結論與建議

5-1 結論

本研究之目的在探討使用鹼性臭氧去除水中全氟碳化物，找尋其降解機制與增加效率之方法，並嘗試將最佳效率操作條件投用於實廠廢水。經實驗後可得到以下之結論：

1. 在中性或酸性條件下，臭氧直接反應無法有效去除水中 PFOA；鹼性條件(pH=11) 下，臭氧能將PFOA 降解至低碳數短鏈形式，其降解效率與所用之臭氧濃度有關，使用2、7、9.5、10.5 wt%之臭氧，4 小時可去除 40 %~60 %的 PFOA，而最佳操作條件為使用2.5 wt%臭氧，PFOA 降解效率可達 90%。

2. 過氧化氫與腐值酸分別為氫氧自由基穩態濃度的增加劑與抑制劑。當使用 2.5 wt%之鹼性臭氧處理 50 ppb 之 PFOA 時，在反應溶液中添加 20 %過氧化氫，

反應2 小時可使 PFOA 降解效率效率從 83 %提升到 98 %；若添加 15 mg/L 腐值酸則會降低PFOA 之降解效率，反應 2 小時之效率從 83 %降低至 39 %。推斷鹼性臭氧去除水中PFOA 之機制為氫氧自由基攻擊目標污染物。

3. 使用 2.5 wt%之鹼性臭氧處理 50 ppb 或 5 ppm 之 PFOA 時，降解效率並無明顯差異，4 小時均可使 PFOA 降解 90 %。當使用 9.5 wt%之鹼性臭氧處理不同濃度PFOA 時，初始濃度 50 ppb 於 4 小時反應時間內降解效率為 43 %，5 ppm 則降解95 %，此結果亦符合擬一階反應原理。

4. 若使用 2.5 wt%之鹼性臭氧外加超音波場源震盪處理 50 ppb 之 PFOA，4 小時僅將效率由90 %提升至 92 %，而超音波場源震盪為一種相當耗能的處理方法，

顯示當使用鹼性臭氧處理PFOA 時，外加超音波場源並非經濟有效的方法。

5. 使用 2.5 wt%之鹼性臭氧處理實廠廢水，6 小時反應時間可去除 PFOA 達 92 %，

顯示鹼性臭氧處理方法亦適合使用於實廠廢水處理PFCs。此外，因臭氧分解水中基質時造成酸性物質形成，處理3 小時後會逐漸使水體酸鹼值呈現中性，不需另外調整放流水酸鹼值，且可將PFOA 去除約 79 %，為一種方便且有效的處理方法。

6. 鹼性條件下臭氧去除PFOA之中間產物，可有效偵測到到全氟庚酸(PFHpA, C7)、全氟己酸(PFHxA, C6)、全氟戊酸(PFPeA, C5)、全氟丁酸(PFBA, C4)與氟離子(F-ion)的生成，故可證明 PFOA在本實驗之設計程序上，可有效的降解至其他碳數較少的全氟碳化合物，使之無害化。

7. 使用 2.5 wt%之鹼性臭氧處理 50 ppb 之 PFOS，4 小時反應時間之效率為 84%，

顯示鹼性臭氧無論PFOA、PFOS 皆可得到良好的去除效果。PFOS 在降解的過程中，偵測到PFOA 的存在，證明鹼性臭氧處理方法可能會促使 PFOS 轉變為 PFOA。

5-2 建議

1. 鹼性臭氧去除水中 PFOS 經初步實驗已證實有效，後續可比照本研究之方法找尋降解PFOS 之最佳操作條件與其作用機制。

2. 鹼性臭氧處理 PFOA 之中間產物、氟離子與所降解之目標污染物無法呈現出質量平衡的狀態，可試圖分析氣相產物濃度，或中間產物、氟離子與其他物質再生成之產物，以完成質量平衡並建立更嚴謹之反應機制。

第六章未來工作

本實驗將處理 PFOA 之最佳操作臭氧濃度套用至 PFOS，但實際上處理 PFOS 之最佳操作條件不一定會與PFOA 相同，因此未來仍需以較嚴謹的方法嘗試找出處理PFOS 之最佳操作條件，並考慮實廠水體中實際 PFCs 濃度，尋找出鹼性臭氧處理PFCs 之最佳化操作條件，以達到經濟與效率兼顧的處理效果。

