系統識別號 | U0002-1201201710543100 |
---|---|
DOI | 10.6846/TKU.2017.00371 |
論文名稱(中文) | 以聚電解質加強超過濾結合化學還原法去除及回收重金屬 銅:pH和不同聚電解質的影響 |
論文名稱(英文) | Integration of PEUF and chemical reduction for copper removal and recovery:effect of pH and polyelectrolytes |
第三語言論文名稱 | |
校院名稱 | 淡江大學 |
系所名稱(中文) | 水資源及環境工程學系博士班 |
系所名稱(英文) | Department of Water Resources and Environmental Engineering |
外國學位學校名稱 | |
外國學位學院名稱 | |
外國學位研究所名稱 | |
學年度 | 105 |
學期 | 1 |
出版年 | 106 |
研究生(中文) | 周依宣 |
研究生(英文) | Yi-Hsuan Chou |
學號 | 602480328 |
學位類別 | 博士 |
語言別 | 英文 |
第二語言別 | |
口試日期 | 2017-01-09 |
論文頁數 | 101頁 |
口試委員 |
指導教授
-
李奇旺(chiwangli@gmail.com)
委員 - 陳孝行(f10919@ntut.edu.tw) 委員 - 劉志成(jhychern0212@gmail.com) 委員 - 簡義杰(chienichieh@gmail.com) 委員 - 彭晴玉(cypeng@uw.edu) |
關鍵字(中) |
化學還原法 銅 聚乙烯亞胺 連二亞硫酸鈉 聚電解質 |
關鍵字(英) |
chemical reduction copper dithionite PEUF PEI PSS PAA polyelectrolyte |
第三語言關鍵字 | |
學科別分類 | |
中文摘要 |
本研究以聚電解質加強超過濾(PEUF)結合化學還原法去除及回收重金屬(銅),探討pH和不同聚電解質的影響。在以化學還原法處理聚電解質加強超過濾(PEUF)濃縮液(PEI及銅)的結果中發現,當固定銅:還原劑(Na2S2O4):PEI的莫耳比,並逐漸提升銅的初始濃度時,銅的去除率會隨著初始濃度降低而下降。另一組實驗則為固定銅的初始濃度,改變PEI:Cu(II)的莫耳比,測試銅去除率之變化。結果顯示當PEI的濃度提高,則銅的去除率會隨之下降。透過TEM和更換濾膜(超濾膜)的實驗,證實去除率的降低是因奈米顆粒穿透0.45 μm的濾膜所造成。 研究中也分別探討以化學還原法處理三種不同的聚電解質(PSS, PAA, PEI)的PEUF濃縮液之銅去除率差異。結果中發現,若是以化學還原法處理PSS的含銅濃縮液,則無論操作在任一pH條件下,去除率均可達到約95%,且聚電解質不會附著在還原的銅顆粒上。在PAA系統中,銅的去除率在鹼性條件下有些微下降,不過除了pH10有降到85%以外,其它pH仍有95%以上的去除率。PEI是三種聚電解質中表現最差的,除了pH3、4有達到85%以外,其它pH的銅去除率都只有在40%以下。而三種不同聚電解質中的含銅濃縮液經化學還原法處理後所還原出的銅顆粒,大部均以氧化亞銅(Cu2O)及金屬銅(Cu)兩種形式存在。且經熱重分析儀(TGA)分析後,除了PEI系統中所產生的銅顆粒有聚電解質附著,PSS和PAA的還原銅顆粒都沒有聚電解質附著在上面。 綜合上述結果,以化學還原法回收PEUF濃縮液中的銅,在PSS的系統中,無論操作在任何pH條件下(pH3-10),銅去除率均可高達99-100%。不過由於PSS為帶負電的聚電解質,僅能靠靜電吸附吸引帶正電的污染物。若是水中存在的是帶負電的污染物(如:CuEDTA2-),則PSS無法在PEUF系統中將其去除,也因此PEI仍是較為合適的選擇。此外實驗結果中也顯示,當水中有EDTA的存在時,以化學還原法去除PEI系統中的銅時,其去除率也較沒有EDTA時更高。 另外為了解以化學還原法回收PEUF濃縮液中的銅和聚電解質時,是否會對聚電解質的結構或鍵結能力造成破壞或是影響,實驗中也以螢光滴定法和吸附穿透法測試PEI在多次重覆使用後,對銅離子鍵結力的影響。實驗結果中發現,還原劑(Na2S2O4)確實會造成溶液中離子強度提升,而降低了PEI對銅的鍵結能力,不過透過連續式系統的操作,還原劑(Na2S2O4)會隨著出流水流出,使系統中的離子強度不致累積提升。 總結,以聚電解質加強超過濾(PEUF)結合化學還原法去除及回收重金屬(銅)的實驗中發現,PEI是較合適的聚電解質選項。雖然在瓶杯試驗中,因為奈米顆粒的形成,使得銅的去除率偏低。但透過連續式的系統中,不但顆粒有機會在系統中成長使粒徑增加,進而提升銅的去除率;連二亞硫酸鈉所造成的離子強度影響,也可以透過連續式的系統,將水中的離子強度保持在一定的濃度。 |
英文摘要 |
Chemical reduction was firstly employed to treat synthetic wastewaters of various compositions prepared to simulate the retentate stream of polyelectrolyte enhanced ultrafiltration (PEUF). With fixed Cu:polyethylenimine (PEI) monomer:dithionite molar ratio, increasing copper concentration increases copper removal efficiency. Under fixed Cu:dithionite molar ratio and fixed Cu concentration, increasing PEI monomer:copper molar ratio decreases copper removal efficiency. The formation of nano-sized copper particles, which readily pass through 0.45 μm filter used for sample pretreatment before residual copper analysis, might be the reason behind the decreasing copper removal efficiency observed. Particle size analysis shows that the size of copper particles, which are formed through reduction reaction, increases with decreasing pH value and increasing reaction time. As ultrafiltration is capable of removing these nano-sized particles, integration of chemical reduction and PEUF is proposed to simultaneously achieve regeneration of polyelectrolyte and recovery of copper in one process. Results show