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1.
Environ Technol Innov ; 21: 1-11, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-35586272

RESUMO

Enhancing rapid remediation strategies is paramount for recovery after a large-scale nuclear contamination event in an urban environment. Some current strategies recommend use of readily available equipment, materials, and facilities to expedite recovery. For example, applying pressurized water to contaminated surfaces may effectively remove radioactive contamination. In this study, a commercial power washer removes soluble forms of 152Eu3+, 85Sr2+, and 137Cs+ contamination from common porous building materials, and computer simulations characterize the recycling of the resultant contaminated wash water. Pressure washing the porous building materials under spray conditions typical with do-it-yourself units improved decontamination factors (DFs) for 152Eu compared to low-pressure application of tap water (majority of two-tailed t-test p-values < 0.1), but pressure did not improve DFs for 137Cs or 85Sr. For both pressurized and low-pressure applications, adding potassium ions (K+) to promote ion exchange reactions produced significantly higher DFs for tested radionuclides on asphalt, brick, and concrete. The resultant contaminated wash water can be processed through self-prepared chemical filtration beds of clay and sand. Modeled in a prior study, the beds yielded linear trends (R2 > 0.98) in sensitivity analyses between most bed configuration variables and bed performance variables, permitting flexible ad-hoc bed design. The experimental and simulation results led to estimates of the remediation rate and waste generated after cleaning 250 m2 of cesium-contaminated concrete from the combined deployment of a power washer and two different mobile treatment beds. The first treatment bed was designed to reduce treatment time and processed 1900 L of wash solution in 70 min using 880 kg of clay/sand infill material. Designed to reduce the solid waste generated, the second bed processed the same solution volume in 1040 min (17 h) using 170 kg of clay/sand infill material. The results of this analysis warrant further investigation of power washing with recycled salt solution as an effective rapid decontamination method with manageable waste.

2.
Environ Sci Technol ; 54(3): 1623-1633, 2020 02 04.
Artigo em Inglês | MEDLINE | ID: mdl-31909596

RESUMO

Current predictive models of organic cation sorption assume that sorbates interact with all sites on aluminosilicate minerals in the same manner. To examine whether differences in aluminosilicate structure and the resultant changes in electrostatic potential influence the sorption of organic cations, seven smectites were chosen with different proportions of isomorphic substitutions (origin of clay charge) located in octahedral versus tetrahedral layers and with the presence or absence of aluminosilicate interlayers. Sorption coefficients for 14 benzylamine derivatives with systematic differences in compound structures were collected to understand the possible influence of aluminosilicate mineralogy. Benzylamine compounds with methyl group substitution on the charged amine or with electron-donating or -withdrawing ring substituents displayed decreases in cation exchange-normalized sorption coefficients (KCEC), by up to one order of magnitude, between hectorite (100% isomorphic substitution in the octahedral layer) and nontronite (100% isomorphic substitution in the tetrahedral layer). To understand this difference across aluminosilicates, stochastic molecular models of the various aluminosilicate minerals with interlayers were performed. These models showed that negative charge density associated with tetrahedral sites results in high positive electrostatic energy barriers within the interlayer, creating a penalty for compounds with positive charge spread over a larger compound surface area as occurs from primary to quaternary amines. Conversely, clays with charge originating from octahedral sites produce low electrostatic potential barriers within the interlayer, decreasing the penalty for quaternary amine sorption. Trends for nine cationic pharmaceutical compounds, which varied in size, group alkylation, and/or polar substituents, demonstrated similar decreases in KCEC values to aluminosilicate minerals with high electrostatic energy barriers. Overall, aluminosilicate mineralogy was found to exert a large influence (0.5-1 order of magnitude in sorption coefficients) on organic cation sorption. The application of atomistic electrostatic potential mapping of both sorbent and sorbate structures provided insights to explain trends in sorption coefficients that could not be described by the basic electrostatic potential theory or by assuming that sorbate structure moieties yielded additive sorption contributions.


