臺灣博碩士論文加值系統

本研究探討工廠廢棄活性白土吸附水溶液重金屬之特性，以銅、鎳、鋅、鉛、鎘五種重金屬離子作為吸附對象，研究探討相關操作條件對其吸附特性的影響，包括：溶液pH值、離子強度、重金屬濃度、溫度等因子，以了解廢棄活性白土對五種重金屬離子吸附行為之影響。
廢棄活性白土經由咖啡機沸水沖洗，其吸附效果顯著，結果發現，加熱處理過之廢棄活性白土，其吸附效果雖低於活性白土(Activated Clay)，卻相對明顯高於廢棄活性白土，為一吸附性質頗佳之材料。
咖啡機清洗廢棄活性白土(SAC)對水溶液中重金屬離子去除之研究結果顯示，經由動力及平衡吸附試驗，在pH值增高的情況下，重金屬離子被吸附有增加之趨勢。而在低離子濃度及高反應溫度(50℃)下，對吸附重金屬離子，會呈現較高的去除效率。且離子強度增加，咖啡機處理廢棄活性白土吸附重金屬離子則有減少趨勢。結果顯示試驗條件如各重金屬濃度的改變、pH值的變化、溫度的高低、離子強度的不同，對其去除率皆會有不同之影響。

This thesis was forcus on studying adsorption characteristic of heavy metals onto spent activated clay（SPAC）. Five metals,Cu, Ni, Zn,Pb,Cd were used as absorbate. Parameters that may be affected the adsorption including, solution pH, ionic strength, metal concentration, and temperature were conducted.
Experimental results showed that the SPAC treated by coffee machine. Exhibited in a higher adsorption capacities than that of the SPAC without treated. Results also showed both increasing pH and temperature could increase the adsorption. However, as experimental condition was controlled at low ionic strength, the adsorption capacity was decreased according. The result,also demonstrated as changing the testing conditions including, heavy metals concentration, the pH, the temperature, the ion intensity , all can have the different influence to its removing rate.

摘要…………………………………………Ι
英文摘要……………………………………………………Ⅱ
目錄……………………………………………………Ⅲ
圖目錄……………………………………………………Ⅶ
表目錄……………………………………………………ⅩⅣ
第一章 緒論 ……………………………………………………1
1-1 前言……………………………………………………………………1
1-2 研究目的與內容………………………………………………………3
第二章 文獻回顧……………………………………………………4
2-1 活性白土資源化技術…………………………………………………4
2-2 吸附原理及理論………………………………………………………6
2-3 等溫吸附模式…………………………………………………………7
2-4 吸附特性之主要影響因子……………………………………………11
第三章 研究材料與方法……………………………………………………12
3-1 研究流程………………………………………………………………12
3-2 研究設備與儀器………………………………………………………13
3-3 實驗器皿之清潔………………………………………………………14
3-4 研究材料及藥品………………………………………………………14
3-5 研究方法………………………………………………………………18
3-6 實驗控制條件…………………………………………………………22
3-7 分析方法………………………………………………………………25
3-8 活性白土與未處理、已處理廢棄活性白土之吸附重金屬動力實驗
綜合比較………………………………………………………………30
第四章 結果與討論……………………………………………………32
4-1 Cu動力吸附實驗……………………………………………………32
4-1-1不同Cu初始濃度下SAC吸附Cu之影響……………………32
4-1-2不同離子強度下SAC吸附Cu之影響…………………………34
4-1-3不同pH值下SAC吸附Cu之影響……………………………37
4-1-4不同溫度下對SAC吸附Cu之影響……………………………39
4-1-5不同吸附劑下吸附Cu之影響……………………………………41
4-2 Ni動力吸附實驗……………………………………………………44
4-2-1不同Ni初始濃度下SAC吸附Ni之影響………………………44
4-2-2不同離子強度下SAC吸附Ni之影響…………………………46
4-2-3不同pH值下SAC吸附Ni之影響………………………………48
4-2-4不同溫度下SAC吸附Ni之影響………………………………50
4-2-5不同吸附劑下SAC吸附Ni之影響……………………………52
4-3 Zn動力吸附實驗……………………………………………………54
4-3-1不同Zn初始濃度下SAC吸附Zn之影響………………………54
4-3-2不同離子強度下SAC吸附Zn之影響…………………………56
4-3-3不同pH值下SAC吸附Zn之影響………………………………58
4-3-4不同溫度下SAC吸附Zn之影響………………………………60
4-3-5不同吸附劑對SAC吸附Zn之影響……………………………62
4-4 Pb動力吸附實驗……………………………………………………64
4-4-1 不同Pb初始濃度下SAC吸附Pb之影響………………………64
4-4-2 不同離子強度下SAC吸附Pb之影響…………………………66
4-4-3 不同條件pH值下SAC吸附Pb之影響…………………………68
4-4-4不同溫度下SAC吸附Pb之影響…………………………………69
4-4-5不同吸附劑下SAC吸附Pb之影響………………………………71
4-5 Cd動力吸附實驗…………………………………………………73
4-5-1不同Cd初始濃度下SAC吸附Cd之影響………………………73
4-5-2不同離子強度下SAC吸附Cd之影響……………………………75
4-5-3不同pH值下SAC吸附Cd之影響………………………………77
4-5-4不同溫度下SAC吸附Cd之影響…………………………………79
4-5-5不同吸附劑下SAC吸附Cd之影響………………………………81
4-6 不同重金屬動力實驗影響因子綜合比較……………………………83
4-7 Cu平衡吸附實驗……………………………………………………85
4-7-1 pH值對SAC吸附Cu之影響……………………………………85
4-7-2離子強度對Cu平衡吸附線之影響………………………………86
4-7-3 pH值對Cu吸附等溫線之影響……………………………………88
4-7-4溫度對Cu吸附等溫線之影響……………………………………90
4-7-5各種材料對Cu去除之概況………………………………………93
4-8 Ni平衡吸附…………………………………………………………95
4-8-1 pH值對SAC吸附Ni之影響………………………………………95
4-8-2離子強度對Ni平衡吸附線之影響………………………………96
4-8-3 pH值對Ni吸附等溫線之影響……………………………………98
4-8-4溫度對Ni吸附等溫線之影響……………………………………99
4-8-5各種材質對Ni去除之概況………………………………………101
4-9 Zn恆溫平衡吸附實驗……………………………………………104
4-9-1 pH值對SAC吸附Zn之影響……………………………………104.
