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Abundance and fractionation of Al, Fe and trace metals following tidal inundation of a tropical acid sulfate soil

- Johnston, Scott, Burton, Edward, Bush, Richard, Keene, Annabelle, Sullivan, Leigh, Smith, Douglas, McElnea, Angus, Ahern, Col, Powell, Bernard

  • Authors: Johnston, Scott , Burton, Edward , Bush, Richard , Keene, Annabelle , Sullivan, Leigh , Smith, Douglas , McElnea, Angus , Ahern, Col , Powell, Bernard
  • Date: 2010
  • Type: Text , Journal article
  • Relation: Applied Geochemistry Vol. 25, no. 3 (2010), p. 323-335
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  • Description: Tidal inundation was restored to a severely degraded tropical acid sulfate soil landscape and subsequent changes in the abundance and fractionation of Al, Fe and selected trace metals were investigated. After 5 a of regular tidal inundation there were large decreases in water-soluble and exchangeable Al fractions within former sulfuric horizons. This was strongly associated with decreased soil acidity and increases in pH, suggesting pH-dependent immobilisation of Al via precipitation as poorly soluble phases. The water-soluble fractions of Fe, Zn, Ni and Mn also decreased. However, there was substantial enrichment (2-5×) of the reactive Fe fraction (FeR; 1 M HCl extractable) near the soil surface, plus a closely corresponding enrichment of 1 M HCl extractable Cr, Zn, Ni and Mn. Surficial accumulations of Fe(III) minerals in the inter-tidal zone were poorly crystalline (up to 38% FeR) and comprised mainly of schwertmannite (Fe8O8(OH)6SO4) with minor quantities of goethite (α-FeOOH) and lepidocrocite (γ-FeOOH). These Fe (III) mineral accumulations provide an effective substrate for the adsorption/co-precipitation and accumulation of trace metals. Arsenic displayed contrary behaviour to trace metals with peak concentrations (∼60 μg g-1) near the redox minima. Changes in the abundance and fractionation of the various metals can be primarily explained by the shift in the geochemical regime from oxic-acidic to reducing-circumneutral conditions, combined with the enrichment of reactive Fe near the soil surface. Whilst increasing sequestration of trace metals via sulfidisation is likely to occur over the long-term, the current abundance of reactive Fe near the sediment-water interface favours a dynamic environment with respect to metals in the tidally inundated areas. © 2009 Elsevier Ltd. All rights reserved.

Arsenic mobilization during seawater inundation of acid sulfate soils - Hydrogeochemical coupling at the tidal fringe

- Johnston, Scott, Burton, Edward, Keene, Annabelle, Bush, Richard, Sullivan, Leigh

  • Authors: Johnston, Scott , Burton, Edward , Keene, Annabelle , Bush, Richard , Sullivan, Leigh
  • Date: 2012
  • Type: Text , Conference proceedings
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  • Description: Coastal Acid Sulfate Soils (CASS) are rich in meta-stable iron (Fe - III) minerals that are important sorbents for arsenic (As) under oxic conditions. Tidal seawater inundation to remediate CASS has recently been trialed on a large scale and has potential to mobilize arsenic during the redox transition. Tidal seawater inundation caused reductive dissolution of As(V)-bearing Fe(III) minerals, resulting in elevated concentrations of Fe 2+ (2000 mg L -1) and As (∼400 μg L -1) in upper-intertidal zone groundwater. Oscillating vertical and horizontal hydraulic gradients caused by tidal pumping promoted upward advection of As and Fe 2+-enriched groundwater within the intertidal zone. This led to flux of As aq and Fe 2+ aq to surface waters and the accumulation of As(V)-enriched Fe(III) (hydr)oxides at the oxic sediment-water interface. Fe(III) (hydr)oxides at the sediment-water interface act as a natural reactive-barrier, retarding As flux to overlying surface waters. However, they also represent a highly transient phase that is prone to reductive dissolution during future redox boundary migration. A conceptual model is presented to explain landscape-scale patterns of As and Fe hydro-geochemical zonation. © 2012 Taylor & Francis Group.

