臺灣博碩士論文加值系統

鐵礦燒結製程中戴奧辛（Polychlorinated dibenzo-p-dioxins and dibenzofurans; PCDD/Fs）及多環芳香烴化合物（polycyclic aromatic hydrocarbons; PAHs）之逸散及其勞工之暴露為重要之環境衛生議題。本研究主題共分成二部分，第一部分為勞工暴露評估：為擬定適當之汙染控制策略，以燒結場勞工血液戴奧辛指標物特徵（indicatory pattern）為基礎，鑑別其主要暴露之汙染源。第二部分為汙染控制：建立直接削減鐵礦燒結製程逸散之戴奧辛及多環芳香烴化合物之有效方法。第一部分研究首先量測燒結場勞工及其附近居民血液戴奧辛濃度，依戴奧辛指標物特徵並彼此比對後，找出與燒結場勞工職業暴露有關之指標性血液戴奧辛。再者收集並分析燒結場中四個不同作業形態之工作場所及三個不同周界環境（背景環境）之空氣戴奧辛濃度。相互比對其戴奧辛指標物特徵後，可得到與四個工作場所職業暴露有關之指標性空氣戴奧辛。最後比對和職業暴露有關之指標性血液及空氣戴奧辛，結果發現在所挑選的受測勞工中，其所有可能與職業暴露有關之汙染源（suspected pollutant sources）皆可以被鑑別。且該汙染源鑑別技術可經由勞工的時間活動模式、呼吸防護具使用狀況及戴奧辛暴露濃度得到驗證，該技術在未來不僅可鑑別勞工之主要暴露汙染源，還可以應用於其他暴露族群經由各種汙染源及途徑暴露。在第二部分研究，利用田口實驗設計法（Taguchi experimental design），決定最佳操作條件來直接降低鐵礦燒結製程中所產生之戴奧辛及多環芳香烴化合物逸散。所選用之四種操作參數包括含水量(Wc; range = 6.0?7.0 wt%)、抽氣壓力(Ps; range = 1000?1400 mmH2O)、燒結床高度(Hb; range = 500?600 mm)及墊料成分 (HL; 包括燒結礦(sinter), 赤鐵礦(hematite)及褐鐵礦(limonite))。實驗設備為模擬燒結實場各種操作條件之燒結鍋（sinter pot）。若只考量以削減戴奧辛逸散為目的，其結果與目前燒結實場所採用之操作條件（參考操作條件）(reference combination; Wc = 6.5 wt%, Hb = 550 mm, Ps = 1200 mmH2O, and HL = sinter)相較下，最佳操作條件(optimal combination; Wc = 6.5 wt%, Hb = 500 mm, Ps = 1000 mmH2O, and HL = hematite)可有效降低總戴奧辛毒性當量排放系數(EFPCDD/Fs) 62.8%。經由ANOVA分析後，Wc為主要降低EFPCDD/Fs之顯著操作參數，其貢獻度達74.7%。若單獨以控制多環芳香烴化合物逸散為考量，相較於參考操作條件，其最佳操作條件(Wc = 6.5 wt%, Hb = 600 mm, Ps = 1400 mmH2O, and HL = limonite)可削減總BaP毒性當量排放系數(EFBaPeq) 達 57.6%。Ps 及 Hb二者為主要顯著影響總EFBaPeq之操作參數，分別貢獻70.9% 及21.2%。本研究除分別降低戴奧辛及多環芳香烴化合物之逸散外，與燒結製程有關之重要燒結效益指標：燒結產率（sinter productivity; SP）與燒結強度（sinter strength; SS）也同時被評估。若以提高燒結產率為優先考量進行評估，其燒結產率從參考操作條件到最佳操作條件(i.e., Wc = 7.0 wt%, Ps = 1400 mmH2O, Hb = 500 mm, and HL= hematite)可有效提高20.2%。Wc與Ps為主要顯著影響之操作參數，二者可分別貢獻50.3%及36.7%。若只以提高燒結強度為目的，相較於參考操作條件之實驗結果，其最佳操作條件(i.e., Wc = 6.5 wt%, Ps = 1200 mmH2O, Hb = 600 mm, and HL = hematite)卻只能小幅提升2.2%，且所選用之四種操作參數及其水準對燒結強度皆無顯著影響。最後計算戴奧辛及多環芳香烴化合物逸散所導致之致肺癌風險，在同時考量風險與其對應之燒結效益（燒結產率與燒結強度）下進行風險效益分析（risk-benefit analysis）。以風險效益比(risk-benefit ratio; RBR)作為評估指標，將所得之計算結果再利用上述之田口實驗設計法來決定最佳操作參數。最佳操作參數(Wc = 6.5 wt%, Hb = 600 mm, Ps = 1400 mmH2O, and HL = hematite)結果與參考操作條件比較後，發現RBR可顯著降低68.6%，且致肺癌風險可降低49.8%（EFPCDD/Fs及EFBaPeq分別降低55.8%與58.6%），對應之燒結效益可提高10.1%（SP及SS分別提高10.2%與1.5%）。Ps為主要顯著影響參數(p = 0.012)，貢獻度可達48.6%。該最佳操作條件未來可應用於燒結實場，來降低戴奧辛及多環芳香烴化合物所造成之環境衝擊與勞工暴露並同時提升燒結效益。

Emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs) from iron ore sintering processes and their exposures to workers are an important environmental health issue. This is a two-part study. In the first part, we conducted exposure assessment for workers based on the indicatory pattern of PCDD/F concentrations in blood to identify the main pollutant sources for initiating emission control purpose. In the second part, we developed a direct control method for reducing PCDD/F and PAH emissions from sintering process. For the first part of the study, we measured blood PCDD/F concentrations of sinter plant workers and residents living near the sinter plant. Then, the indicatory pattern of blood PCDD/F concentrations found for residents were compared with those for sinter plant workers to identify workplace-related exposures to PCDD/Fs for each selected worker. We then monitored PCDD/F concentrations in four different sinter plant workplaces and three different ambient environments that served as the background. By comparing the patterns of airborne PCDD/Fs found in ambient environments with those for sinter plant workplaces, exposure-related airborne indicatory PCDD/Fs for each workplace were obtained. Finally, by matching exposure-related blood indicatory PCDD/Fs with exposure-related airborne indicatory PCDD/Fs, all suspected pollutant sources were identified for each selected worker. By matching exposure-related blood indicatory PCDD/Fs with exposure-related airborne indicatory PCDD/Fs, two to three suspected pollutant sources were identified for each selected worker. The developed integrated approach can identify all suspected pollutant sources effectively for selected workers based on their blood concentrations of PCDD/Fs. The identified pollutant sources are theoretically plausible since they can be verified by examining workers’ time/activity patterns, their status in using dust respirators, and the concentrations of PCDD/Fs found in the selected workplace atmospheres. The developed technique can be used to identify possible pollutant sources not only for workers but also for many other exposure groups associated with various emission sources and exposure routes in the future.