Assuntos
Silicatos de Alumínio , Adsorção , Cátions , Eletricidade Estática
3.
J Environ Radioact ; 208-209: 105858, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31202509

RESUMO

The release of radiological material from a nuclear incident has the potential to cause extensive radiological contamination requiring rapid decontamination. A promising method for rapid remediation is the use of pressure washers to decontaminate building and street surfaces. Pressure washers utilize both physical removal through surface ablation and chemical removal through desorption of bonded radionuclides. To understand the extent that each removal mechanism is present, overall removals, depth profiles, and wash water were analyzed from the pressure washing of various surfaces contaminated with cesium, strontium, and europium. Removals were dependent on surface type with over 80% of the radionuclides removed from concrete, 50-80% from asphalt, and only 20-25% from brick. Generally, the closer the radionuclide was to the surface of the material, the higher the removal, with europium being removed most readily followed by cesium then strontium, though some exceptions were evident. Comparing these removals and depth profiles of radionuclides in non-decontaminated coupons revealed that cesium and europium are mostly removed through surface ablation. Strontium, on the other hand, is desorbed from the surface, especially from brick and asphalt surfaces. Correspondingly, cesium and europium were attached to the particulates that were likely removed with the pressurized water. Strontium was primarily dissolved in the wash water, supporting the observation that the radionuclide is desorbed from each surface. Finally, the faster the surfaces were brought through the high pressure spray, the lower the removals, arising from decreases in both the physical and desorption mechanisms. Pressure washers were concluded to be a promising decontamination method during radiological incident relief. However, the surface and radionuclide identity must be considered when developing proper procedures.


Assuntos
Materiais de Construção , Descontaminação/métodos , Liberação Nociva de Radioativos
4.
Chemosphere ; 222: 106-113, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30699369

RESUMO

Recent characterization of radioactive particles indicate that a large percentage of the radioactivity observed during the Fukushima Daiichi nuclear meltdown was insoluble 137Cs bound within silica microparticles. Therefore, much of the decontamination research performed prior to the Fukushima incident that used either soluble radionuclides deposited onto wet surfaces or large (∼100 µm) particles characteristic of nuclear weapons fallout do not accurately represent the characteristics of potential contamination. Thus, the common practice of extrapolating radioactive decontamination methods generically to all radioactive release events is, at best, suspect. In response, a method to produce chemically-inert, radiolabeled silica particles was developed. Binding 152Eu within a sodium silicate coating required proper temperature control and ethanol was beneficial as a volatile dispersant to limit residues. In the end, a step-wise method, which first deposited 152Eu or 241Am as a nitrate salt, decomposed the salt to a sesquioxide, and finally coated the surface with sodium silicate led to dispersed particles of the desired 2 or 0.5 µm diameters. Dynamic light scattering and scanning election microscopy confirmed the particle size was unchanged. Leaching studies into several common decontaminants were performed to ensure particle inertness. Our approach allows for substitution of other radionuclides making it a robust, simple, and novel method to produce inert particle surrogates for a release event that allows direct comparison of decontamination techniques and contaminant fate studies, greatly aiding the development of response and recovery plans.


Assuntos
Descontaminação/métodos , Monitoramento de Radiação/métodos , Cinza Radioativa/prevenção & controle , Silicatos/farmacologia , Poluentes Radioativos da Água/isolamento & purificação , Amerício , Radioisótopos de Césio , Einstêinio , Acidente Nuclear de Fukushima , Japão , Tamanho da Partícula , Monitoramento de Radiação/normas
5.
Environ Sci Technol ; 51(11): 6193-6201, 2017 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-28459593

