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And Shewanella Putrefaciens Surfaces in the Presence of As(V) Using Extended X-Ray Absorption Fine Structure Spectroscopy

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And Shewanella Putrefaciens Surfaces in the Presence of As(V) Using Extended X-Ray Absorption Fine Structure Spectroscopy American Journal of Innovative Research and Applied Sciences. ISSN 2429-5396 I www.american-jiras.com ORIGINAL ARTICLE INVESTIGATING THE MECHANISMS OF U(VI) SORPTION ONTO FE(0) AND SHEWANELLA PUTREFACIENS SURFACES IN THE PRESENCE OF AS(V) USING EXTENDED X-RAY ABSORPTION FINE STRUCTURE SPECTROSCOPY 1* | Clement N’zau Umba-di-Mbudi | 1. Université de Kinshasa | Département de geosciences | Groupe Geo-Hydro-Energie | Kinshasa, RD Congo | | Received May 19, 2020 | | Accepted May 26, 2021 | | Published June 01, 2021 | | ID Article | Clement-Ref6-ajira210521| ABSTRACT Background: Sorption processes control the mobility, biodisponibility, bio-transformation, speciation and ultimately the toxicity of metals and metalloids in the subsurface. Methods: This paper analyses the electronic and geometric structure of solid samples of uranium onto scrap metallic iron and the versatile bacterium Shewanella putrefaciens surfaces in the presence of arsenic by means of U L3 and As K- edge extended X-ray absorption fine structure (EXAFS) measurements prepared by batch sorption experiments. Results: This analysis complements a companion XANES fingerprinting investigation both aiming at uncovering the underlying major mechanism controlling the state of the uranium atoms. The sorption experiment samples comprise of the systems Fe(0)- 0.1 mM U, Fe(0)-0.1 mM U-0.1 mM As and the anoxic Fe(0)-0.1 mM U-0.1 mM As-DSMZ Shewanella putrefaciens strain 6067 at concentration of two optical density units (600 nm) equilibrated for 24 hours in the dark without shaking. EXAFS spectra evaluation confirms the presence and prevalence of respectively U(VI)-O/O-OH axial and equatorial bonds in the mono-component uranium system and both U(VI)-O/O-OH and tetrahedron As(V)-(O,OH) in the bi-components uranium–arsenic systems sorbed onto scrap metallic iron and Shewanella putrefaciens surfaces. Conclusion: The absence of peaks beyond the major axial and equatorial U(VI)-O/O-OH bonds in the mono-component uranium system and the concurrent occurrence of U(VI)-O/O-OH and As(V)-(O,OH) bonds in the bi-component uranium-arsenic systems suggest the likely plausibility of precipitation/co-preciptation mechanism as the leading control of uranium behavior. Keywords: sorption, uranium, arsenic, XAFS, modeling, iron, bacteria. 1. INTRODUCTION Sorption processes control the mobility, biodisponibility, bio-transformation, speciation and ultimately the toxicity of metals and metalloids in the subsurface [1, 2, 3]. They play a capital role in contaminant hydrogeology, reactive transport and site remediation. Thus, a sound understanding and prediction of the specific sorption mechanisms regulating the fate of contaminants of concerns such as uranium and arsenic in the subsurface is paramount in the design of a remediation technology such as a permeable reactive barrier. Uranium and arsenic sorption onto metallic iron and corrosion products as well as onto bacteria surfaces have gained much interest among environmental technologists, scientists and engineers owing partly to the former strong redox potentials and the latter high surface area. Besides, over the last decades, some bacteria have been recognized as uranium and arsenic scavengers. For instance, dissimilatory Fe(III) reducing bacteria such as Geobacter metallireducens and Shewanella putrefaciens have gained attention owing to their capability to couple the oxidation of organic matter to the reduction of Fe(III) and alternatively various metals/metalloids including uranium and arsenic [4, 5]. However, conditions that can inhibit these often presented as enzymatically driven biotransformation processes are still not well known. As aforementionned, for a contaminated site remediation engineer perspective, a good understanding of the binding mechanisms of uranium and arsenic onto metallic iron and corrosion products as well as onto bacteria surfaces is a key design input for an effective dimensioning and operation of an efficient reactive barrier. To date, however, the mechanistic description of uranium sorption onto metallic iron has been based on hypotheses that include either reductive precipitation induced by elemental Fe(O), structural Fe(II) or even H2, chemisorption at the surfaces of Fe(O) and corrosion products, precipitation/co-precipitation, or their combination [6,7,8,9,10,11]. Similarly, arsenic sorption onto elemental iron and corrosion products has also been reported either as co-precipitation of the reduced As (III) from As (V) or as adsorption of both As (V) and As (III) on iron corrosion products or other pre-existent oxyhydroxides [12, 13, 14]. Among the large array of interfacial investigation techniques, extended x-ray absorption fine structure (EXAFS) spectroscopy is well suited to elucidate the coordination chemistry and ultimately to better comprehend the binding mechanism of uranium onto elemental iron and corrosion products, and bacteria