Elsevier

Chemosphere

Volume 198, May 2018, Pages 556-564
Chemosphere

EDDS enhanced Shewanella putrefaciens CN32 and α-FeOOH reductive dechlorination of carbon tetrachloride

https://doi.org/10.1016/j.chemosphere.2018.01.083Get rights and content

Highlights

  • Bio-reduction of α-FeOOH was attributed to strong complexation ability of EDDS.

  • Surface of α-FeOOH were looser due to EDDS form complexes with Fe (III).

  • Combination between EDDS and Fe2+ produced triple bondFeIIEDDS complex.

  • triple bondFeIIEDDS has low reductive potential to enhance dechlorination rate of CT.

Abstract

S,S-ethylenediamine-N,N-disuccinic acid (EDDS) enhanced reductive dissolution of α-FeOOH by Shewanella putrefaciens CN32 (CN32), resulting in formation of surface-bound Fe(II) species (triple bondFeIIEDDS) to improve reductive dechlorination of carbon tetrachloride (CT). The pseudo-first-order rate constants for bio-reduction extents of α-FeOOH by CN32 in the presence of 1.36 mM EDDS was 0.023 ± 0.0003 d−1 which was higher than without EDDS. The enhancement mechanism of bio-reduction was attributed to the strong complexation ability of EDDS to formed triple bondFeIIIEDDS, which could be better utilized by CN32. The dechlorination kinetic of CT by triple bondFeIIEDDS (2.016 h−1) in the presence of 1.36 mM EDDS was 24 times faster than without EDDS. Chloroform were detected as main products for the degradation of CT. The chemical analyses and morphological observation showed that combination between EDDS and Fe2+ produced triple bondFeIIEDDS complex, which had a reductive potential of −0.375 V and significantly enhanced CT dechlorination. The results showed that EDDS played an important role in enhancing the bio-reduction of α-FeOOH to accelerate reductive dechlorination of CT.

Introduction

It has reported that microbial reduction of iron oxides by dissimilatory iron-reducing bacteria (DIRB) has been acknowledged as a significant process in anaerobic environments (Li et al., 2010, Bae and Lee, 2012). It was generally believed that there were two mechanisms for electron transfer between bacterial cells and Fe (III) surfaces: through ligands which solubilize Fe(III) by complex formation; by redox cycling of electron shuttle between the bacterial cell and Fe(III) surface (Esther et al., 2014). The bio-reduction rate and extent of Fe(III) oxide was influenced by many factors, for example, the composition of the culture medium; availability; surface area and crystallinity; microbial community structure and biomass; and the adsorption affinity with iron oxides and bacteria (Glasauer et al., 2001).

Available literature provided evidence that the rate of bio-reduction was higher for amorphous Fe(III) than crystalline Fe(III) (Eric E. Roden and Zachara†, 1996). The decrease in bio-reduction rate of Fe(III) oxide could be attributed to the adsorption or precipitation of accumulation Fe(II) which blocking reaction dissolution sites of Fe(III) oxides (Royer et al., 2004). Delaying in sorption or precipitation of surface-bound Fe(II) could further accelerate the bio-reduction of Fe(III) oxide to form surface-bound iron species (Royer et al., 2002). Attempts were made to add ligands such as citric acid complexes agent, EDTA and NTA, followed by its solubilization on the oxide surface or the biological Fe(II), keeping Fe2+ in soluble form and thereby preventing Fe2+ adsorption (Taillefert et al., 2007, Manzella et al., 2013). In addition, the formation of Fe-ligand complexes affected the redox potential of the Fe2+/Fe3+ which was direct relevance to the remediation of contaminated environmental systems (Song et al., 2017).