此外，因本研究使用開放式反應系統，勢必有許多反應中間產物轉化為氣相而散失，導致質量無法平衡，若能設法分析氣相中的產物，必能使研究更臻完美。

值得一提的是，本實驗中曾使用 2.5 wt%臭氧添加 10 mM MtBE，如圖 6-1 所示，亦可得到良好的處理效果，但其作用機制尚未找出，未來可以就此結果延伸研究，以建立更完善的處理方法。

圖6-1. 鹼性臭氧添加 MtBE 處理 PFOA (initial pH=11, ozone: 9.5 wt%, MtBE: 10 mM)

Figure 5-1. PFOA ozonation with MtBE (initial pH=11, ozone: 9.5 wt%, MtBE: 10 mM)

0 10 20 30 40 50 60

0 1 2 3 4

PFOA concentration (ppb)

Time (hr)

Ozone alone

Ozone + 10mM MtBE

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附錄

A02-O3-85W-0 0 50.4 5.92 50.66 0.208806 A02-O3-85W-1 1 51.4 5.01 50.80667 0.531162 A02-O3-85W-2 2 50.3 4.74 50.3 0.1 A02-O3-85W-3 3 50.2 4.56 50.13333 0.057735 A02-O3-85W-4 4 50.2 4.43 49.25333 0.820081 A29-O3-85W-0 0 50.8 5.42

9.5 wt% ozone

A10-O3pH60W-0 0 50.5 0.187409

A10-O3pH60W-1 1 39.3 2.54937

A10-O3pH60W-2 2 32.9 1.95376

A10-O3pH60W-3 3 25.3 2.40762

A10-O3pH60W-4 4 22.1 0.854326

2.5 wt% ozone

O3pH-85W-0 0 50.7 0.208806 O3pH-85W-1 1 16.7 1.653635 O3pH-85W-2 2 8.3 1.637635 O3pH-85W-3 3 7.3 1.764351 O3pH-85W-4 4 5.9 1.85809 7.0 wt% ozone

A11-O3pH190W-0 0 48.7 0.126541

A11-O3pH190W-1 1 36.5 1.75236

A11-O3pH190W-2 2 27.8 1.67398

A11-O3pH190W-3 3 22.9 1.965417

A11-O3pH190W-4 4 18.6 2.054325

9.5 wt% ozone

O3pH-0 0 54.1 2.628688

O3pH-1 1 44.7 2.165641

O3pH-2 2 37.3 1.504438

O3pH-3 3 32.4 1.513275

O3pH-4 4 30.9 1.193035

10.5 wt% ozone

O3pH-470W-0 0 50.0 0

O3pH-470W-1 1 46.1 0.815689 O3pH-470W-2 2 37.9 4.821153 O3pH-470W-3 3 32.4 5.074446 O3pH-470W-4 4 29.2 0.962315

附錄-4 臭氧添加過氧化氫(O

₃

/H

₂

O

₂

)實驗數據

413.0PFOA Time (hr) AVG STD pH

2.5 wt% ozone 0% H2O2

A02-O3pH-85W-0 0 50.66 0.208806 A02-O3pH-85W-15 15 38.5 1.653635 A02-O3pH-85W-30 30 27.7 1.637635 A02-O3pH-85W-1 60 16.71667 1.764351 A02-O3pH-85W-2 120 8.28 1.85809

5% H2O2

A24-5%H2O2-0 0 50.20 0.208167 A24-5%H2O2-15 15 27.00 1.652271 A24-5%H2O2-30 30 17.50 0.757188 A24-5%H2O2-60 60 11.90 0.72111 A24-5%H2O2-120 120 8.10 1.457166

10% H2O2

A28-O3PpH 10H2O2-0 0 50.49 1.487852 A28-O3PpH 10H2O2-15 15 27.03 1.908752 A28-O3PpH 10H2O2-30 30 15.97 0.950438 A28-O3PpH 10H2O2-60 60 12.57 1.28582 A28-O3PpH 10H2O2-2H 120 6.67 2.886751

20% H2O2

A28-O3PpH 20H2O2-0 0 50.43333 0.602771 A28-O3PpH 20H2O2-15 15 25.12778 2.209596 A28-O3PpH 20H2O2-30 30 17.23889 1.855497 A28-O3PpH 20H2O2-60 60 6.930556 1.358112 A28-O3PpH 20H2O2-2H 120 1.111111 0.277555

