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|標題:||Effects of C/Fe ratios, pH, and Al on the Structures of Dissolved Organic Matter-Fe Hydroxides Co-precipitates and Cr(VI) Transformations|
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|摘要:||可溶性有機質與鐵離子的共沉澱作用對於穩定土壤中的碳及鐵扮演相當重要的角色，而土壤中豐富的鋁離子會影響可溶性有機質-鐵氫氧化物共沉澱物的結構發展，此外，可溶性有機質-鐵氫氧化物共沉澱物可能成為土壤及沉積物中重金屬，如:六價鉻，重要的清除者。本篇研究的目標為探討碳鐵比、pH及鋁離子影響可溶性有機質-鐵氫氧化物共沉澱物的結構與其對六價鉻轉變，研究目的包括: (1)觀察在不同pH值及碳鐵比變化下，可溶性有機質-鐵氫氧化物共沉澱物的結構發展及穩定性；(2)瞭解鋁離子在不同pH值及鐵鋁比的影響下，對於可溶性有機質-鐵氫氧化物共沉澱物結構發展的影響；(3)檢視在不同pH值及碳鐵比的影響下，鉻在可溶性有機質-鐵氫氧化物共沉澱物上的轉移及鍵結機制。結果顯示，可溶性有機質-鐵氫氧化物共沉澱物的結構依C/(C+Fe)比大致可分類為三種: (1) 當C/(C+Fe) ≤ 0.65，可溶性有機質-鐵氫氧化物共沉澱物以類水合鐵礦的結構為主(DFC I)；(2) C/(C+Fe)介於0.71及0.89，則以類水合鐵礦與共用邊/共用角的鐵八面體連結Fe-C 鍵的混合結構為主(DFC II)；(3)當C/(C+Fe) ≥ 0.92，結構則逐漸轉變為共用角的鐵八面體連結Fe-C鍵(DFC III)。此外，添加鋁離子也會影響可溶性有機質與鐵離子在不同pH值及Fe/Al比的共沉澱行為，其可區分為五種: (1)當Fe/(Fe+Al) > 0.25及pH 3.0時，可溶性有機質-鐵氫氧化物共沉澱物為主要的物種；(2)在Fe/(Fe+Al)為0.25 及pH ≤ 4.5時，可溶性有機質上的含氧官能基會與鐵鋁均勻的分佈在共沉澱物上；(3)然而當Fe/(Fe+Al) > 0.25及pH 4.5時，形成均勻分佈帶有共用角的鐵八面體之可溶性有機質-鐵氫氧化物共沉澱物，且鐵的結構會逐漸被鋁及可溶性有機質所覆蓋；(4)當Fe/(Fe+Al) 為 0.25及pH 6.0時，生成的鋁氫氧化物被散佈的鐵八面體與可溶性有機質包埋；(5)在Fe/(Fe+Al) > 0.25 及pH 6時，可溶性有機質與鋁的鍵結可能會促進鐵核的生成。一旦可溶性有機質-鐵氫氧化物共沉澱物在土壤中生成，其可能會變成六價鉻重要的清除劑之一。然而，六價鉻在可溶性有機質-鐵氫氧化物共沉澱物上的轉移主要與C/(C+Fe)比例及溶液pH值有關，例如，當C/(C+Fe)比小於0.89時，可溶性有機質-鐵氫氧化物共沉澱物中的鐵氫氧化物可以快速的吸附六價鉻；六價鉻的還原量則與可溶性有機質含量及溶液pH值兩者有關，但是溶液pH值似乎是控制六價鉻還原的關鍵因子。可溶性有機質-鐵氫氧化物共沉澱物與六價鉻的交互作用，可依沉澱物的C/(C+Fe)比及pH值分為四種不同機制: (1) 在C/(C+Fe) ≤ 0.65，接近100 %的六價鉻吸附在DFC I結構類似水合鐵礦的表面上；(2)當C/(C+Fe)介於0.71及0.89時，鐵氫氧化物吸附六價鉻為主要的物種，而還原的產物三價鉻部分的鍵結在DFC結構上之鐵氫氧化物或是可溶性有機質的表面；(3)然而，C/(C+Fe) ≥ 0.89及pH 4.5與6.0時，大部分的六價鉻被可溶性有機質還原成三價鉻，進而吸附在DFC結構的鐵氫氧化物表面；(4)當C/(C+Fe) ≥ 0.92及pH 3.0時，還原後的三價鉻則鍵結在DFC III結構之可溶性有機質上。總結來說，本篇研究發現C/Fe比控制可溶性有機質-鐵氫氧化物共沉澱物的結構發展而碳鐵比及溶液pH值兩者均會影響與其對六價鉻的吸附/還原反應，然而，pH值可能為控制鋁離子影響碳鐵之間的結構及共沉澱反應，同時影響六價鉻在可溶性有機質-鐵氫氧化物共沉澱物之還原行為之重要因子。|
Co-precipitation of dissolved organic matter (DOM) and Fe is an important process occurring naturally that may stabilize C and Fe in the soil systems. Aluminum ions are abundant in soils, and thus, the structural developments of DOM/Fe co-precipitates (DFC) can be greatly affected by the element. In addition, the nanosized DOM/Fe co-precipitates may be a potential scavenger of heavy metals, e.g., Cr(VI), in soils and sediments. Thus, the overall goal of this research was to determine the effects of C/Fe ratios, pH, and Al ions on the structures of DOM/Fe co-precipitates and Cr(VI) transformations. The specific objectives were: (1) to determine the structural development and stabilization of DOM/Fe co-precipitates in relation to the changes of pH and C/Fe molar ratios; (2) to understand the effects of Al ions on the structural stabilization of DOM-Fe co-precipitates accompanied with the changes of pH and Fe/Al molar ratios; and (3) to examine the mechanisms of Cr bonding/transformation on DOM/Fe co-precipitates as influenced by the changes of pH and C/Fe molar ratios. Results showed that rhe local structures of DFC samples could be