adults. Cognitive effects are considered by regulatory agencies to be the most sensitive endpoint at low doses. Although ~95% of the body burden of lead is stored in the bones, the adverse effects of lead correlate with the concentration of lead in the blood better than with that in the bones. NASA has found that prolonged exposure to microgravity during spaceflight results in a significant loss of bone minerals, the extent of which varies from individual to individual and from bone to bone, but generally averages about 0.5% per month. During such bone loss, lead that had been stored in bones would be released along with calcium. The effects on the concentration of lead in the blood (PbB) of various concentrations of lead in drinking water (PbW) and of lead released from bones due to accelerated osteoporosis in microgravity, as well as changes in exposure to environmental lead before, during, and after spaceflight were evaluated using a physiologically based pharmacokinetic (PBPK) model that incorporated exposure to environmental lead both on earth and in flight and included temporarily increased rates of osteoporosis during spaceflight.
Garcia, H.↗
Activation of lead coolant in Westinghouse lead fast reactor
The Westinghouse Lead-cooled Fast Reactor (LFR) is a medium-sized, passively safe, scalable reactor being developed by Westinghouse in collaboration with domestic and international organizations with the primary goals of reducing front-end capital cost and generating flexible and cost-competitive electricity while satisfying the highest standards in terms of safety and sustainability. An important aspect of new plant design is an assessment of activation level of its components so that an appropriate nuclear waste management plan can be established. As lead coolant is a distinguishing design feature of the LFR, its activation due to irradiation and the implications on establishing an appropriate waste disposal approach are important for engagement of project stakeholders, customers and nuclear safety regulators. This paper provides a brief description of the Westinghouse LFR design, a background on lead activation phenomenology, and then describes the methodology used for lead activation analysis performed with the computer code Serpent 2. It was determined that impurities naturally occurring in lead have the biggest contribution to lead activation. Corrosion and erosion products from the components immersed in lead can also be important contributors to lead activity and their impact can be limited by appropriate selection of materials and operating conditions. Polonium isotopes, resulting from bismuth generated from lead irradiation and its impurities, bring a notable contribution to the inhalation and ingestion doses during the plant operation and in the first years after the plant shutdown. However, it is not by far as important as for lead-bismuth coolant.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
Electrochemical deposition of amorphous aluminum oxides on lead pipes to prevent lead leaching into the drinking water
Over 5000 public drinking water systems in the US are out of compliance with the Lead and Copper Rule. Lead leaching from lead pipes is limited by the solubility of a naturally occurring scale. Changes in water quality may cause this scale to become more soluble, releasing lead into the drinking water. We propose a novel electrochemical method to prevent lead leaching from lead pipes. In this method, an aluminum wire and an alkaline phosphate electrolyte are inserted into the pipes. The pipes are then anodized for 2 h by using an external power supply, resulting in the electrodeposition of an insoluble aluminum oxide layer on top of the preexisting scale. This technology was tested on lead pipes from the EBMUD water distribution systems located in Berkeley, CA, using recirculating synthetic and actual tap water for 120 days. The untreated pipes leached an average of 23 ppb and 38 ppb of lead respectively, when using free chlorine and monochloramine as disinfection residuals. In contrast, the treated pipes leached 3 ppb and 5 ppb respectively. These results suggest that the proposed treatment has the potential to prevent lead leaching regardless of the disinfection residual and thus should be further explored in a field trial.
36 MATERIALS SCIENCE↗
Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability
Bond length and bond angle exhibited by valence electrons is essential to the core of chemistry. Using lead-based organic–inorganic perovskite compounds as an exploratory platform, it is demonstrated that the modulation of valence electrons by compression can lead to discovery of new properties of known compounds. Yet, despite its unprecedented progress, further efficiency boost of lead-based organic–inorganic perovskite solar cells is hampered by their wider bandgap than the optimum value according to the Shockley–Queisser limit. By modulating the valence electron wavefunction with modest hydraulic pressure up to 2.1 GPa, the optimized bandgap for single-junction solar cells in lead-based perovskites, for the first time, is achieved by narrowing the bandgap of formamidinium lead triiodide (HC(NH 2 ) 2 PbI 3 ) from 1.489 to 1.337 eV. Strikingly, such bandgap narrowing is partially retained after the release of pressure to ambient, and the bandgap narrowing is also accompanied with double-prolonged carrier lifetime. With First-principles simulation, this work opens a new dimension in basic chemical understanding of structural photonics and electronics and paves an alternative pathway toward better photovoltaic materials-by-design.
14 SOLAR ENERGY↗
Environmental and take-home lead exposure in children living in the vicinity of a lead battery smelter in Serbia
Highlights: • Children living near a battery recycling plant had elevated blood lead levels (BLLs). • Children 0–6 years old living closest to the plant had the highest BLLs. • Higher lead exposure was found in children whose fathers worked in the plant. • The contribution of take-home lead exposure was between 25% and 40%. Blood lead levels (BLLs) have been falling steadily worldwide due to restricted use of lead (Pb) and its compounds. although they remain above preindustrial Pb levels. Elevated BLL can still be found in children living near secondary Pb smelters that represent around 50% of Pb production. There have been no studies on Pb exposure in children living in Serbia ever since the 1980s. The aim of this study was to evaluate the BLLs in children living in two villages in Serbia (Zajača, the location of a secondary lead smelter, and Paskovac, 5 km away), identify the primary determinants of children’s BLLs, and investigate the impact of BLLs on children’s health symptoms and school achievement. The study was conducted in 2011 on 127 children, aged 1–18 years, whose BLLs were measured using inductively coupled argon plasma mass spectrometry (ICP-MS). The median BLL in children was 12 μg/dl, with a significantly higher value of 17.5 μg/dl in Zajača, compared to 7.6 μg/dl in Paskovac. Only 1 out of 75 and 12 out of 52 children from Zajača and Paskovac, respectively, had BLLs below the CDC recommended 5 μg/dl level. Living near the smelter resulted in 19 times, and having a father who works in the plant 4 times higher odds of elevated BLLs. No significant effects of elevated BLLs health symptoms were seen in this study. BLLs of children living near a battery recycling plant in Serbia, an upper-middle income European country, were in the range and even higher than those of children living in developing countries. For the first time, the contribution of environmental and take-home lead exposure was quantified using mixed-effect modeling, and our results indicate a contribution of 25–40% of the take-home lead exposure to the BLLs of children living in the vicinity of a secondary lead smelter.
54 ENVIRONMENTAL SCIENCES↗