4-9-2離子強度對Zn平衡吸附線之影響………………………………105
4-9-3 pH值對Zn吸附等溫線之影響…………………………………107
4-9-4溫度對Zn吸附等溫線之影響……………………………………108
4-9-5各種材質對Zn去除之概況………………………………………111
4-10 Pb恆溫平衡吸附實驗……………………………………………112
4-10-1 pH值對SAC吸附Pb之影響…………………………………112
4-10-2離子強度對Pb平衡吸附線之影響……………………………113
4-10-3 pH值對Pb吸附等溫線之影響…………………………………115
4-10-4溫度對Pb吸附等溫線之影響…………………………………116
4-10-5各種材料對Pb去除之概況……………………………………119
4-11 Cd恆溫平衡吸附實驗…………………………………………120
4-11-1不同pH值下SAC吸附Cd之百分比影響……………………120
4-11-2離子強度吸附Cd平衡吸附線之影響…………………………121
4-11-3 pH值對Cd吸附等溫線之影響………………………………123
4-11-4溫度對Cd吸附等溫線之影響…………………………………124
4-11-5各種材料對Cd去除之概況……………………………………126
4-12 不同重金屬平衡實驗影響因子綜合比較………………………128
第五章 結論與建議…………………………………………………………130
5-1 結論……………………………………………………………130
5-2 建議……………………………………………………………132
參考文獻……………………………………………………………………133
圖目錄
Fig2-1-1 活性白土……………………………………………………………5
Fig2-3-1 吸附等溫曲線分類………………………………………………10
Fig3-1-1 咖啡機清洗廢棄活性白土對重金屬吸附試驗架構圖 …………15
Fig3-4-1 活性白土 …………………………………………………………15
Fig3-4-2 廢棄活性白土 ……………………………………………………15
Fig3-4-3 咖啡機熱處理廢棄活性白土 ……………………………………15
Fig3-4-4 活性白土SEM影像 x600 ………………………………………16
Fig3-4-5 廢棄活性白土SEM影像 x200 ……………………………………16
Fig3-4-6 廢棄活性白土SEM影像 x500 ……………………………………16
Fig3-5-1 Comparison different adsorbets for SAC adsorption kinetics………19
Fig3-7-1 Relationship between Cu prepares and measwerd from AA………26
Fig3-7-2 Relationship between Ni prepares and measwerd from AA………27
Fig3-7-3 Relationship between Zn prepares and measwerd from AA………28
Fig3-7-4 Relationship between Pb prepares and measwerd from AA………29
Fig3-7-5 Relationship between Cd prepares and measwerd from AA………30
Fig3-8-1 Comparison different adsorbets for Cu adsorption kinetics；solid lines represent best fit of modified Freundlich equation………………31
Fig4-1-1 Effect of initial Cu (Ⅱ) concentration on adsorption kinetics; solid lines represent best fit of modified Freundlich equations…………33
Fig4-1-2 Realtionship between initial Cu concentration and rate constant k , Data was obtained from Table 4-1-1………………………………34
Fig4-1-3 Effect of ionic strength on adsorption kinetics;solid lines represent best fit of modified Freundlich.equation.………………………35
Fig4-1-4 Realtionship between ionic strength concentration and rate constant k , Data was obtained from Table 4-1-2………………………………36
Fig4-1-5 Effect of pH on adsorption kinetics; solid lines represent best fit of modified Freundlich. Equation……………………………………38
Fig4-1-6 Effect of temperature on adsorption kinetics; solid lines represent best fit of modified Freundlich.equation.………………………………40
Fig4-1-7 Piot for determination of acfivation energy E for the kinetic adsorption of Cu(Ⅱ) onto SAC………………………………………………41
Fig4-1-8 Comparison different adsorbets for Cu adsorption kinetics; solid lines represent best fit of modified Freundlich. equation………………42
Fig4-2-1 Effect of initial Ni (Ⅱ) concentration on adsorption kinetics;solid lines represent best fit of modified Freundlich equations…………………44
Fig4-2-2 Realtionship between initial Ni concentration and rate constant k , Data was obtained from Table 4-2-1……………………………………45
Fig4-2-3 Effect of ionic strength on adsorption kinetics; solid lines represent best fit of modified Freundlich equation………………………………47
Fig4-2-4 Realtionship between ionic strength concentration and rate constant k , Data was obtained from Table 2…………………………………48
Fig4-2-5 Effect of pH on adsorption kinetics; solid lines represent best fit of modified Freundlich equation…………………………………49
Fig4-2-6 Effect of temperature on adsorption kinetics; solid lines represent best fit of modified Freundlich. equation……………………………51
Fig4-2-7 Piot for determination of acfivation energy E for the kinetic adsorption of Ni(Ⅱ) onto SAC……………………………………………52