that the proposed process could achieve almost complete copper removal without being affected by reaction pH. Three polyelectrolytes (PSS, PAA, and PEI) containing various functional groups and having various molecular weight were also studied to explore their effects on the copper removal in PEUF and on the copper recovery by chemical reduction under various pH conditions. With PSS as the polyelectrolyte, copper was removed reasonably well (75%) by PEUF even under acidic pH value of 3. With PAA which contains carboxylic group, a weak acidic functional group relative to sulfonic group in PSS, copper removal was a bit low (~60%) under pH of 3.0 but increased substantially at pH of 4.0. On the other hand, a branched PEI having amine group interacted with Cu ions through coordination bonding; the highest Cu removal of 94% was obtained at pH of 3 and Cu to PEI monomer molar ratio of 1:5. The copper removal efficiency decreased slightly with increasing pH. The decreasing removal efficiency of Cu at alkaline pH values is due to the high permeation of PEI through membrane compared to both PSS and PAA. For copper recovery by chemical reduction, the complete copper recovery was realized and was almost independent of pH for solution containing PSS. The copper recovery efficiencies were more than 95% for PAA solution with pH values ranging from 3 to 9 at reaction time of one hour. For PEI, the recovery efficiencies ranged from 20~96% and were pH dependent. Aggregated and settled readily copper particles were produced by chemical reduction in PSS solution. XRD analysis identified cuprous oxide in all of the samples collected. Dependent of pH and polyelectrolytes, additional peaks matching those of elemental copper were identified. TGA analysis showed that solids produced from PSS and PAA systems contained no polyelectrolytes while solid collected from PEI system contained 32% of polyelectrolyte. The destruction of polyelectrolyte after chemical reduction was investigated by both fluorescence quenching titration and adsorption breakthrough method. The maximum binding capacity of PEI decreases dramatically for several times of reused causing by increasing of ionic strength, which can be flushed out through the membrane with continuous system. |
第三語言摘要 | |
論文目次 |
List of Figure I List of Table I Chapter 1 Introduction 1 1.1 Background 1 1.2 Objectives and outline of this research 5 Chapter 2 Literature Review 12 2.1 PEUF process 12 2.1.1 The binding mechanism and capacity of different polyelectrolytes 13 2.1.2 The maximum binding capacity of PEI 17 2.1.3 Different methods for maximum binding capacity determination 18 2.1.4 Effects of MW of polyelectrolytes, ligands (EDTA) and ionic strength on PEUF removal 21 2.2 Regeneration of retentate of PEUF 23 2.3 Chemical reduction method 25 2.3.1 Effect of reductant concentration and power on the size of reduced particles 25 2.3.2 Reducing agent used for wastewater treatment and nanoparticle synthesis 26 2.3.3 The reduction potential of different species 27 2.3.4 Effect of capping agent on the size of nanoparticles 31 Chapter 3 Material and methods 33 3.1 Materials and reagents 33 3.2 Analytical method 34 3.3 Experiment method 38 3.3.1 Effective