Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/28150
標題: 受污染農業環境重金屬(鉻、銅、鋅、鎳、鉛、鎘)之物種分佈及轉化研究
A study of the distribution and the transformation of metal speciation in contaminated agro-environment exemplified by Cr, Cu, Zn, Ni, Pb, and Cd
作者: 傅威程
Fu, Wei-Cheng
關鍵字: Sequential extraction procedure;連續萃取法;Synchrotron radiation;Metal;Speciation;Soil;Sediment;Suspended particulates;同步輻射;金屬;物種;土壤;底泥;懸浮微粒
出版社: 土壤環境科學系所
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摘要: 
土壤受重金屬污染為環境重要議題之ㄧ,傳統對於重金屬污染評估主要係以重金屬總量濃度為基準,惟近年來許多文獻指出重金屬對環境生態風險評估及後續整治方法之應用,除需掌握總量濃度外,應進一步探究重金屬物種分佈(speciation)。農田土壤重金屬污染推斷其源自於灌溉渠道,重金屬由污染源排放至渠道後,經灌溉作業進入農地之傳輸途徑及其重金屬污染物之型態、物種轉變及移動機制為何,尚未深入了解。因此本篇研究目的為利用修改之Tessier連續萃取法及同步輻射X光吸收光譜(鉻)探討污染場址農田土壤、渠道底泥及懸浮微粒之重金屬(鉻、銅、鋅、鎳、鉛、鎘)物種分佈。研究地點為台灣中部受污染之農地及其渠道,樣品採集包括灌溉渠道之底泥、懸浮微粒與農地土壤之表土(Topsoil, 0 - 15 cm)、裏土(Sub-soil, 15 - 30 cm),上述採集樣品皆經室溫風乾、研磨、過篩 (100 mesh篩網,0.149 mm)後以聚乙烯袋儲存備用。連續性萃取技術主要參考Tessier(1979)建議之方法,萃取型態大致可分為:可交換態、碳酸鹽結合態、鐵-錳氧化物結合態、有機物結合態及殘留態五個型態。由於溶解、沉澱和吸附等現象,致使金屬於農業環境傳輸過程中經歷許多變化。從目前研究結果得到下述結論:(1) 五污染場址之王水全量濃度,鉻、銅、鋅、鎳、鉛及鎘分析結果可觀察出,渠道樣品與農地土壤樣品於金屬間有高的皮爾森相關性。 (2) 五污染場址之入水口至出水口農田土壤樣品,其全量濃度分析結果顯示,金屬的濃度會隨灌溉距離及剖面深度之增加而減低。 (3) 五污染場址之入水口至出水口農田土壤樣品,鉻、銅、鋅、鎳、鉛及鎘的鐵-錳氧化物結合態,有57 %的數據顯示其相對百分比趨勢之變化隨著距離的增加而逐漸降低;而殘留物結合態有70%的數據與其反之。 (4) 偏態係數結果顯示五場址所有金屬總濃度皆為非常態分佈,其為正偏態(57%數據為強偏態分配),因此農田土壤污染現象為非均質。 (5) 上述四點結論可推估農田土壤污染之來源,可能為底泥或懸浮微粒透由灌溉模式,將固相微粒輸入至農田土壤中,以致於農田污染濃度會隨灌溉距離有所差異。 (6) XANES結果得知場址A之渠道底泥及六價鉻土壤吸附樣品,無六價鉻K edge之特徵波峰。由前人文獻得知環境土壤中,存在二價鐵、硫化物、亞硫酸鹽及有機物,會使六價鉻還原成三價鉻(Pettine and Capri, 2005)。故推斷本研究土壤樣品中,重金屬鉻為以三價型態存在,三價鉻對環境及生物體較無毒性。 (7) 金屬之生物有效性、毒性及移動性,可由物種分析的可交換態及碳酸鹽結合態加總去評估。由場址A灌溉渠道底泥之鉻金屬物種結果顯示,可交換態與碳酸鹽結合態兩者加總所佔百分比只有0.05 %,可瞭解鉻金屬的生物有效性、毒性及移動性相當低,與同步輻射之結果相同。 (8) 入水口之0.-15 cm土壤與15-30 cm土壤的鉻金屬型態或物種組成分佈相近,而土壤剖面樣品與底泥之鉻金屬型態或金屬物種差異甚大。其可能為金屬與底泥粒子或土壤粒子鍵結後,因為底泥處於厭氧環境,而土壤處於乾濕交替的環境下至使金屬之物種有所差異。

Recently, the relationship between the heavy metals pollution of the irrigation soil and the sediment from the irrigation channel has drawn great attentions from the scientific communities. Traditionally, heavy metal pollutions are assessed by total extraction. Since the toxicity of a metal depends more on its chemical forms than on its total amount, determination of metal speciation is essential to evaluate metal toxicity in the environment. It has been speculated that irrigation water is the major source of metal contamination on agricultural soils.However, no information is available on the transformations of heavy metals, variations in metal speciation, and transport mechanisms between the sediment of the irrigation channel and the soil of the farm land. This research was intended to assess the speciation of heavy metals (Cr, Cu, Zn, Ni, Pb, and Cd) in soils, sediments and suspended particulate of contamination sites. Two experiments, the sequential extraction procedure and synchrotron radiation (Cr), were conducted to assess the behavior of contamination. Sediments and suspended particulate of irrigation channel, and agricultural soils were collected from sites in Central Taiwan in polyethylene bags. The samples were immediately air dried and stored in the laboratory before further study. Large debris such as stones and plant fragments were removed from the dried samples by screening using 0.149-mm sieve. The metal extraction procedure was modified from that proposed by Tessier. The sequential extraction produced five fractions: exchangeable, carbonate, Fe-Mn oxides, organic material, and silicate residues. In agriculture environmental, trace metals undergo numerous changes during their transport due to dissolution, precipitation and sorption phenomena. From the results of the present investigation, the following conclusions can be drawn: (1) Based on calculating the results of the Pearson correlation coefficient indicated that had good relation between soil and samples of irrigating channel. (2) Total metal content results indicated that the concentration decreased exponentially as the irrigation distance and profile depth in the agricultural soils. (3) Speciation results indicated that the percentage of Fractions 3 (57 % data) decreased exponentially as the irrigation distance in the five site whereas that of Fraction 5 (70 % data) increased along the irrigation distance. (4) Therefore, based on the aforementioned results can presumed that heavy metal transportation was via the sediment or suspended particulate to the field. (5) For all metals, skewness coefficient results indicated that total concentrations were not normally distributed, showing rather positively skewed (57 % data are strongly skewed). Therefore, agricultural soils contaminant phenomena were Non-homogeneous. (6) XANES results indicated that the Cr species in the soils were mostly in trivalent chromium, which presents a low risk for the environment and human health. Cr(VI) may reduce with many reductants in the soil, such as Fe(II), sulfide, and organic compounds(Pettine and Capri, 2005). (7) Based on the sequential extraction and XANES results are consistent with a poor Cr mobility since the exchangeable and adsorbed forms corresponded only to 0.05 % and the chromium was present in the soil as the barely soluble Cr3+ species. (8) The closest atoms to the Cr species of soils and sediments appeared to have the different bonding structure based on the EXAFS spectra by synchrotron radiation technique.
URI: http://hdl.handle.net/11455/28150
其他識別: U0005-2508200823412200
Appears in Collections:土壤環境科學系

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