Fig4-2-8 Comparison different adsorbets for Ni adsorption kinetics; solid lines represent best fit of modified Freundlich. equation……………53
Fig4-3-1 Effect of initial Zn (Ⅱ) concentration on adsorption kinetics;solid lines represent best fit of modified Freundlich equations……………54
Fig4-3-2 Realtionship between initial Zn concentration and rate constant k , Data was obtained from Table 4-3-1………………………………55
Fig4-3-3 Effect of ionic strength on adsorption kinetics; solid lines represent best fit of modified Freundlich equation…………………………57
Fig4-3-4 Realtionship between ionic strength concentration and rate constant k , Data was obtained from Table 4-3-2…………………………58
Fig4-3-5 Effect of pH on adsorption kinetics; solid lines represent best fit of modified Freundlich. Equation………………………………59
Fig4-3-6 Effect of temperature on adsorption kinetics; solid lines represent best fit of modified Freundlich. equation…………………………61
Fig4-3-7 Piot for determination of acfivation energy E for the kinetic adsorption of Zn(Ⅱ) onto SAC………………………………………62
Fig4-3-8 Comparison different adsorbets for Zn adsorption kinetics; solid lines represent best fit of modified Freundlich. equation…………………63
Fig4-4-1 Effect of initial Pb (Ⅱ) concentration on adsorption kinetics;solid lines represent best fit of modified Freundlich equations…………………64
Fig4-4-2 Realtionship between initial Pb concentration and rate constant k , Data was obtained from Table 4-4-1…………………………………65
Fig4-4-3 Effect of ionic strength on adsorption kinetics; solid lines represent best fit of modified Freundlich equation………………………………66
Fig4-4-4 Realtionship between ionic strength concentration and rate constant k , Data was obtained from Table 4-4-2………………………………67
Fig4-4-5 Effect of pH on adsorption kinetics; solid lines represent best fit of modified Freundlich. equation……………………………………68
Fig4-4-6 Effect of temperature on adsorption kinetics; solid lines represent best fit of modified Freundlich. equation………………………………70
Fig4-4-7 Piot for determination of acfivation energy E for the kinetic adsorption of Pb (Ⅱ) onto SAC……………………………………………71
Fig4-4-8 Comparison different adsorbets for Pb adsorption kinetics; solid lines represent best fit of modified Freundlich. equation………………72
Fig4-5-1 Effect of initial Cd (Ⅱ) concentration on adsorption kinetics;solid lines represent best fit of modified Freundlich equations…………………73
Fig4-5-2 Realtionship between initial Cd concentration and rate constant k , Data was obtained from Table 4-5-1………………………………74
Fig4-5-3 Effect of ionic strength on adsorption kinetics; solid lines represent best fit of modified Freundlich equation………………………………75
Fig4-5-4 Realtionship between ionic strength concentration and rate constant k , Data was obtained from Table 4-5-2………………………………76
Fig4-5-5 Effect of pH on adsorption kinetics; solid lines represent best fit of modified Freundlich. Equation……………………………………78
Fig4-5-6 Effect of temperature on adsorption kinetics; solid lines represent best fit of modified Freundlich. Equation………………………………80
Fig4-5-7 Piot for determination of acfivation energy E for the kinetic adsorption of Cd (Ⅱ) onto SAC……………………………………………81
Fig4-5-8 Comparison different adsorbets for Cd adsorption kinetics; solid lines represent best fit of modified Freundlich. equation…………………82
Fig4-6-1 Effect of initial Metal concentration on adsorption kinetics; solid lines represent best fit of modified Freundlich equations…………………83
Fig4-7-1 Surface Complex formation model. Experimental conditions………85
Fig4-7-2 Effect of ionic strength on the isotherm for Cu adsorption onto SAC ………………………………………………………………87
Fig4-7-3 Relationship between the equilibrium adsorption constants, K, and the first layer adsorption density, Qm, on the thickness of the electrical double layer, 1/κ…………………………………………………88
