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Chemosphere ; 238: 124466, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31425866


Arsenite is a highly toxic compound present in many water sources around the world. The removal of arsenite from water requires its oxidation to arsenate which is much more amenable to treatment using well attested technologies. Prior research has shown that the oxidation of arsenite by hydroxyl radicals is significantly accelerated in the presence of carbonate ions but the intrinsic mechanisms of the acceleration have not yet been established. The main goal of the present work was to examine the oxidation of arsenite in the framework of the density functional theory, to establish a detailed microscopic level mechanism of interactions between arsenite and hydroxyl radicals and to elucidate the nature of the catalytic effect of carbonate ions. Results of this study demonstrate that the [As(OH)2CO3]- complex is the thermodynamically most stable species formed in the system H3AsO3-CO32-/HCO3--H2O. Interactions of the hydroxyl radical with the [As(OH)2CO3]- complex yield the pre-reaction complex [As(OH)3CO3]-∗ in the reaction of subsequent oxidation of arsenite. The structures of the reactants, products and transition states, as well as pre- and post-reaction complexes corresponding to several possible mechanisms of the first stage of As(III) oxidation to As(IV) intermediate using hydroxyl radicals in the absence and in the presence of [As(OH)2CO3]-, were determined in this study. The data demonstrate that the arsenite-carbonate complexes [As(OH)2CO3]- are characterized by a significantly lower activation energy of the first oxidation stage under the action of a hydroxyl radical (2.8 kcal/mol) compared to that for the free arsenite H3AsO3 (13.6 kcal/mol).

Arsenitos/química , Carbonatos/química , Radical Hidroxila/química , Teoria Quântica , Água/química , Catálise , Modelos Moleculares , Conformação Molecular , Oxirredução , Termodinâmica
Water Sci Technol ; 63(1): 40-4, 2011.
Artigo em Inglês | MEDLINE | ID: mdl-21245551


Among known but unregulated disinfection by-products (DBPs), several nitrogenous species (N-DBPs) have been found in drinking waters. While concentrations of N-DBP are much lower than those of trihalomethanes (THMs) and haloacetic acids (HAAs), their potential toxicity is higher. In this study the relationships between the formation of N-DBPs and the changes in NOM caused by the chlorination of raw Ancipa water quantified by the use of differential absorbance and fluorescence indexes were investigated. Very strong relationships were found between selected N-DBPs (i.e. trichloronitromethane and dichloroacetonitrile) and the proposed spectroscopic indexes that were previously developed to quantify the changes in natural organic matter (NOM) during chlorination at varying reaction conditions (chlorine dose, reaction time and temperature) and the generation of DBPs. Obtained results clearly indicate that the changes in NOM absorbance and fluorescence are fundamental descriptors of the formation of both commonly controlled halogenated DBPs and N-DBPs. This approach may be suitable for real time monitoring of emerging N-DBPs and for studying their formation pathways.

Cloro/análise , Desinfecção , Nitrogênio/análise , Espectrometria de Fluorescência/métodos , Espectrofotometria Ultravioleta/métodos
J Hazard Mater ; 168(2-3): 782-6, 2009 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-19299084


A kinetic model capable of simulating by-products formation in bromide-containing waters during disinfection processes is presented in this paper. The model is based on two parallel sequences of incorporation and oxidation reactions induced by bromine or chlorine reacting with natural organic matter (NOM). Each sequence starts from a different type of NOM functionality that has its own set of specific reaction rate. Decay reactions of NOM and halogenated intermediates are assumed to follow a first order kinetic, while disinfection by-product (DBP) generation reactions are simulated introducing so-called splitting coefficients. This approach allows obtaining explicit expressions for DBP species. Model's results are compared with experimental data obtained for seawater samples. Comparison of the data confirms the model's ability to predict DBPs formation with high precision.

Brometos/química , Desinfetantes/química , Modelos Teóricos , Oxirredução
Water Res ; 35(15): 3545-50, 2001 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-11561613


The influence of heating or boiling on the formation and behavior of disinfection by-products (DBPs) was investigated in DBP-spiked reagent water, municipal tap water, and synthetic water containing chlorinated aquatic humic substances. Thermal cleavage of larger halogenated species leads to both formation of smaller chlorinated molecules (including THMs and HAAs) and dechlorination of organics. In parallel with their formation from larger molecules, THMs can be volatilized, and this latter process dominates the change in their concentration when water is boiled. HAAs are not volatile, but they can be destroyed by chemical reactions at elevated temperatures, with the net effect being loss of trihalogenated HAAs and either formation or loss of less chlorinated HAAs. Although other identifiable DBPs can be generated at slightly elevated temperatures, in most cases their concentrations decline dramatically when the solution is heated.

Compostos Clorados/química , Desinfetantes/química , Purificação da Água , Abastecimento de Água , Halogênios , Substâncias Húmicas , Oxidantes/química , Temperatura Ambiente
Environ Sci Technol ; 35(24): 4905-9, 2001 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-11775169


The ability of iron oxide-coated sand (IOCS) to adsorb strontium from synthetic wastes simulating the tank wastes at the Hanford Nuclear Reservation was examined in this study. These wastes have high pH and high ionic strength, containing up to 5.5 M Na+, 3.7 M NO3-, and 1.2 M OH-. The use of IOCS in such applications may be advantageous because it is inexpensive, is nontoxic, and can be prepared from readily available materials. IOCS can selectively remove strontium from solutions, even when they contain overwhelmingly higher concentrations of potentially competing cations such as Ca2+, Al3+, and Cr3+. Sr-EDTA chelates do not adsorb to IOCS. However, the interference caused by EDTA can be substantially overcome by the addition of excess Ca to the solution since Ca displaces Sr from EDTA. The adsorbed Sr can be released, and the IOCS can be regenerated by exposure to dilute acid (pH approximately 3) for short periods. The physical and adsorptive properties of the IOCS remain essentially unaltered over at least several dozens of regeneration cycles, corresponding to treatment of at least 20000 bed volumes of influent. The only byproduct of the regeneration process is a small volume of residual waste containing essentially only strontium and dilute acid.

Compostos Férricos/química , Resíduos Radioativos/análise , Dióxido de Silício/química , Estrôncio/química , Gerenciamento de Resíduos/métodos , Adsorção , Algoritmos , Ácido Edético/química , Filtração , Concentração de Íons de Hidrogênio , Quelantes de Ferro/química , Nitratos/química , Concentração Osmolar , Estrôncio/isolamento & purificação