博碩士論文 100326009 詳細資訊




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姓名 廖炳傑( Ping-Chieh Liao)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 異化性鐵還原狀態下非生物性汞氧化還原 作用及其對地下水水質之影響
(Abiotic Redox Transformation of Hg under Dissimilatory Iron-Reducing Conditions and its Impact on Groundwater Quality)
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摘要(中) 汞是毒性最高的元素之一,當地下水源受汞污染時對公眾與生態是一大威脅,尤其當汞藉由地下水傳輸進入表面水體並進一步形成甲基汞後更為嚴重,但目前對於汞在地下水環境的轉換與流佈機制仍不清楚。即使如此,現有的調查資料顯示地下水汞污染可能跟厭氧微生物的代謝活動與其所引起的地化條件有關,且近期文獻亦指出部份鐵還原菌可不需透過生物性抗汞機制即可將汞還原,尤其當以固態三價鐵礦作為電子接受者時,此效果更加顯著。這些線索說明鐵還原菌生長時所形成的生源性亞鐵在汞氧化態的轉換作用上可能扮演著關鍵性的角色。為此,本研究藉由模擬地下水的環境條件,設計非生物性的汞還原縮模試驗,以測試「造成汞還原的物種乃是生源性的吸附型與晶格型亞鐵,且其還原程度由表面化學所主導」的假說。實驗結果證實當溶解態亞鐵於pH中性條件下與環境中常見的三價鐵礦goethite與hematite形成吸附型亞鐵時,有顯著的汞還原效應產生;此外,鐵還原菌利用鐵礦生長後所形成的二次礦物siderite,同樣對汞的還原效用也相當顯著。然而,在測試溶解態亞鐵與Hg(II)反應時,藉由PHREEQC對反應系統內的化學組成模擬時意外的發現,當Hg(II)與帶有胺基的有機物錯合時,將可能會提高汞本身被溶解態亞鐵離子還原的可能性,使得近80%的 Hg(II)被還原成Hg(0)。本研究結果意味著目前常用的現地生物整治工程需更為謹慎,因同樣依賴受污染地下含水層中的厭氧菌,使其刺激後進行污染物降解,過程中可能會無預警地改變汞或其他非整治標地污染物於地下水中的流佈行為,導致二次污染的情形發生。
摘要(英) Groundwater contamination with mercury (Hg) is an increasing problem worldwide, as Hg is one of the most toxic elements on Earth. Hg present in groundwater may not only render this water resource unsuitable for domestic use, it may also be transported to surface waters, where it would be converted by microbes to methylmercury, a potent neurotoxin, thus posing a greater threat to public and ecosystem health. However, the mechanisms that lead to transformation and movement of Hg in the groundwater environment are still largely unknown. Nonetheless, it has been suggested that Hg-contaminated groundwater may result from stimulation of microbial activities in subsurface environments. Relevantly, recent studies have shown that certain strains of dissimilatory iron-reducing bacteria (DFeRB) are able to reduce Hg(II) via an unknown pathway that is independent of mer activities, particularly when iron minerals are supplemented as terminal electron acceptors for DFeRB to respire. All these observations suggest that biogenic ferrous species produced by DFeRB may be a key player in the redox transformation of Hg in the subsurface anoxic zone. As a result, in this study laboratory microcosm experiments were conducted to explore the interaction between Hg and ferrous-iron under environmentally relevant iron-reducing conditions to test the following hypotheses: (i) in anoxic groundwater environments Hg(II) reduction under iron-reducing conditions is predominantly carried out by biogenic surface-bound and crystalline ferrous species, instead of dissolved ferrous; (ii) the degree to which the redox transformation of Hg by biogenic Fe(II) proceeds is primarily modulated by surface chemistry of iron minerals. Results from these microcosm tests showed that under neutral pH conditions when ferrous species were bound to goethite and hematite, two of the most commonly found ferric (oxyhydr)oxides in the environment, enhanced reduction of Hg(II) to Hg(0) was observed. In addition, siderite, one of secondary iron minerals frequently formed during the growth of iron-reducers in carbonate-buffering sedimentary environments, showed the capacity to reduce Hg(II) as well. Surprisingly, Hg(II) reduction by dissolved ferrous species was also observed when complexation of Hg(II) with amino-functionalized organic matter in the solution. Taken together, these results imply that conventional in situ bio-remedial actions relying on stimulation of indigenous microbial activities to enhance bio-degradation and reductive transformation of pollutants in contaminated subsurface sediments should be more cautious, as they might inadvertently mobilize Hg in the aquifer.
關鍵字(中) ★ 生源性亞鐵
★ 汞還原
★ 地下水
★ 異化性鐵還原菌
關鍵字(英) ★ biogenic ferrous species
★ mercury redox transformation
★ groundwater environments
★ dissimilatory iron-reducing bacteria
論文目次 摘要 i
Abstract ii
致謝 iv
目錄 v
圖目錄 viii
表目錄 xii
第一章 前言 1
1.1. 研究背景 1
1.2. 研究目的 3
第二章 文獻回顧 4
2.1. 異化性鐵還原菌 4
2.2. 汞的基本介紹 6
2.2.1. 汞的型態與化性 6
2.2.2. 汞的毒性與國內外相關法規 7
2.3. 土壤、表面水與地下水之汞來源以及其地化循環 9
2.4. 地下水背景濃度與汞污染案例 11
2.5. 汞在土壤與地下水的生地化反應 13
2.5.1. Hg(II)在地下含水層中非生物性還原以及吸附作用 14
2.5.2. Hg(II)在厭氧條件下非藉由mer活性驅使的生物性Hg(II)還原作用 15
第三章 實驗材料、方法與設備 17
3.1. 實驗流程 17
3.2. 實驗藥品與試劑 18
3.2.1. 藥品 18
3.2.2. 試劑 18
3.3. 實驗設備與儀器 20
3.3.1. 實驗設備 20
3.3.2. 分析儀器 23
3.4. 氧化鐵製備 24
3.5. Hg(II)還原實驗 25
3.5.1. 溶解態亞鐵(Fe(II)aq)對汞還原效應實驗 26
3.5.2. 氧化鐵礦物對汞還原效應實驗 28
3.5.3. 吸附型亞鐵(sorbed-Fe(II))對汞還原效應實驗 28
3.6. 非生物性縮模實驗 28
3.7. 分析方法 29
3.7.1. 氧化鐵礦物基本特性分析 29
3.7.2. 汞分析實驗 30
3.7.3. 鐵分析實驗 31
第四章 結果與討論 33
4.1. 合成鐵礦物基本特性分析 33
4.1.1. 外觀 33
4.1.2. 晶相 35
4.2. 回收率試驗 35
4.3. 有機緩衝溶劑(Good’s buffers)與Hg(II)還原作用 39
4.4. 溶解態亞鐵(Fe(II)aq)與Hg(II)還原作用 42
4.5. 吸附型亞鐵與汞還原作用 58
4.6. 結晶型亞鐵與汞還原作用 65
4.7. 非生物性縮模實驗 70




第五章 結論與建議 75
5.1. 結論 75
5.2. 建議 76
參考文獻 77
附錄一 85
附錄二 90
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指導教授 林居慶(Chu-Ching Lin) 審核日期 2014-1-23
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