9.5 wt% ozone 20 mL H₂O₂

A13-O3pH-H2O2-0 0 49.3 10.99

A13-O3pH-H2O2-1 1 15.8 12.05

A13-O3pH-H2O2-2 2 3.59 11.99

A13-O3pH-H2O2-3 3 0.144 11.91

A13-O3pH-H2O2-4 4 0.335 11.87

0.6 mL H₂O₂

A09-O3pH-H2O2-0 0 51.63333 0.172434 A09-O3pH-H2O2-1 1 33.9 1.167604 A09-O3pH-H2O2-2 2 26.13333 1.267057 A09-O3pH-H2O2-3 3 21.9 1.02235 A09-O3pH-H2O2-4 4 19.16667 0.903124

No H₂O₂

A02-O3pH-85W-1 60 16.71667 1.764351 A02-O3pH-85W-2 120 8.28 1.85809

15 mg/L HA

A02-O3pH-85W-HA-0 0 51.60 0.573811 11.01 A02-O3pH-85W-HA-15 15 47.80 4.954945 10.38 A02-O3pH-85W-HA-30 30 43.60 5.327323 9.86

A02-O3pH-85W-HA-1 60 40.50 5.72192 9.26 A02-O3pH-85W-HA-2 120 31.00 3.966106 9.14

9.5 wt% ozone No HA

A02-O3pH-0 0 54.1 2.628688 11.0

A02-O3pH-15 1 44.7 2.165641 10.7

A02-O3pH-30 2 37.26667 1.504438 10.3

A02-O3pH-1 3 32.4 1.513275 10.4

A02-O3pH-2 4 30.93333 1.193035 10.3 15 mg/L HA

A02-O3pH-HA-0 0 50.26 0.40289

附錄-6 初始濃度影響實驗數據

TIME(HR) AVG STD C/C0 (avg) C/C0 STD 2.5 wt% ozone

50 ppb

A-0 0 50.66 0.208806 1 0.004122 A-1 1 16.71666667 1.764351 0.3299776 0.034827 A-2 2 8.28 1.85809 0.1634426 0.036678 A-3 3 7.31 1.113688 0.1442953 0.021984 A-4 4 5.863333333 0.829779 0.1157389 0.016379 5 ppm O3pH-1 1 44.7 2.165641 0.8262477 0.04003 O3pH-2 2 37.26666667 1.504438 0.6888478 0.027808 O3pH-3 3 32.4 1.513275 0.5988909 0.027972 O3pH-4 4 30.93333333 1.193035 0.5717807 0.022052

5 ppm

A14-O3pH5ppm-0 0 52.3 0.565685 1 0.010816 A14-O3pH5ppm-1 1 14.55 2.616295 0.2782027 0.050025 A14-O3pH5ppm-2 2 6.9 0.565685 0.1319312 0.010816 A14-O3pH5ppm-3 3 4.12 2.5173 0.0787763 0.048132 A14-O3pH5ppm-4 4 2.715 2.23 0.051912 0.042639

A02-O3pH-HA15 1 50.28 7.035341 A02-O3pH-HA30 2 47.20 7.401356 A02-O3pH-HA1 3 44.90 7.104028 A02-O3pH-HA2 4 41.71 9.779476

附錄-7 臭氧外加超音波場源影響實驗數據

Time

(hr) AVG STD C/C0

2.5 wt% ozone Sonozone

A02-SO3-85W-0 0 51.09 0.5315 1.000

A02-SO3-85W-1 1 17.30 2.6963 0.339

A02-SO3-85W-2 2 7.63 3.6116 0.149

O3pH-0 0 54.10 2.6287 1.000

RW21-2 120 19.70 8.29

附錄-9 中間產物與反應機制實驗數據

2.5 wt% ozone TIME 413PFOA 363PFHpA 313PFHxA 263PFPeA 213 F-ion A18-O3pH-2.5%-0 0 4580 0.168 0.00 0 0 0 A18-O3pH-2.5%-15 15 2950 10.00 10.50 3.850 10.40 1.68 A18-O3pH-2.5%-30 30 2070 11.60 13.80 4.400 11.20 3.22 A18-O3pH-2.5%-1H 60 1470 10.80 14.40 5.260 12.40 4.84 A18-O3pH-2.5%-2H 120 746 10.00 15.50 5.440 13.00 6.6 A18-O3pH-2.5%-3H 180 651 10.40 16.70 5.560 13.00 8.5 A18-O3pH-2.5%-4H 240 462 10.50 19.90 5.660 13.30 25.85 2.5 wt% ozone+H2O2 TIME 413PFOA 363PFHpA 313PFHxA 263PFPeA 213 F-ion