classified into three categories depending on the molar ratios of C/(C+Fe): (1) the ferrihydrite-like domain with the C/(C+Fe) molar ratios ≤ 0.65 (DFC structure I); (2) the mixtures of the edge/corner-sharing FeO6 octahedra associated with Fe-C bonds and ferrihydrite-like domains with the C/(C+Fe) molar ratios between 0.71 and 0.89 (DFC structure II); and (3) the corner-sharing FeO6 octahedra associated with Fe-C bonds with the C/(C+Fe) molar ratios ≥ 0.92 (DFC structure III). Additionally, influences of Al ions on the co-precipitation behaviors of DOM and Fe in relation to the changes of pH and Fe/Al ratios were categorized into five types : (1) DOM/Fe co-precipitates were the dominant species with a Fe/(Fe+Al) molar ratios > 0.25 at pH 3.0; (2) the O-containing groups of DOM homogenously associated with Fe(III) and Al domains of co-precipitates with a Fe/(Fe+Al) molar ratio of 0.25 at pH ≤ 4.5; (3) the mixtures of homogeneous distributions of DOM/Fe co-precipitates with a smaller size of Fe domain, and the Fe domain was gradually covered by Al domains and DOM molecules with Fe/(Fe+Al) molar ratios > 0.25 and at pH 4.5; (4) Al hydroxides covered by the homogeneous distributions of DOM and FeO6 with a Fe/(Fe+Al) molar ratio of 0.25 at pH 6.0; and (5) when the Fe/(Fe+Al) molar ratios > 0.25 at pH 6.0, the association between Al domains and DOM may promote the formation of Fe core. Once the DFC was formed in soil, it became an important scavenger of Cr(VI). However, Cr(VI) transformations on the DFC depend greatly on the C/(C+Fe) molar ratios and solution pH. For instance, the Fe domains of the DFC adsorbed rapidly Cr(VI) when the bulk C/(C+Fe) molar ratios of DFC were less than 0.89. The amounts of Cr(VI) reductions were related to both DOM contents and solution pH, but the pH seemed to be the key factor of controlling Cr(VI) reduction. The reactive mechanisms of Cr(VI) with DFC could be grouped into four types depending on C/(C+Fe) molar ratios and pH values: (1) Nearly 100% of Cr(VI) were associated with ferrihydrite-like domains of DFC with the bulk C/(C+Fe) molar ratios ≤ 0.65; (2) The Fe hydroxides-Cr(VI) was the dominant species of Cr, and the reductive products of Cr(III) were associated with Fe hydroxides or DOM when the bulk C/(C+Fe) molar ratios were between 0.71 and 0.89; (3) With C/(C+Fe) molar ratios ≥ 0.89, Cr(VI) was reduced by DOM and then associated with Fe(III) hydroxides at pH 4.5 and 6.0; and (4) At pH 3.0 and the C/(C+Fe) molar ratios ≥ 0.92, the DOM-Cr(III) complexes became the dominant Cr species. In general, the studies show that C/Fe molar ratios control the structural developments of DFC, and both of C/Fe molar ratios and solution pH affect adsorption/reduction reactions of Cr(VI) on DFC. However, the pH may be a key factor of controlling the formation of DFC in the presence of Al ions and regulating Cr(VI) reduction behavior on DFC.
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