RESUMO

With the increasing number of emerging contaminants that are cationic at environmentally relevant pH values, there is a need for robust predictive models of organic cation sorption coefficients (Kd). Current predictive models fail to account for the differences in the identity, abundance, and affinity of surface-associated inorganic exchange ions naturally present at negatively charged receptor sites on environmental solids. To better understand how organic cation sorption is influenced by surface-associated inorganic exchange ions, sorption coefficients of 10 organic cations (including eight pharmaceuticals and two simple probe organic amines) were determined for six homoionic forms of the aluminosilicate mineral, montmorillonite. Organic cation sorption coefficients exhibited consistent trends for all compounds across the various homoionic clays with sorption coefficients (Kd) decreasing as follows: KdNa+ > KdNH4+ ≥ KdK+ > KdCa2+ ≥ KdMg2+ > KdAl3+. This trend for competition between organic cations and exchangeable inorganic cations is consistent with the inorganic cation selectivity sequence, determined for exchange between inorganic ions. Such consistent trends in competition between organic and inorganic cations suggested that a simple probe cation, such as phenyltrimethylammonium or benzylamine, could capture soil-to-soil variations in native inorganic cation identity and abundance for the prediction of organic cation sorption to soils and soil minerals. Indeed, sorption of two pharmaceutical compounds to 30 soils was better described by phenyltrimethylammonium sorption than by measures of benzylamine sorption, effective cation exchange capacity alone, or a model from the literature (Droge, S., and Goss, K. Environ. Sci. Technol. 2013, 47, 14224). A hybrid approach integrating structural scaling factors derived from this literature model of organic cation sorption, along with phenyltrimethylammonium Kd values, allowed for estimation of Kd values for more structurally complex organic cations to homoionic montmorillonites and to heteroionic soils (mean absolute error of 0.27 log unit). Accordingly, we concluded that the use of phenyltrimethylammonium as a probe compound was a promising means to account for the identity, affinity, and abundance of natural exchange ions in the prediction of organic cation sorption coefficients for environmental solids.


Assuntos
Cátions , Poluentes do Solo , Adsorção , Troca Iônica , Solo
6.
Chemosphere ; 162: 165-71, 2016 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-27494317

RESUMO

Procedures for removing harmful radiation from interior and exterior surfaces of homes and businesses after a nuclear or radiological disaster may generate large volumes of radiologically contaminated waste water. Rather than releasing this waste water to potentially contaminate surrounding areas, it is preferable to treat it onsite. Retention barrels are a viable option because of their simplicity in preparation and availability of possible sorbent materials. This study investigated the use of aluminosilicate clay minerals as sorbent materials to retain (137)Cs, (85)Sr, and (152)Eu. Vermiculite strongly retained (137)Cs, though other radionuclides displayed diminished affinity for the surface. Montmorillonite exhibited increased affinity to sorb (85)Sr and (152)Eu in the presence of higher concentrations of (137)Cs. To simulate flow within retention barrels, vermiculite was mixed with sand and used in small-scale column experiments. The GoldSim contaminate fate module was used to model breakthrough and assess the feasibility of using clay minerals as sorbent materials in retention barrels. The modeled radionuclide breakthrough profiles suggest that vermiculite-sand and montmorillonite-sand filled barrels could be used for treatment of contaminated water generated from field operations.


Assuntos
Liberação Nociva de Radioativos , Radioisótopos/química , Radioisótopos/isolamento & purificação , Águas Residuárias/química , Poluentes Radioativos da Água/química , Poluentes Radioativos da Água/isolamento & purificação , Adsorção , Silicatos de Alumínio/química , Bentonita/química , Argila , Cinética , Modelos Teóricos
7.
Environ Sci Technol ; 50(15): 8196-204, 2016 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-27379799

RESUMO

Column chromatography was evaluated as a method to obtain organic cation sorption isotherms for environmental solids while using the peak skewness to identify the linear range of the sorption isotherm. Custom packed HPLC columns and standard batch sorption techniques were used to intercompare sorption isotherms and solid-water sorption coefficients (Kd) for four organic cations (benzylamine, 2,4-dichlorobenzylamine, phenyltrimethylammonium, oxytetracycline) with two aluminosilicate clay minerals and one soil. A comparison of Freundlich isotherm parameters revealed isotherm linearity or nonlinearity was not significantly different between column chromatography and traditional batch experiments. Importantly, skewness (a metric of eluting peak symmetry) analysis of eluting peaks can establish isotherm linearity, thereby enabling a less labor intensive means to generate the extensive data sets of linear Kd values required for the development of predictive sorption models. Our findings clearly show that column chromatography can reproduce sorption measures from conventional batch experiments with the benefit of lower labor-intensity, faster analysis times, and allow for consistent sorption measures across laboratories with distinct chromatography instrumentation.


Assuntos
Cátions/química , Solo/química , Adsorção , Cromatografia , Poluentes do Solo
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