Fig4-7-4 Effect of pH on the isotherm for Cu adsorption onto SAC (Spent Activated Clay）…………………………………………………89
Fig 4-7-5 Effect of temperature on the isotherm for Cu adsorption onto SAC (Spent Activated Clay) ……………………………………………91
Fig4-7-6 Relationship between ln K and1/T. ………………………………92
Fig4-8-1 Surface Complex formation model. Experimental conditions………95
Fig4-8-2 Effect of ionic strength on the isotherm for Ni adsorption onto SAC ………………………………………………………96
Fig4-8-3 Relationship between the equilibrium adsorption constants, K, and the first layer adsorption density, Qm, on the thickness of the electrical double layer, 1/κ…………………………………………………97
Fig4-8-4 Effect of pH on the isotherm for Ni adsorption onto SAC…………98
Fig4-8-5 Effect of temperature on the isotherm for Ni adsorption onto SAC……………………………………………………………100
Fig4-8-6 Relationship between ln K and1/T………………………………101
Fig4-9-1 Surface Complex formation model.………………………………104
Fig4-9-2 Effect of ionic strength on the isotherm for Ni adsorption onto SAC……………………………………………………………105
Fig4-9-3 Relationship between the equilibrium adsorption constants, K, and the first layer adsorption density, Qm, on the thickness of the electrical double layer, 1/κ…………………………………………………106
Fig4-9-4 Effect of pH on the isotherm for Zn adsorption onto SAC…………107
Fig4-9-5 Effect of temperature on the isotherm for Zn adsorption onto SAC……………………………………………………………109
Fig4-9-6 Relationship between ln K and1/T………………………………110
Fig4-10-1 Surface Complex formation model.………………………………112
Fig4-10-2 Effect of ionic strength on the isotherm for Pb adsorption onto SAC…………………………………………………………113
Fig4-10-3 Relationship between the equilibrium adsorption constants, K, and the first layer adsorption density, Qm, on the thickness of the electrical double layer, 1/κ………………………………………………114
Fig4-10-4 Effect of pH on the isotherm for Pb adsorption onto SAC……………………………………………………………115
Fig4-10-5 Effect of temperature on the isotherm for Pb adsorption onto SAC…………………………………………………………117
Fig4-10-6 Relationship between ln K and1/T………………………………118
Fig4-11-1 Surface Complex formation model………………………………120
Fig4-11-2 Effect of ionic strength on the isotherm for Cd adsorption onto SAC …………………………………………………………121
Fig4-11-3 Relationship between the equilibrium adsorption constants, K, and the first layer adsorption density, Qm, on the thickness of the electrical double layer, 1/κ………………………………………………122
Fig4-11-4 Effect of pH on the isotherm for Cd adsorption onto SAC………123
Fig4-11-5 Effect of temperature on the isotherm for Cd adsorption onto SAC……………………………………………………………125
Fig4-11-6 Relationship between ln K and1/T………………………………126
Fig4-12-1 Effect of temperature on the isotherm for Cu 、Ni 、Zn、 Pb、 Cd adsorption onto SAC. ………………………………………128
表目錄
Table2-3-1 處理對策……………………………………………………………5
Table2-3-1 物理吸附與化學吸附之比較………………………………………7
Table3-4-1 活性白土特性分析…………………………………………………17
Table3-4-2 活性白土的性質……………………………………………………17
Table3-5-1 各種白土處理情形之比表面積及平均孔徑………………………20
Table3-6-1 動力實驗控制條件（Cu、Ni、Zn、Pb、Cd）………………… 24
Table3-6-2 平衡吸附條件（Cu、Ni、Zn、Pb、Cd）……………………… 25
Table3-8-1 Modified Freundlich Constants for adsorption of Cu onto SAC … 31
Table4-1-1 Modified Freundlich Constants for adsorption of Cu onto SAC…33
Table4-1-2 Modified Freundlich Constants for adsorption of Cu onto SAC…36
Table4-1-3 Modified Freundlich Constants for adsorption of Cu onto SAC…38
Table4-1-4 Modified Freundlich Constants for adsorption of Cu onto SAC…40
Table4-1-5 Modified Freundlich Constants for adsorption of Cu onto SAC…43
Table4-1-6 各種吸附劑之比表面積及平均孔徑……………………………43
Table4-2-1 Modified Freundlich Constants for adsorption of Ni onto SAC…45
