水溶液相中多壁奈米碳管分散懸浮與抑菌效果之相關性探討

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齊慕凡(Mu-fan Chi) 查詢紙本館藏

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論文名稱

水溶液相中多壁奈米碳管分散懸浮與抑菌效果之相關性探討
(Investigation of the correlation between dispersivity and microbial toxicity of multi-walled carbon nanotubes in aquesous phase)

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摘要(中)

奈米科技由於可廣泛應用於各個領域，已被視為是二十一世紀最重要的新興科技之一。然而，近年來奈米材料的大量製造與利用逐漸使得這些奈米顆粒進入環境中的機率大增；不僅如此，這些奈米材料所具有的獨特高比表面積使其被歸類為高反應性和高物化動態的材料，易於環境和生物系統中發生許多轉化，特別是與自然界存在之天然有機物或人為有機污染物之間的吸附反應，而這些轉化作用終將改變奈米材料的宿命、傳輸以及毒性作用，因此實有必要在這些材料的生產製造有顯著進展前了解其轉化的性質和程度，以推估其所帶來的環境風險。有鑒於此，為了解具微生物毒性潛力的奈米碳管 (carbon nanotubes, CNTs) 在與常見的有機物質作用後，其物化特性的改變對其所引起的生物毒性的影響為何，本研究透過平板計數、OD600生長曲線、螢光染劑染色以及量測細胞ATP總量等方法，觀察改質前後與吸附有機質前後的多壁奈米碳管 (multiwalled carbon nanotubes, MWCNTs) 對模式生物E. coli所造成之細胞毒性效應（毒性的觀察以細胞致死或生長抑制的程度顯示）。結果顯示在暴露期間為震盪搖晃的條件下，裸露未吸附有機質的原始碳管A-MWCNTs (本身分散性差) 比裸露的改質碳管H-MWCNTs (本身分散性佳) 所造成的E. coli細胞毒性較強，可能是由於H-MWCNTs表面帶含有COO－等帶電官能基，故較A-MWCNTs不容易與菌接觸。此外，腐植酸 (humic acid, HA) 或鄰苯二甲酸二乙酯 (diethyl phthalate, DEP) 吸附於碳管表面所形成的高分子層空間位阻，除了能增加A-MWCNTs於水相中的分散穩定性外，亦能減緩其與E. coli的直接接觸，致使A-MWCNTs的細胞毒性減緩。H-MWCNTs吸附HA後在碳管表面形成之HA高分子層同樣能減輕H-MWCNTs的毒性，但在高濃度DEP溶液中之H-MWCNTs卻增加了碳管的微生物毒性，然其中的原因還無法確定。整體而言，這些結果顯示未改質之碳管在環境中與含苯環的有機物相互作用後，對於水生生態較為友善，但在評估環境風險時也不能忽視H-MWCNTs於較高DEP濃度的溶液中，些微增加微生物毒性此種特殊之現象。

摘要(英)

Recent advances in nanotechnology have created numerous and promising applications in all sectors of society, thus making nanotechnology been considered as one of the most important technologies in the 21st century. However, the rapid worldwide development of nanotechnology seems inevitably increase the likelihood of the release of engineered nanomaterials (ENMs) to the environment. As being classified as a highly reactive and dynamic type of materials, ENMs are expected to easily undergo a number of transformations once released to the environment, thereby ultimately influencing the fate, transport and toxicity of these materials in both environmental and biological systems. Given that organic matter (OM) is a key factor controlling the behavior of chemicals in aquatic settings and microbes are the foundation of many ecosystems, probing the “OM-nanomaterial reactions” and consequent effect on microbial toxicity is one step towards understanding the lifetimes of nanomaterials in the environment and their potential toxicity on organisms exposed to them.

In this study, laboratory experiments that incorporated approaches of viable count, growth monitoring (through optical-density measurement), LIVE/DEAD fluorescent staining, as well as total cellular ATP analysis were carried out to investigate the toxic extent of multi-walled carbon nanotubes (MWCNTs) towards the model organism E. coli. Specifically, this study focused on the microbial toxicity comparison of “surface-modified vs. surface-unmodified” and “OM-adsorbed vs. OM-unadsorbed” MWCNTs. Results indicated that over the course of exposure in the absence of OM, agitation led to higher cytotoxicity in unmodified MWCNTs (designated as A-MWCNTs) solution than in modified MWCNTs (designated a H-MWCNTs), probably due to more quantities of charged COO- moieties on the surface of H-MWCNTs that eventually prevented direct contact between E. coli cells and H-MWCNTs. Similarly, although humic acid (HA)- and diethyl phthalate (DEP)-sorption increased the dispersivity of A-MWCNTs, adsorption of these OM on A-MWCNTs minimized the toxicity of A-MWCNTs on E. coli owing to the same steric-obstruction effect. However, such sheltering effects were only observed in the H-MWCNTs solution containing HA as opposed to DEP, because H-MWCNTs equilibrated with higher concentrations of DEP resulted in higher growth inhibition, instead of toxicity mitigation. Explanations for this observation were currently unavailable.

Together, these results suggested that while the interaction of MWCNTs and phenolic OM may not significantly cause a deleterious effect in the aquatic ecosystem, care should be taken when assessing environmental risk arising from exposure of H-MWCNTs in the presence of higher DEP concentrations.

關鍵字(中)

★ 多壁奈米碳管
★ 腐植酸
★ 鄰苯二甲酸二乙酯
★ 空間位阻
★ 分散性
★ 微生物毒性

關鍵字(英)

★ multi-walled carbon nanotubes
★ humic acid
★ diethyl phthalate
★ steric obstructions
★ dispersivity
★ microbial toxicity

論文目次

摘要 I
ABSTRACT III
圖目錄 VII
表目錄 XI
第一章前言 1
1.1 研究動機 1
1.2 研究目的 3
第二章文獻回顧 4
2.1 奈米材料 4
2.1.1 碳基奈米材料 4
2.1.2 奈米碳管 6
2.2 奈米材料在環境中的轉化 8
2.2.1 化學轉化 9
2.2.2 物理轉化 11
2.2.3 生物行為轉化 12
2.2.4 奈米材料與生物高分子間的交互作用 13
2.3奈米碳管於水相中的吸附及分散行為 15
2.4奈米碳管之微生物毒理機制 17
第三章實驗方法 20
3.1 多壁奈米碳管改質 20
3.2 多壁奈米碳管儲備液的準備 21
3.3 腐植酸儲備液的準備 22
3.4 鄰苯二甲酸二乙酯儲備液的準備 23
3.5 試驗培養基的成分與配製 24
3.6 實驗用之模式菌種 29
3.7 微生物毒性試驗 30
3.7.1 平板計數法 32
3.7.2 光學密度生長曲線法 32
3.7.3 高通量細菌存活率試驗 33
3.7.4 細胞ATP總量之測定分析 35
3.8 統計分析 38
第四章結果與討論 39
4.1碳管懸浮穩定性及表面化性對微生物毒性的影響 44
4.1.1吸附不同濃度HA對碳管微生物毒性之影響 44
4.1.2吸附不同濃度DEP對碳管微生物毒性之影響 53
4.2細菌存活率試驗 64
4.3細胞ATP總量分析 77
4.4 環境意義 83
第五章結論與建議 86
5.1 結論 86
5.2 建議 87
參考文獻 89

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指導教授

林居慶

審核日期

2014-8-28

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