For the second part of the study, we tried to reduce PCDD/F and PAH emissions separately from the iron ore sintering process by optimizing its operation parameters using the Taguchi experimental design. Four operating parameters, including the water content (Wc; range = 6.0?7.0 wt%), suction pressure (Ps; range = 1000?1400 mmH2O), bed height (Hb; range = 500?600 mm) and type of hearth layer (HL; including sinter, hematite, and limonite) were selected. The experiments were conducted using a pilot-scale sinter pot to simulate various sintering operating conditions of a real-scale sinter plant. If we only considered the abatement of PCDD/F emissions, we found that the resultant optimal combination (Wc = 6.5 wt%, Hb = 500 mm, Ps = 1000 mmH2O, and HL = hematite) can decrease the emission factor of total I-TEQ (total EFPCDD/Fs) by 62.8% in comparison with the current operating condition of the real-scale sinter plant (Wc = 6.5 wt%, Hb = 550 mm, Ps = 1200 mmH2O, and HL = sinter). Through analysis of variance (ANOVA), Wc was found to be the most significant parameter in determining total EFPCDD/Fs (accounting for 74.7% of the total contribution of the four selected parameters). If we only considered PAH emissions control, the emission factor of total BaP equivalent concentration (EFBaPeq) from the reference combination to the optimal combination (Wc = 6.5 wt%, Hb = 600 mm, Ps = 1400 mmH2O, and HL = limonite) was decreased by 57.6%. Ps and Hb were the top two parameters affecting total EFBaPeq (accounting respectively for 70.9% and 21.2% of the total contribution of the four selected parameters). In addition to reduce PCDD/F and PAH emissions, their corresponding sinter output benefit (sinter productivity (SP) and sinter strength (SS)) of sintering process has also been evaluated. Both the SP and SS for their optimal operation combinations were also obtained. By only considering the enhancement of SP, the resultant optimal operation combination (i.e., Wc = 7.0 wt%, Ps = 1400 mmH2O, Hb = 500 mm, and HL = hematite) can increase by 20.2%. Wc and Ps were significant factors for increasing SP in the sintering process, by accounting for 50.3% and 36.7% of the total contribution of the selected parameters, respectively. If we only took SS into account, the increased SS from reference combination to optimal combination (i.e., Wc = 6.5 wt%, Ps = 1200 mmH2O, Hb = 600 mm, and HL = hematite) was 2.2%. There are no significant operational parameters affecting SS. Finally, we considered both the risk associated with PCDD/F and PAH emissions and the corresponding output benefit of sintering process in a risk-benefit analysis. The converted inputs (risk-benefit ratio; RBR) were estimated for determining the optimal operation combination based on the results obtained from the Taguchi experimental design. The decrease of the RBR from the reference combination to the optimal combination (Wc = 6.5 wt%, Hb = 600 mm, Ps = 1400 mmH2O, and HL = hematite) was 68.6%. The estimated lung cancer risk decreased 49.8% (total EFPCDD/Fs and EFBaPeq also decreased by 55.8% and 58.6%, respectively) and the corresponding output benefit of sintering process increased 10.1% (SP and SS also increased by 10.2% and 1.5%, respectively). Ps was a significant parameter (p = 0.012) accounting for 48.6% of the total contribution of the four selected parameters. The optimal operation combination further can be applicable to the real-scale sinter plant for reducing environmental impacts and worker exposures as well as increasing sinter benefits.

