鄰苯二甲酸酯類於人工溼地之流布與去除率探討-以大樹舊鐵橋人工溼地為例

Distribution and Removal of Phthalate Esters (PAEs) in a Constructed Wetland－a Case Study of Dashu Old Railroad Bridge Constructed Wetland

陳哲瑋(Zhe-wei Chen)

指導教授 ： 黃益助

國立屏東科技大學/工學院/環境工程與科學系所/碩士(2012年)

https://doi.org/10.6346/NPUST.2012.00006

摘要

本研究於2012年2月至9月份間，自高雄市大樹舊鐵橋人工溼地之B系統6個採樣點，共進行4次水質與底泥採樣。利用固相萃取法(solid phase extraction, SPE)及吹氮濃縮進行樣品前處理，再以氣相層析儀搭配電子捕捉偵測器(GC-ECD)，進行6種鄰苯二甲酸酯類(分別為DIBP、DBP、DNHP、BBP、DEHP、DNOP)分析。主要探討鄰苯二甲酸酯類於舊鐵橋人工溼地水質與底泥中之分布情形與溼地淨化效率，並瞭解底泥總有機碳與底泥PAEs濃度之相關性。
結果顯示，鄰苯二甲酸酯類於水體濃度方面，整體以DBP濃度為最高，濃度範圍於0.04-2.85 μg L-1，其餘PAEs分別是DIBP濃度範圍ND~0.82 μg L-1、DNHP濃度範圍ND~0.59 μg L-1、BBP濃度範圍ND~0.05 μg L-1、DEHP濃度範圍ND~0.49 μg L-1、DNOP濃度範圍ND~4.48 μg L-1；溼地平均去除各項PAEs效率，以BBP為最高，平均去除效率為86 %，其次為DIBP、DEHP及DBP，去除效率分別為72 %、70 %、61 %；6種 PAEs於各點水體中之累加平均濃度，分別S1平均濃度為1.64 μg L-1、S2平均濃度為1.89 μg L-1、S3平均濃度為3.10 μg L-1、S4平均濃度為2.57 μg L-1、S5平均濃度為1.47 μg L-1、S6平均濃度為1.44 μg L-1，由上述累加濃度可看出，PAEs於S3為最高，其次為S4，人工溼地對於6種PAEs之整體去除效率為54 %，而溼地各季累加去除效率分別為二月份48 %、四月份53 %、六月份78 %、九月份 20 %；PAEs於人工溼地底泥濃度分布情形，整體以DEHP為最高，濃度範圍為0.26-10.65 μg g-1，其餘PAEs分別是DIBP濃度範圍ND-1.35 μg g-1、DNHP濃度範圍ND-0.87 μg g-1、BBP濃度範圍 ND-0.16 μg g-1、DBP濃度範圍 ND-2.39 μg g-1、DNOP濃度為ND，其中以DEHP之檢出率為最高(100 %)，其次為DIBP檢出率96 %及DBP檢出率78 %；DEHP於溼地底泥之濃度分布中，採樣點S2於本研究四次採樣分析皆高於底泥品質指標之下限值(1.97 μg g-1)，另採樣點S3及S4則分別於2月、4月及6月高於底泥品質指標之下限值，而溼地底泥DEHP最高濃度出現於採樣點S4，濃度為10.65 μg g-1，幾乎已達指標上限值(19.7 μg g-1)的一半，建議針對該項目增加其檢測頻率，以免造成長期生態及人體之健康危害；水體與底泥濃度相關性，以DEHP、DBP之正相關性較高，相關係數(r)分別為0.62、0.56；底泥與其總有機碳之相關性，以DBP之r = 0.61為最高。本研究顯示，鄰苯二甲酸酯類普遍存在於水體環境中，底泥中之鄰苯二甲酸酯類濃度大多高於水體中，且與底泥總有機碳含量呈正相關性。
關鍵字：鄰苯二甲酸酯類、底泥、固相萃取法、總有機碳、溼地