Despite the fact that previous study reported the dissolution of Fe(II) can be combined with the polycarboxylic acid on the surface of the iron oxide to form surface bound Fe(II) (adsorbed Fe(II)–polycarboxylic ligand complexation) (Roden, 2004), however the mechanism of formation surface bound Fe(II) (Fe(II)–ligand complexation) on the surface of the iron oxide was still unknown. It was also known that carboxylic acid such as ethylenediamine tetra acetic acid (EDTA) could prevent iron precipitation even at neutral pH. However, the widespread use of EDTA might lead to some undesirable environmental consequences because of its poor biodegradability and strong heavy metal chelating capacity (Englehardt et al., 2007, Prieto et al., 2013). Recently, (S,S)-N,N0-ethylenediamine disuccinic acid (EDDS), as a structural isomer of EDTA, has been successfully applied to the remediation of heavy metal contaminated soils instead of traditional chelating agents such as EDTA or NTA (Attinti et al., 2017, Beiyuan et al., 2017). One of the main advantages of EDDS that has enhanced its use for soil washing of potentially toxic metals in contaminated soils is certainly its biodegradability (Meers et al., 2005, Leštan et al., 2008). Iron-reducing reaction has recently been recognized as an important process under anaerobic conditions, especially in Fe-bearing soil. So the widely application of EDDS may affect the iron reduction process in contaminated sites. Although previous study considered the interactions between EDDS and soil minerals (Yip et al., 2009), However, to date, there are few studies reported that EDDS improve bio-reduction efficiency of iron oxides by DIRB and stimulate the generation of surface-bound Fe(II). Several studies have reported the importance of surface-bound iron species to the abiotically reductive transformation of chlorinated hydrocarbons (Tobler et al., 2007, Maithreepala and Doong, 2009). So the addition of EDDS may also effect the removal of chlorinated hydrocarbons in contaminated sites.

In this research, α-FeOOH and Shewanella putrefaciens CN32 (CN32) were selected as mineral and DIRB to investigate the mechanism of EDDS enhance the bio-reduction of mineral in anaerobic environments. The objectives of this study was to characterize the generation of surface-bound Fe(II) (triple bondFeIIEDDS) during the bio-reduction of α-FeOOH by CN32 when addition of EDDS, to investigate the role of triple bondFeIIEDDS during the reductive dechlorination of chlorinated organic. Carbon tetrachloride (CT) was selected as a representative target chlorinated organic which classified as potential carcinogens and caused toxicity to human beings and ecosystems (Bae et al., 2017).

Section snippets

Chemicals

CT (>99.8%, GC grade), chloroform (CF) (>99.8%, GC grade), dichloromethane (DCM) (>98%, GC grade) and chloromethane (CM) (>98%, GC grade) were purchased from Aladdin Biochemical Technology Co. Ltd (Shanghai, China). EDTA (C10H16N2O8, 99%), EDDS (C10H16N2O8, >98%) and Sodium lactate (C3H5NaO3, 99%) were purchased from Kuer Chemical Technology Co. Ltd (Beijing, China). All the other chemicals were of analytical grade and were used as received without further purification. α-FeOOH was synthesized

EDDS enhanced bio-reduction of α-FeOOH by CN32

Bio-reduction of 10 mM α-FeOOH (0.56 g-Fe L−1) by CN32 in the presence of various concentrations EDDS or EDTA at neutral pH was characterized by measuring the concentration of dissolved Fe(II) (Fig. 1). The concentrations of Fe(II) significantly increased in the presence of various concentrations EDTA or EDDS with CN32 in 15 d, while no increase of Fe(II) was observed in the controls. The concentration of Fe(II) in α-FeOOH suspension without CN32 was low due to its slow dissolution rate and/or

Conclusion

EDDS as a new type of environmentally friendly chelating agent, have been used for contaminant degradation purposes in the recently published works, especially in removal of heavy metal ions in contaminated sites (Kowalczyk et al., 2013, Cui et al., 2017). In this study, it found that addition EDDS significantly enhanced the production of dissolved and sorbed Fe(II) after incubation due to EDDS has strong complexation abilities to combine with iron oxides. The reductive dechlorination of CT can

Acknowledgements

This work was supported jointly by the National key research and development plan (2016YFC0206200), the National Natural Science Foundation of China (51578240), the Fok Ying Tung Education Foundation (141077), Open Foundation of State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences (SKLECRA2016OFP19), Open Foundation of Shanghai Key Lab for Urban Ecological Processes and Eco-Restoration, and the Innovation Program of the Shanghai

References (45)

  • S.O. Lee et al.