Contents
摘要 i
Abstract iii
誌謝 vi
Chapter 1 Introduction 1
Chapter 2 Literature review 5
2.1 Iron ore sintering process 5
2.2 The physical and chemical properties for PCDD/F and PAHs 7
2.3 Toxicity, carcinogen and health effects for PCDD/F and PAHs 13
2.4 Formation mechanism of PCDD/F and PAHs 18
2.5 Emission source of PCDD/F and PAHs 22
2.6 Emission characteristics of PCDD/F and PAHs 29
2.7 PCDD/Fs and PAHs exposure assessment at various workplaces 32
2.8 Control techniques for PCDD/F and PAH emissions 37
2.9 The principle of the Taguchi experimental design 40
2.10 The concept of risk-benefit analysis 40
Chapter 3 Materials and Methods 41
3.1 Study framework 41
3.2 Part 1 — Exposure assessment?the technique for the identification of main exposure source for workers 43
3.2.1 Collection and analysis of airborne samples 43
3.2.2 Subjects and their demographic information 44
3.2.3 Collection and analysis of blood samples 44
3.2.4 Data analysis 45
3.2.5 Calculation of indicatory PCDD/Fs 46
3.2.6 Identification of exposure-related indicatory PCDD/Fs 46
3.3 Part 2? Emission control 50
3.3.1 Pilot scale sinter pot and its operating procedures 50
3.3.2 The Taguchi experimental design 51
3.3.3 Selected operation parameters, levels and orthogonal array 51
3.3.4 Sample samplings 52
3.3.5 Sample analysis 53
3.3.6 Evaluation of sinter productivity and sinter strength 56
3.3.7 Data analysis 56
3.3.8 Risk-benefit analysis 57
Chapter 4 Results and Discussion 63
4.1 Exposure assessment ?Identification of main exposure sources for workers 63
4.1.1 PCDD/Fs in workplace atmospheres and nearby ambient environments 63
4.1.2 PCDD/F exposure concentrations for sinter plant workers 63
4.1.3 Demographic information of all participants 64
4.1.4 Blood PCDD/F concentrations and congener profiles 64
4.1.5 Correlation between worker’s airborne PCDD/Fs exposure and blood concentration of PCDD/Fs 65
4.1.6 Exposure-related airborne indicatory PCDD/Fs 65
4.1.7 Exposure-related blood indicatory PCDD/Fs 66
4.1.8 Identification of suspected pollutant sources 67
4.1.9 Discussion 67
4.2 Emission Control ? determining optimal operation combination for reducing PCDD/F emissions 77
4.2.1 Concentrations and characteristics of PCDD/Fs emitted from the sintering process 77
4.2.2 S/N ratios and ANOVA analysis 77
4.2.3 Comparison PCDD/F emissions between the reference and the optimal operation combination 79
4.2.4 Sinter productivity and sinter strength of the reference and optimal operation combination 80
4.3 Emission control ? determining optimal operation combination for reducing PAH emissions 85
4.3.1 Concentrations and characteristics of PAHs emitted from the sintering process 85
4.3.2 Comparison of PAH characteristics and concentrations between this sinter pot and sinter plants. 85
4.3.3 S/N ratios and ANOVA analysis 86
4.3.4 Comparison PAH emissions between the reference and the optimal operation combination. 87
4.3.5 Sinter productivity and sinter strength of the reference and optimal operation combination 88
4.4 Determining optimal combination to improve sinter productivity and sinter strength 98
4.4.1 SP, SS and their S/N ratio 98
4.4.2 S/N ratio response and ANOVA analysis 98
4.4.3 Comparison SP and SS between the reference and the optimal combination 99
4.5 Determining the optimal operation combination by combining both the decrease of the health risk associated with PCDD/F and PAH emissions and the increase of the corresponding sinter output benefit 106
4.5.1 The need for using a comprehensive approach for the selection of the optimal operation combination 106
4.5.2 Risk-benefit analysis characterization 107
4.5.3 S/N ratio of RBR 107
4.5.4 Comparison of RBR between the reference and the optimal operation combination 108
4.5.5 The explanations for suppressing PCDD/F and PAH emissions using the optimal operation combination based on the risk-benefit analysis combining the Taguchi experimental design 108
Chapter 5 Conclusions 117
References 119

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