Table4-2-2 Modified Freundlich Constants for adsorption of Ni onto SAC…47
Table4-2-3 Modified Freundlich Constants for adsorption of Ni onto SAC…49
Table4-2-4 Modified Freundlich Constants for adsorption of Cu onto SAC…51
Table4-2-5 Modified Freundlich Constants for adsorption of Ni onto SAC…53
Table4-3-1 Modified Freundlich Constants for adsorption of Zn onto SAC…54
Table4-3-2 Modified Freundlich Constants for adsorption of Zn onto SAC…55
Table4-3-3 Modified Freundlich Constants for adsorption of Znonto SAC…59
Table4-3-4 Modified Freundlich Constants for adsorption of Zn onto SAC…61
Table4-3-5 Modified Freundlich Constants for adsorption of Zn onto SAC…63
Table4-4-1 Modified Freundlich Constants for adsorption of Pb onto SAC…65
Table4-4-2 Modified Freundlich Constants for adsorption of Pb onto SAC…67
Table4-4-3 Modified Freundlich Constants for adsorption of Pb onto SAC…69
Table4-4-4 Modified Freundlich Constants for adsorption of Pb onto SAC…70
Table4-4-5 Modified Freundlich Constants for adsorption of Pb onto SAC…72
Table4-5-1 Modified Freundlich Constants for adsorption of Pb onto SAC…74
Table4-5-2 Modified Freundlich Constants for adsorption of Cd onto SAC…76
Table4-5-3 Modified Freundlich Constants for adsorption of Cd onto SAC…78
Table4-5-4 Modified Freundlich Constants for adsorption of Cd onto SAC…80
Table4-5-5 Modified Freundlich Constants for adsorption of Cd onto SAC…82
Table4-6-1 Comparison of rate constant（k）and（m）for 5metals…………84
Table4-7-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption .…………………………………87
Table4-7-2 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.…………………………………89
Table4-7-3 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption…………………………………92
Table4-7-4 Thermodynamic parameters for the adsorption of Cu onto SAC…92
Table4-7-5 Adsorption Capacity of Cu(II) by Various Adsorbents…………94
Table4-8-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption…………………………………97
Table4-8-2 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.…………………………………99
Table4-8-3 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………100
Table4-8-4 Thermodynamic parameters for the adsorption of Ni onto SAC…101
Table4-8-5 Adsorption Capacity of Ni(II) by Various Adsorbents…………103
Table4-9-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption…………………………………106
Table4-9-2 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………108
Table4-9-3 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………110
Table4-9-4 Thermodynamic parameters for the adsorption of Zn ontoSAC…110
Table4-9-5 Adsorption Capacity of Zn(II) by Various Adsorbents…………111
Table4-10-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………114
Table4-10-2 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………116
Table4-10-3 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………117
Table4-10-4 Thermodynamic parameters for the adsorption of Pb onto SAC …………………………………………………………118
Table4-10-5 Adsorption Capacity of Pb(II) by Various Adsorbents…………119
Table4-11-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………122
Table4-11-2 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption.………………………………124
Table4-11-3 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption………………………………125
Table4-11-4 Thermodynamic parameters for the adsorption of Cd onto SAC …………………………………………………………126
Table4-11-5 Adsorption Capacity of Cd (II) by Various Adsorbents………127
Table4-12-1 Equilibrium adsorption constants and specific surface area as determined by SAC adsorption. ………………………………129
Table4-12-2 Thermodynamic parameters for the adsorption of Cu 、Ni 、Zn、 Pb、 Cd onto SAC.………………………………………… 129

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