reduction concentration of sodium dithionite 39 3.3.2 Effect of PEI concentration on copper removal efficiency and the size of particles 40 3.3.3 Effect of seed adding on copper removal efficiency 41 3.3.4 Effect of polyelectrolytes and pH on Cu removal efficiency by PEUF (Without reduction process) 42 3.3.5 Effect of pH on copper removal efficiency with chemical reduction process 43 3.3.6 The destruction of polyelectrolytes after chemical reduction 43 Chapter 4 Results and Discussions 47 4.1 Effective operation concentrations of dithionite and Cu(II) 47 4.2 Effect of PEI concentration on copper removal efficiency and the size of particle 49 4.3 Improving copper removal efficiency by seed addition 52 4.4 Effect of polyelectrolytes and pH on Cu removal efficiency by PEUF 53 4.5 Effects of pH and polyelectrolytes on Cu recovery by chemical reduction 64 4.6 The destruction of polyelectrolytes after chemical reduction 70 4.7 Effect of EDTA on copper removal efficiency in PEUF and chemical reduction process 79 4.8 Structural analysis of reduced copper species 85 Chapter 5 Conclusions and suggestions 91 5.1 Conclusion 91 5.2 Suggestion 94 Reference 96 List of Figure Figure 1. The distribution of various heavy metal contaminated farmlands in Taiwan [1]. 2 Figure 2. 10 years zinc and copper prices chart [4]. 4 Figure 3. The schematic of metal removal mechanism in PEUF. (Cu(II) is selected as the target contaminant.) 12 Figure 4. Chemical interaction between PSS, Cu(II) and EDTA. 14 Figure 5. The process of nucleation and growth of nanoparticles by chemical reduction 25 Figure 6. The standard redox potential of various redox couples shows in both pe and mV scales [36]. 30 Figure 7. Preventing particles from aggregation by capping agent 31 Figure 8. The schematic diagram of PEUF system 38 Figure 9. The flow chart of fluorescence quenching titration for Cu(II) to PEI. (R0=Fresh PEI, R1=Reused for one time, R2=Reused for two time, R3=Reused for three times) 45 Figure 10. The collision theory of reaction rates 48 Figure 11. Copper removal efficiency by chemical reduction as a function of copper concentration. Cu:PEI monomer:dithionite molar ratio = 1:1.5:3. pH = 3.5. Reaction time = 30 min. Error bar represents one standard deviation from the mean. 48 Figure 12. Copper removal efficiency in three different PEI monomer:Cu molar ratios. Initial copper concentration = 5mmol/L, pH=6, reaction time = 60 min, and Cu:dithionite molar ratio = 1:3. 50 Figure 13. TEM analysis of particles produced in three different PEI monomer:Cu molar ratios of (A) 1.5:1, (B) 3:1, and (C) 6:1 from Figure 12. 51 Figure 14. Removal efficiency of copper by chemical reduction and PEUF integrated process as a function of pH and reaction time. Cu:PEI monomer:Dithionite molar ratio of 1:1.5:3. Initial copper concentration is 5 mM. 52 Figure 15. Cu removal efficiency as a function of time at pH 9 both with and without seeding. Experimental conditions: Cu:dithionite:PEI molar ratio = 1:3:1.5, initial copper concentration = 5 mM. The concentration of copper seed used was 3.17 mg Cu/L. Error bars represent one standard deviation from the mean of experiments carried out in triplicate. 