A18-S O3pH-2.5%-0 0 4310 0 0 0 0 0 A18-S O3pH-2.5%-15 15 1360 7.40 9.300 5.5 4.30 3.56 A18-S O3pH-2.5%-30 30 303 9.48 13.100 8.7 4.300 7.88 A18-S O3pH-2.5%-1H 60 152 12.40 13.700 8.5 4.20 11.68 A18-S O3pH-2.5%-2H 120 146 16.20 15.800 7.5 3.90 20.2 A18-S O3pH-2.5%-3H 180 111 12.60 9.72 8.400 0.00 38.5 A18-S O3pH-2.5%-4H 240 74.8 6.05 7.83 10.170 0.00 44.8

Sonozone TIME 413PFOA 363PFHpA 313PFHxA 263PFPeA 213 F-ion A18-S O3pH-2.5%-0 0 5170 0 0.00 0 0 0

A18-S O3pH-2.5%-15 15 2680 1.61 3.35 1.190 1.23 3.5 A18-S O3pH-2.5%-30 30 2010 2.63 9.80 2.400 0.203 3.8 A18-S O3pH-2.5%-1H 60 1600 2.80 14.40 3.260 0.00 5.4 A18-S O3pH-2.5%-2H 120 880 3.67 15.60 4.740 0.00 8.5 A18-S O3pH-2.5%-3H 180 751 5.40 17.70 5.560 0.00 8.9 A18-S O3pH-2.5%-4H 240 510 7.50 19.90 6.660 0.00 9.2

附錄-10 鹼性臭氧處理 PFOS 實驗數據

413.0PFOA Time (hr) 369.0pair pH AVG STD

S19-O-0 0 0.00 11.05 0 0

S19-O-1 1 4.58 6.93 4.705 0.176777 S19-O-2 2 4.25 7.11 3.685 0.799031 S19-O-3 3 5.24 8.8 4.00625 1.74125 S19-O-4 4 5.93 9.63 4.5225 1.983435

S21-O3-0 0 0 11.01

S21-O3-1 1 4.83 9.08

S21-O3-2 2 3.12 9.47

S21-O3-3 3 2.775 9.61

S21-O3-4 4 3.12 9.81

499.0PFOS Time (hr) 99.0pair pH AVG STD

S19-O-0 0 52.3 11.05 49.625 3.712311 S19-O-1 1 23.5 6.93 24.25 1.06066 S19-O-2 2 13.1 7.11 13.4625 0.477297 S19-O-3 3 7.81 8.8 9.05625 1.758928 S19-O-4 4 7.35 9.63 7.855 0.714178

S21-O3-0 0 47 11.01

S21-O3-1 1 25 9.08

S21-O3-2 2 13.8 9.47

S21-O3-3 3 10.3 9.61

S21-O3-4 4 8.36 9.81

附錄-11 鹼性臭氧添加MtBE處理PFOA實驗數據

413.0PFOA Time (hr) 369.0pair pH AVG STD A23-O3pHMtBE-0 0 64.6 50.5 10.99 50.85938 1.033497 A23-O3pHMtBE-1 1 6.92 5.4 7.19 5.192708 0.503911 A23-O3pHMtBE-2 2 6.05 4.7 7.38 5.869792 1.95313 A23-O3pHMtBE-3 3 12.3 9.6 9.39 9.973958 1.213665 A23-O3pHMtBE-4 4 15.5 12.1 9.85 8.830729 2.943875 A24-O3pHMtBE-0 0 64.1 50.1 11.01

A24-O3pHMtBE-1 1 5.91 4.6 7.25 A24-O3pHMtBE-2 2 10.4 8.1 7.45 A24-O3pHMtBE-3 3 14.5 11.3 8.78 A24-O3pHMtBE-4 4 10.2 8.0 9.54 A25-O3pHMtBE-0 0 66.6 52.0 11.00 A25-O3pHMtBE-1 1 7.11 5.6 7.79 A25-O3pHMtBE-2 2 6.09 4.8 7.75 A25-O3pHMtBE-3 3 11.5 9.0 8.93 A25-O3pHMtBE-4 4 8.21 6.4 9.63

全文完

在文檔中鹼性條件下臭氧去除水中全氟辛酸 (頁 76-97)