surfaces in the presence of arsenic. Noteworthy however, despite the well-established EXAFS efficiency in uncovering the binding mechanisms of metals/metalloids on environmental solids [15] (Brown 1990), yet studies trying to decipher uranium fixation onto solids in the presence of arsenic are scarce. Denecke et al., (2005) used EXAFS techniques to assess the mechanisms *Corresponding author Author & Copyright Author © 2021: | Clement N’zau Umba-di-Mbudi *|. All Rights Reserved. All articles published in American Journal of 231 Innovative Research and Applied Sciences are the property of Atlantic Center Research Sciences, and is protected by copyright laws CC-BY. See: http://creativecommons.org/licenses/by- nc/4.0/. American Journal of Innovative Research and Applied Sciences. ISSN 2429-5396 I www.american-jiras.com that led to the immobilization of uranium in tertiary sediment from a waste disposal natural analogue site in the presence of arsenic either as As(V) or As(0) [16]. Mbudi et al., (2007) discussed the speciation of uranium and arsenic sorbed onto scrap metallic iron and Shewanella putrefaciens surfaces based on x-ray absorption near edge structure (XANES) fingerprinting investigation [19]. This investigation focuses on uncovering the coordination chemistry of uranium and arsenic sorbed onto scrap metallic iron and corrosion products and Shewanella putrefaciens surfaces prepared in no growth and ultimately on conditions that potentially inhibit these bacteria enzymatic capabilities to biotransform uranium and arsenic. To this end, this analysis applies ab initio calculations and least square fitting routines to model bulk EXAFS spectra from batch experiments systems that equilibrated uranium alone with scrap metallic iron, uranium with arsenic in contact with scrap metallic iron and bi-component water containing uranium and arsenic onto scrap metallic iron and Shewanella putrefaciens cells. The coordination chemistries and hence fixation mechanisms of both uranium and arsenic are assessed and compared in these three systems with the ultimate goal of uncovering the influence of arsenic and bacteria on the fate of uranium under experimental conditions. 2. MATERIELS AND METHODES 2.1 Materials Uranyl nitrate 6-hydrate UO2(NO3)2.6H20 (Chemapol, Germany) and sodium arsenate Na2HAsO4.7H20 (Baker, Germany) of analytical grade were used to prepare stock solutions of uranium and arsenic. The reagents used for bacterium growth include yeast extract (Roth, Germany), peptone (VEB Berlin Chemie, Germany) and NaCl (Riedel- de-Haen, Germany). The background electrolyte used in every experiment was prepared from sodium nitrate from Merk (Germany) dissolved in deionized water with a Milli-Q Water Purification System (Millipore, France). The scrap metallic iron type S69 from Metallaufbereitung Zwickau (Germany) was crushed and sieved. The homogeneous 0.1 mm fraction was used as sorbent. The elemental composition of the selected scrap metallic iron used throughout is 92.8% Fe, 3.5% C, 2.1% Si, 0.9% Mn and 0.7% Cr. 2.2 Bacteria Culturing and Harvesting The Shewanella putrefaciens bacterium referred to as strain 6067 was purchased as dried culture from Deutsche Sammlung von Mikroorganismen und Zellkulturen GmbH (DSMZ). The strain was resuscitated following routine DSMZ protocol and the active stock was thereafter used to inoculate a Petri dish containing yeast extract, peptone and agar, and incubated at room temperature (about 23oC). Cells culturing was carried out aerobically at similar ambient temperature using a set of 250 ml glass Erlenmeyer filled with 100 ml of the growth medium and inoculated with a loopful of Shewanella putrefaciens colonies from Petri dish. The growth medium comprised 2 g/l yeast extract, 5 g/l peptone and 5 g/l NaCl adjusted to pH 7 with NaOH prior to sterilization. The culture vessels were put on a shaker and incubated at room temperature until the late exponential growth phase. Cells harvesting was achieved through centrifugation at 7000 g for 15 minutes at a temperature of 10oC. The harvested cells were washed twice using a sterile and anoxic 0.01 M KOH solution. The re-suspension of the washed pellets was carried out in anoxic 0.01 M NaNO3 background electrolyte solution of the biotic batch sorption experiment reaction vessel. 2.3 Batch Sorption Experiments Two samples representing the reacted solid phase from the experimental design systems Fe(0)-0.1 mM U and Fe(0)- 0.1 mM U-0.1 mM As were prepared abiotically using 100 ml polyethylene reaction vessels. Each reaction vessel contained 2 g of 0.1 mm particulate sized scrap metallic iron set to equilibrate in a solid to solution ratio (weight/weight) of 1/50 using a background electrolyte solution of 0.01 M NaNO3 spiked respectively with uranium 0.1 mM U alone or with the bi-component 0.1 mM U-0.1 mM As adjusted in either case at pH 4.5. A third sample was prepared from a biotic batch sorption experiment of the system Fe(0)-0.1 mM U-0.1 mM As-bacteria cells. The solutions used in this system were adjusted at pH 4.5 and purged with high purity nitrogen gas prior to sterilization. A 75 ml glass bottle capped with rubber crimped with an aluminium seal as the reaction vessel.
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