53 Figure 16. Effect of pH on (A) Cu removal efficiency and (B) TOC permeation with various polyelectrolyes. Experimental conditions: Cu:polyelectrolyte monomer molar ratio = 1:5. Initial Cu concentration = 5 mM. Error bars represent one standard deviation from the mean of triplicate experiments. 55 Figure 17. PEI titration curve from pH 2 to pH 10. PEI concentration is fixed at 30 mM. 0.5 M HNO3 was prepared in the container of piston burette. The titration pH is start from 10 to 2 with automatic speed. 57 Figure 18. Effect of pH on binding capacity of Cu(II) to PEI. (A) Wavelength scans from 250-800 nm (B) The binding percentage and copper removal efficiency of Cu(II) to PEI. The wavelength was fixed at 600 nm. (pH=2-4, Cu(II) concentration=5 mM, PEI concentration = 7.5 mM, 25 mM, 30 mM.) 59 Figure 19. Distribution of Cu(II), Cd(II), and Hg(II) species as a function of pH with presence of ammonia. Modeled with MINEQL+. Total concentrations for Cu, Cd, and Hg are all 5 mM, and that for total ammonia is 25 mM. CuLx ,CdLx and HgLx are Cu/ammonia, Cd/ammonia and Hg/ammonia complexes. For example, CuL3 is Cu(NH3)32+. 63 Figure 20. Copper removal efficiency by chemical reduction as a function of time for solution containing (A) PSS, (B) PAA, and (C) PEI. Cu:polyelectrolyte monomer:Dithionite molar ratio of 1:5:3. Initial copper concentration of 5 mM. pH varied from 3 to 10. Samples were filtered with 0.45-m membrane filters. Error bars represent one standard deviation from the mean of triplicate experiments. 65 Figure 21. Photos of chemical reduction at various pH values for PSS, PAA, and PEI systems at the reaction time of 60 min. Cu: polyelectrolytes monomer: dithionite molar ratio of 1:5:3. Initial copper concentration is 5 mM. Left to Right: pH from 3 to 10. Photo was taken after an hour of settling. 68 Figure 22. Photos of chemical reduction for PSS systems at pH 6 condition. Initial copper concentration of 5mM. Cu:PSS monomer:Dithionite molar ratio of 1:5:3. (The full video could be seen in the following link: (https://www.youtube.com/watch?v=r_aTeJoKWZY) 69 Figure 23. Particle size analysis of particles in PEI system for different reaction times Cu:PEI monomer:Dithionite molar ratio of 1:5:3. Initial copper concentration of 5 mM. pH = 6.0. 70 Figure 24. PEI fluorescence scan for Ex: 200-400 and Em: 250-900 nm. PEI concentration fixed at 12.5 mM. 71 Figure 25. Dependence of the normalized PEI emission intensity with (Ib-I)/(Ib-IMb) as a function of Cu(II)/PEI(monomer) molar ratio. PEI concentration = 12.5 mM (monomer), Cu(II) conc. = 0, 1, 2, 4, 10, 20 mM. pH is fixed at 5. Ex: 205 nm, Em: 340 nm. Virgine PEI. Solid curve is data modeled by Eq. (46). 74 Figure 26. Fluorescence quenching titration of Cu(II) to PEI for several recycling used. PEI concentration = 12.5 mM (monomer), and titrate with Cu(II) from 0-20 mM. The excitation and emission wavelength is fixed at 205 nm and 340 nm. Sodium dithionite concentration for R0-R3 = 0, 15, 30, 45 mM (Please refer section 3.3.6 for the definition of R0-R3). 