關鍵字

鄰苯二甲酸酯類 ； 底泥 ； 固相萃取法 ； 總有機碳 ； 溼地

並列摘要

From February to September of 2012, four surveys of water quality and sediment were implemented at six sampling points of the B system of Dashu Old Railroad Bridge constructed wetlands in Kaohsiung City. Solid phase extraction (SPE) method and concentrated with a stream of nitrogen gas were utilized as pretreatment and then analyzed by a gas chromatography equipped with an electron capture detector (GC/ECD) to quantify the concentration of phthalate esters (PAEs) including DIBP, DBP, DNHP, BBP, DEHP, DNOP. The aims of this study are to investigate the distribution of PAEs between water and sediment and their removals in constructed wetlands, and to understand the correlations of total organic carbon (TOC) and PAEs within the sediments.
The results showed that overall the DBP concentrations were the highest among concerned PAEs in water, its concentration ranged from 0.04 to 2.85 μg L-1. The concentration ranges of DIBP, DNHP, BBP, DEHP and DNOP were ND - 0.82, ND - 0.59, ND - 0.05, ND - 0.49, ND - 4.48 μg L-1, respectively. Among the average removal ratios of PAEs by wetlands, BBP was the highest (86%), followed by DIBP (72%), DEHP (70%), and DBP (61%). The average cumulative concentrations of PAEs in water at S1, S2, S3, S4, S5, and S6 were 1.64, 1.89, 3.10, 2.57, 1.47, and 1.44 μg L-1, respectively. As shown from the above mentioned cumulative concentrations, PAEs in S3 was the highest, followed by S4. The overall removal ratio of PAEs by wetlands was 54%. While the cumulative removal ratios of PAEs were 48%, 53%, 78%, and 20% for February, April, June, and September, respectively. Overall DEHP with concentration ranging from 0.26 to 10.65 μg g-1 was the highest PAEs contents within sediment in constructed wetlands. The content ranges of DIBP, DNHP, BBP, DBP, and DNOP were ND - 1.35, ND - 0.87, ND - 0.16, ND - 2.39, and ND, respectively. The detection rates for DEHP (100 %) were the highest, followed by DIBP (96%) and DBP (78%). Four samples drawn from S2 station, the DEHP contents in sediment were higher than the lower limits of 1.97 μg g-1 set by sediment quality index Samples taken from stations S3 and S4 in February, April, and June, the DEHP contents were also higher than the lower limits of sediment quality index. The highest DEHP content of 10.65μg g-1 in sediment occurred at station S4 was more than one half of the higher limit (19.7 μg g-1), it is recommended to increase the survey frequency so as to avoid long-time hazards to ecology and human health. As seen from the correlation of PAEs concentrations between water and sediment, DEHP and DBP showed higher positive correlation with respective correlation coefficient (r) of 0.62 and 0.56. As shown from the correlation of PAEs and TOC in sediment, DBP was the highest with r = 0.61. This study showed that prevalence of PAEs in aquatic environment was confirmed. Most PAEs concentrations in sediment were higher than those in water body and were positively correlated with TOC contents in sediment.

Keywords: phthalate esters, sediment, solid phase extraction, total organic carbon, wetland

並列關鍵字

phthalate esters ； sediment ； solid phase extraction ； total organic carbon ； wetland

參考文獻

林建宇，2011，分散性奈米鐵和鈀/鐵雙金屬粒子降解四氯乙烯之研究，碩士論文，國立屏東科技大學，環境工程與科學系，屏東。

行政院環境保護署，2002，去硫淨化法，NIEA M186.00C。

行政院環境保護署，2009，土壤酸鹼值(pH值)測定方法-電極法，NIEA S410.62C。

行政院環境保護署，2011，公告毒性化學物質及其管制濃度與大量運作基準一覽表。

行政院環境保護署，2012a，底泥品質指標之分類管理及用途限制辦法。