Tidally driven water column hydro-geochemistry in a remediating acidic wetland

- Johnston, Scott, Keene, Annabelle, Bush, Richard, Sullivan, Leigh, Wong, Vanessa

  • Authors: Johnston, Scott , Keene, Annabelle , Bush, Richard , Sullivan, Leigh , Wong, Vanessa
  • Date: 2011
  • Type: Text , Journal article
  • Relation: Journal of Hydrology Vol. 409, no. 1-2 (2011), p. 128-139
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  • Description: Managed tidal inundation is a newly evolved technique for remediating coastal acid sulphate soil (CASS) wetlands. However, there remains considerable uncertainty regarding the hydro-geochemical pathways and spatiotemporal dynamics of residual H+ and metal(loid) mobilisation into the tidal fringe surface waters of these uniquely iron-rich landscapes. Here, we examine the hydrology and water column chemistry across the intertidal slope of a remediating CASS wetland during several tide cycles. There was extreme spatial and temporal dynamism in water column chemistry, with pH fluctuating by ∼3 units (∼3.5-6.5) during a single tide cycle. Acute acidity was spatially confined to the upper intertidal slope, reflecting surface sediment properties, and tidal overtopping is an important pathway for mobilisation of residual H+ and Al3+ to the water column. Marine derived HCO3- was depleted from surface waters migrating across the intertidal slope and a strong gradient in HCO3- was observed from the tidal fringe to the adjacent tributary channel and nearby estuary. Tidal forcing generated oscillating hydraulic gradients in the shallow fringing aquifer, favouring ebb-tide seepage and driving rapid, heterogeneous advection of groundwater on the lower intertidal slope via surface connected macropores. A combination of diffusive and advective flux across the sediment-water interface led to persistent, elevated surface water Fe2+ (∼10-1000μM). The geochemical processes associated with Fe2+ mobilisation displayed distinct spatial zonation, with low pH, proton-promoted desorption occurring on the upper intertidal slope, whilst circum-neutral pH, Fe(III)-reducing processes dominated the lower intertidal slope. Arsenic was also mobilised into surface waters on the lower intertidal slope under moderate pH (∼6.0) conditions and was strongly positively correlated with Fe2+. Saturation index values for aragonite were substantially depressed (-1 to -5) and significantly negatively correlated with elevation, thereby presenting a barrier to re-colonisation of the upper intertidal slope by calcifying benthic organisms. These findings highlight the spatially complex hydrological and geochemical controls on surface water quality that can occur in tidally inundated acid sulphate soil environments. © 2011 Elsevier B.V.

Arsenic mobilization in a seawater inundated acid sulfate soil

- Johnston, Scott, Keene, Annabelle, Burton, Edward, Bush, Richard, Sullivan, Leigh, McElnea, Angus, Ahern, Col, Smith, C. Douglas, Powell, Bernard, Hocking, Rosalie

  • Authors: Johnston, Scott , Keene, Annabelle , Burton, Edward , Bush, Richard , Sullivan, Leigh , McElnea, Angus , Ahern, Col , Smith, C. Douglas , Powell, Bernard , Hocking, Rosalie
  • Date: 2010
  • Type: Text , Journal article
  • Relation: Environmental Science and Technology Vol. 44, no. 6 (2010), p. 1968-1973
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  • Description: Tidal seawater inundation of coastal acid sulfate soils can generate Fe- and SO4-reducing conditions in previously oxicacidic sediments, This creates potential for mobilization of As during the redox transition. We explore the consequences for As by investigating the hydrology, porewater geochemistry, solid-phase speciation, and mineralogical partitioning of As across two tidal fringe toposequences. Seawater inundation induced a tidally controlled redox gradient. Maximum porewater As (∼400μg/L) occurred in the shallow (<1 m), intertidal, redox transition zone between Fe-oxidizing and SO 4-reducing conditions. Primary mechanisms of As mobilization include the reduction of solid-phase As(V) to As(III), reductive dissolution of As(V)-bearing secondary Fe(III) minerals and competitive anion desorption. Porewater As concentrations decreased in the zone of contemporary pyrite reformation, Oscillating hydraulic gradients caused by tidal pumping promote upward advection of As and Fe2+-enriched porewater in the intertidal zone, leading to accumulation of As(V)-enriched Fe(III) (hydr)oxides at the oxic sediment-water interface. While this provides a natural reactive-Fe barrier, it does not completely retard the flux of porewater As to overtopping surface waters. Furthermore, the accumulated Fe minerals may be prone to future reductive dissolution, A conceptual model describing As hydro-geochemical coupling across an intertidal fringe is presented. © 2010 American Chemical Society.
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