奈米碳管對於硝基酚與銅之競爭吸附

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李向曦(Hsiang-hsi Lee) 查詢紙本館藏

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論文名稱

奈米碳管對於硝基酚與銅之競爭吸附
(Competitive adsorption of nitrophenol and copper(II)from aqueous solutions on mult-walled carbon nanotubes)

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摘要(中)

本研究利用奈米碳管吸附鄰-硝基苯酚(2-NP)、對-硝基苯酚(4-NP)及銅離子(Cu2+)，探討其競爭吸附及機制。研究結果顯示，經硝酸氧化處理後，比表面積與氧化前差異不大，但在碳管表面引入官能基－COOH，使得碳管表面電荷有所改變，造成對2-NP、4-NP及Cu2+的吸附影響。等溫吸附實驗顯示，碳管的含氧官能基多寡會影響2-NP、4-NP及Cu2+之吸附量，未經氧化奈米碳管吸附2-NP及4-NP之吸附量會優於氧化後奈米碳管，和空間障礙及水簇作用有關。而氧化後奈米碳管對吸附Cu2+之吸附量會大於未氧化碳管，會因官能基的增加提高碳管表面負電荷，導致吸附量提高。2-NP與4-NP因電子分佈之影響，氧化前後奈米碳管對4-NP的吸附能力較2-NP低；不論酸氧化前後奈米碳管，對於2-NP及Cu2+之吸附皆較為符合Langmuir模式，而對於4-NP之吸附則較為符合polanyi 模式。經熱力學分析得知酸氧化前後奈米碳管吸附2-NP及4-NP均為放熱反應；而酸氧化前後奈米碳管吸附Cu2+為吸熱反應。在不同pH值下，酸氧化後奈米碳管吸附2-NP及4-NP之吸附量具有相同的趨勢，與分子解離及表面電荷有關；吸附Cu2+則與表面電荷及沉澱有關。在2-NP及4-NP存在下之競爭結果顯示，碳管吸附Cu2+之吸附量增加，因2-NP及4-NP解離後將可能與Cu2+形成新物質或錯合物，提高Cu2+之吸附百分比；但在pH值小於7時，Cu2+將對氧化後奈米碳管吸附2-NP及4-NP產生抑制作用，與水合作用產生遮蔽效應有關。

摘要(英)

Adsorption of 2-nitrophenol (2-NP), 4-nitrophenol (4-NP), and copper (Cu2+) by multi-walled carbon nanotubes (MWCNTs) with and without oxidation by nitric acid were investigated in this study. The adsorption capacities of 2-NP and 4-NP by A-MWCNT were larger than H-MWCNT, because of steric obstructions and water clustering. On the other hand, H-MWCNT had better adsorption capacity of Cu2+ than A-MWCNT, because the functional groups generated more negatively charged surface. Furthermore, MWCNTs had better adsorption capacity of 2-NP than 4-NP due to the electronic distribution. The adsorption of 2-NP and 4-NP by MWCNTs were endothermic while the adsorption of Cu2+ was exothermic. The enthalpy change and free energy change suggested that the adsorption of 2-NP, 4-NP, and Cu2+ onto MWCNTs were physisorptions. The adsorption at different pH values showed that the adsorption of 2-NP and 4-NP by H-MWCNT had the same trend, relating to the molecular dissociation and surface charge, while the adsorption of Cu2+ was affected by the surface charge and precipitation. When 2-NP or 4-NP were present, the adsorption of Cu2+ was promoted, because complexes of 2-NP/Cu and 4-NP/Cu may form after 2- and 4-NP dissociated. When pH values were lower than 7, the adsorption of 2-NP and 4-NP would be inhibited by Cu2+ due to the shielding from hydration of Cu2+.

關鍵字(中)

★ Polanyi model
★ Langmuir model
★ 競爭吸附

關鍵字(英)

★ competitive adsorption
★ Polanyi model
★ Langmuir model

論文目次

摘要.....i
Abstract.....ii
誌謝.....iii
目錄.....iv
圖目錄.....vii
表目錄.....x
第一章前言.....1
1-1研究緣起.....1
1-2研究內容與目的.....3
1-3研究流程.....4
第二章文獻回顧.....5
2-1奈米碳管.....5
2-1-1基本特性.....5
2-1-2奈米碳管之純化與改質.....7
2-2吸附理論.....11
2-2-1物理吸附與化學吸附.....11
2-2-2 液相吸附擴散機制.....12
2-2-3 等溫吸附模式.....13
2-2-4 吸附熱力學特性.....15
2-2-5 影響吸附之因素.....16
2-3 奈米碳管吸附行為之相關研究.....18
2-3-1 污染物之吸附與機制.....18
2-3-2 環境競爭影響.....21
2-4 銅及硝基苯酚異構物.....23
2-4-1 銅之特性及對環境影響.....23
2-4-2 硝基苯酚異構物之特性.....23
第三章實驗方法.....27
3-1 實驗材料與設備.....27
3-1-1 實驗材料.....27
3-1-2 實驗設備.....28
3-2 實驗方法.....30
3-2-1 奈米碳管之改質方法.....30
3-2-2 硫酸銅溶液配置及檢量線.....32
3-2-3 硝基苯酚異構物之定量分析.....33
3-2-4 等溫吸附實驗.....35
第四章結果與討論.....37
4-1 奈米碳管之定性分析.....37
4-1-1表面形態及孔洞分佈.....37
4-1-2酸氧化前後奈米碳管之純度分析.....43
4-1-3氧化前後奈米碳管之官能基分析.....45
4-2 酸氧化前後對硝基酚吸附能力之影響.....47
4-2-1 等溫吸附模式.....48
4-2-2 吸附機制.....53
4-2-3 吸附熱力學之分析.....58
4-3酸氧化前後對銅的吸附影響.....62
4-3-1等溫吸附模式.....63
4-3-2吸附機制.....65
4-3-3 熱力學之探討.....68
4-4奈米碳管對硝基酚與銅之競爭吸附.....70
第五章結論與建議.....76
5-1 結論.....76
5-2 建議.....78
參考文獻.....79

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指導教授

秦靜如(Ching-Ju Chin)

審核日期

2012-7-30

推文