    Dissolution of iron oxide using oxalic acid

    Hydrometallurgy

    (2007)
  • L. Legrand et al.

    The oxidation of carbonate green rust into ferric phases:solid-state reaction or transformation via solution 1

    Strabismus

    (2004)
  • D. Leštan et al.

    The use of chelating agents in the remediation of metal-contaminated soils: a review

    Environ. Pollut.

    (2008)
  • Y.L. Li et al.

    Iron reduction and alteration of nontronite NAu-2 by a sulfate-reducing bacterium 1

    Geochem. Cosmochim. Acta

    (2004)
  • F. Li et al.

    Enhancement of the reductive transformation of pentachlorophenol by polycarboxylic acids at the iron oxide-water interface

    J. Colloid Interface Sci.

    (2008)
  • F.B. Li et al.

    Enhanced reductive dechlorination of DDT in an anaerobic system of dissimilatory iron-reducing bacteria and iron oxide

    Environ. Pollut.

    (2010)
  • Y.S. Li et al.

    Infrared and Raman spectroscopic studies on iron oxide magnetic nano-particles and their surface modifications

    J. Magn. Magn. Mater.

    (2012)
  • C. Liang et al.

    pH dependence of persulfate activation by EDTA/Fe(III) for degradation of trichloroethylene

    J. Contam. Hydrol.

    (2009)
  • R.A. Maithreepala et al.

    Transformation of carbon tetrachloride by biogenic iron species in the presence of Geobacter sulfurreducens and electron shuttles

    J. Hazard. Mater.

    (2009)
  • E. Meers et al.

    Comparison of EDTA and EDDS as potential soil amendments for enhanced phytoextraction of heavy metals

    Chemosphere

    (2005)
  • C. Prieto et al.

    Enhancing radium solubilization in soils by citrate, EDTA, and EDDS chelating amendments

    J. Hazard. Mater.

    (2013)
  • E.E. Roden

    Analysis of long-term bacterial vs. chemical Fe(III) oxide reduction kinetics

    Geochem. Cosmochim. Acta

    (2004)
  • Cited by (12)

    • Synthesis of zero-valent iron supported with graphite and plastic based carbon from recycling spent lithium ion batteries and its reaction mechanism with 4-chlorophenol in water

      2023, Journal of Environmental Management
      Citation Excerpt :

      Chlorophenols are widely used in the formulation of wood preservatives, coatings, plant fibers and leather as well as in the fungicide manufacturing industry (Wang et al., 2022). They are also used as intermediates or raw materials in the production of pesticides, fungicides, pharmaceuticals and dyes (Zhou et al., 2018; Garba et al., 2020). In addition, chlorophenols can be produced in waste incineration, chlorine bleaching of pulp, and dechlorination of drinking water (Olaniran and Igbinosa, 2011).

    • Rapid biodegradation of chlorpyrifos by plant growth-promoting psychrophilic Shewanella sp. BT05: An eco-friendly approach to clean up pesticide-contaminated environment

      2020, Chemosphere
      Citation Excerpt :

      Shewanella sp. is typical environmental Gram-negative bacteria widespread in fresh water and marine eco-system in warm climates and is rarely pathogenic. It is well known genus for their potential removal of metals and dyes (Zhou et al., 2018; Liu et al., 2018). Therefore, current investigation was centered on the utilization of psychrophilic Shewanella sp. for the biodegradation of CPs.

    • Utilization of formic acid in nanoscale zero valent iron-catalyzed Fenton system for carbon tetrachloride degradation

      2020, Chemical Engineering Journal
      Citation Excerpt :

      This might be due to the rapid transformation of intermediates to inorganic ones under the attack of HO and CO2− radicals, or because of their extremely low concentration. Based on the previous work [15,18] and literatures [43,44], CT degradation likely takes place as follows: The C-Cl bond of CT is firstly split by CO2− radical to yield CCl3, after that CCl3 could either go hydrogen abstraction to form HCCl3 or further be reduced to dichlorocarbene. Dichlorocarbene was easily dechlorinated and hydrolyzed to yield CO2 and Cl−.

    View all citing articles on Scopus
    View full text