75 Figure 27. Dependence of the normalized PEI emission intensity with (Ib-I)/(Ib-IMb) as a function of Cu(II)/PEI(monomer) molar ratio for R0 to R3. Solid curves are data modeled by Eq. (46). (Please refer section 3.3.6 for the definition of R0-R3) 76 Figure 28. Adsorption curve of Cu(II) to PEI monomer molar ratio at fixed pH of 5.0 and fixed PEI(monomer) dosage at 0.625 mmol. R0=Fresh PEI, R1=PEI reused for 1 time. (Please refer section 3.3.6 for the definition of R0 and R1) 77 Figure 29. Copper removal efficiency as a function of Cu(II) to PEI monomer molar ratio at fixed pH of 5.0 and fixed PEI(monomer) dosage at 0.625 mmol. R0=Fresh PEI, R1=PEI reused for 1 time. (Please refer section 3.3.6 for the definition of R0 and R1) 78 Figure 30. Copper removal efficiency and TOCeff / TOCinf of PSS enhanced ultrafiltration (10 kDa) with and without EDTA. Cu : EDTA : PSS molar ratio = 1:1:5, initial Cu(II)=5mM. 81 Figure 31. Copper removal efficiency of chemical reduction for PEUF retentate with and without EDTA. The molar ratio for the experiment with EDTA, Cu: EDTA : dithionite : PEI = 1:1:3:5. The molar ration for experiment without EDTA, Cu : dithionite : PEI = 1:3:5. Initial copper concentration = 5 mM. 84 Figure 32. Distribution of Cu(II) species as a function of pH in the presence of EDTA. Modeled with MINEQL+. Total concentrations for Cu and EDTA are both 5 mM. 84 Figure 33. XRD analysis of solid samples collected from the reduction of (A) Cu/PSS and (B) Cu/PAA solutions at various pH values. 86 Figure 34. TEM images of reduced copper particles collected from PEI system. (1.212 nm / 5 peaks = 0.242 nm). 87 Figure 35. TGA analysis of solid samples collected from the reduction of Cu in polyelectrolyte solution at pH of 6 for PSS and PAA systems, and pH of 3 for PEI system. Cu: polyelectrolyte monomer: dithionite molar ratio =1:1.5:3. Initial Cu concentration of 5 mM. N2 gas flow of 100 mL/min. 90 Figure 36. TEM images of reduced copper particles collected from PEI system at pH 3.5. 90 List of Table Table 1: TOP 5 contaminated regions and their corresponding contaminants in Taiwan[3] 2 Table 2: Irrigation water quality standard from council of agriculture and Effluent Standards from Taiwan EPA 3 Table 3: Specification of polyelectrolytes used in Molinari et al. study [19, 22]. 16 Table 4: The maximum bonding capacities, optimal pH of different structure of PEI from different authors. 18 Table 5: The chemical formula and pe0 value for various species. 30 Table 6: Chemical material 34 Table 7: Polyelectrolyte information 34 Table 8: Experiment flow chart for the effective reduction concentration of sodium dithionite 40 Table 9: Experiment flow chart for effect of PEI concentration on copper removal efficiency and the size of particles 41 Table 10: Experiment flow chart for effect of seed adding on copper removal efficiency 42 Table 11: The flow chart of adsorption breakthrough curve for Cu(II) to PEI. 46 Table 12: The experiment data for copper removal efficiency (%) and TOC in the permeate 56 Table 13: Input of equilibrium constants for Cu, Cd and Hg with ammonium species in MINEQL+. 62 Table 14: Cb and K values for R0-R3 from non-linear regression analysis and Eq. (42). (Please refer section 3.3.6 for the definition of R0-R3) 76 Table 15: The TOC and Cu(II) concentration of permeate for PSS system with and without EDTA. 81 |
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