臺灣博碩士論文加值系統

本研究探討持久性有機污染物，於兩種生質燃燒條件下之排放情形。首先，於工業鍋爐，燃燒木屑及混燒木屑與工業廢水污泥，觀察污染物排放情形。後續於2010及2013年觀察東南亞地區，露天燃燒多種生質物，或夾雜些許垃圾等露天燃燒研究。於工業鍋爐研究中，吾人設定兩種燃料形式，分別為木屑燃燒情形及試混燒木屑（90%比重）與工業廢水污泥（10%比重），觀察其二者排放溴化戴奧辛/呋喃及多溴聯苯醚之情形。於煙道廢氣污染排放，木屑燃燒之溴化戴奧辛/呋喃及多溴聯苯醚濃度分別為 0.121 pg TEQ/Nm3及2,260 pg/Nm3，而於試混燒情形兩者濃度分別上升至0.211 pg TEQ/Nm3及4,200 pg/Nm3。溴化戴奧辛/呋喃及多溴聯苯醚之特徵剖面，分別於木屑燃燒或試混燒之進料及出料中均相似；而木屑燃燒之進出料亦分別與其試混燒之進出料相似，上述之現象均顯示，木屑燃燒或試混燒均有相同之溴化戴奧辛/呋喃及多溴聯苯醚破壞路徑，且不因加入工業污泥而影響。溴化戴奧辛/呋喃及多溴聯苯醚於此工業鍋爐之宿命顯示，兩種燃料情形均有良好破壞及去除效率(〉93.5%)。溴化戴奧辛/呋喃及多溴聯苯醚釋放主要之路徑，因從木屑燃燒轉換為試混燒，而自煙道廢氣轉變至灰渣中。鍋爐燃燒研究顯示，混燒之技術不僅處理廢棄污泥量迅速增長之問題，亦同節省燃料及廢棄物處理之花費達26.3%。
於大氣傳輸研究，詳細探討東南亞露天燃燒排放之氯化戴奧辛/呋喃、多氯聯苯、多氯聯苯醚、溴化戴奧辛/呋喃、多溴聯苯及多溴聯苯醚等，多種持久性有機污染物之傳輸特性。本研究於生質燃燒上風源區，泰國（2010於清邁而2013於安康山）及越南(2010於峴港而2013於山羅)等地進行空氣採樣，特徵化當地露天燃燒排放之持久性有機污染物，及觀察其對下風受體台灣鹿林空氣品質背景站之影響。2010及2013之研究結果顯示，越南受到當地露天燃燒影響較泰國嚴重甚多。於2010之研究顯示，峴港大氣中溴化持久性有機污染物，包括溴化戴奧辛/呋喃、多溴聯苯及多溴聯苯醚等，其濃度升高係由於生質燃燒所貢獻，當地使用之溴化阻燃劑相關性不大；鹿林空氣品質背景站之兩密集觀察期間，大氣中氯化戴奧辛/呋喃之濃度分別為0.00428及0.00232 pg I-TEQ/Nm3，多氯聯苯之濃度分別為0.000311及0.000282 pg WHO-TEQ/m3，溴化戴奧辛/呋喃之濃度分別為0.000379及0.000449 pg TEQ/Nm3，多溴聯苯之濃度分別為0.0208及0.0163 pg/Nm3，與多溴聯苯醚之濃度分別為109及18.2 pg/Nm3；此些濃度數值顯示，鹿林山大氣受東南亞生質燃燒影響。於2013之研究結果中，山羅及安康山大氣中持久性有機污染物濃度之相關性統計分析結果，與其對應之特徵剖面分析結果相似，顯示兩地區均受該區域之露天燃燒所影響。本年度研究亦有採集PM2.5樣品，且其與燃燒產生之個別持久性有機污染物濃度對應時間之變化，呈現一定之相關性。搭配氣流後推軌跡分析，吾人可使用此相關性，將特定區域大氣中PM2.5濃度，推估未來該區域受露天燃燒影響之持久性有機污染物濃度。

The aim of this research is to investigate the emissions of persistent organic pollutants (POPs) from two types of biomass burnings. An industrial boiler study of woodchip combustion and co-combustion of woodchip and industrial wastewater sludge (IWTS) was conducted and followed by a open field study for various biomass open burnings (or few waste burnings) in the region of Southeast Asia in 2010 and 2013. For the industrial boiler study, the emissions of polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs) and polybrominated diphenyl ethers (PBDEs) from trial combustion of 10 wt% dried industrial-wastewater-treatment sludge (IWTS) and 90 wt% woodchip in an industrial boiler were investigated and compared to that from woodchip combustion. The PBDD/F toxic equivalent (TEQ) and PBDE emissions increased from 0.121 pg TEQ/Nm3 and 2,260 pg/Nm3, respectively, of the woodchip combustion to 0.211 pg TEQ/Nm3 and 4,200 pg/Nm3, respectively, of the trial combustion. PBDD/F and PBDE congener profiles of inputs and outputs of the same type of combustion were similar; they also show similarity between woodchip and trial combustions, revealing that the destruction pathway was little affected by the introduction of the IWTS. The fates of PBDD/Fs and PBDEs show that the indigenous pollutants in the feed were effectively depleted (〉93.5%). The dominant releasing route of PBDD/F and PBDE shifted from the stack flue gas of woodchip combustion to the ashes of trial combustion. The industrial boiler study demonstrates that co-combustion not only handles the fast growing sludge stream, but also yields a saving of 26.3% in the fuel cost and treatment fees of sludge and ashes.
The Southeast Asian biomass burning is the first that comprehensively discusses the long-range atmospheric transport behavior of combustion originated POPs, including polychlorinated dibenzo-p-dioxin and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), polychlorinated diphenyl ethers (PCDEs), PBDD/Fs, polybrominated biphenyls (PBBs), and PBDEs. The POP emissions at the biomass burning sites in Vietnam (Da Nang in 2010 and Son La in 2013) and Thailand (Chiang Mai in 2010 and Doi Ang Khang (DAK) in 2013) were characterized, as well as the influence of the Southeast Asian biomass burnings on the Lulin Atmospheric Background Station (LABS) in Taiwan. The ambient air in Vietnam seems to be more seriously affected by the local biomass burnings than that in Thailand for the Southeast Asian biomass burning study in 2010 and 2013. For the study in 2010, the elevated atmospheric brominated POP (PBDD/Fs, PBBs and PBDEs) concentrations in Da Nang were attributed to the biomass burning and viewed as mostly unrelated to the local use of brominated flame retardants. In the spring of 2010, the mean atmospheric concentrations in LABS during the first and second Intensive Observation Periods (IOPs) were 0.00428 and 0.00232 pg I-TEQ/Nm3 for PCDD/Fs, 0.000311 and 0.000282 pg WHO-TEQ/m3 for PCBs, 0.000379 and 0.000449 pg TEQ/Nm3 for total PBDD/Fs, 0.0208 and 0.0163 pg/Nm3 for total PBBs, and 109 and 18.2 pg/Nm3 for total PBDEs, respectively. These values represent the effects by the Southeast Asian biomass burnings. For the study in 2013, results of statistical analyses on the POP concentrations are individually consistent with the characteristics of POP congener profiles in Son La and DAK, revealing they were influenced by the local burnings. The PM2.5 samples were collected in the 2013 study. Well correlations were found between PM2.5 and each of the biomass burning originated-POPs in the three sites. Based on the backward trajectories, the correlations can be used to predict the (site specific) future biomass burning affected POPs from PM2.5.

摘要 II
Abstract V
誌謝 VIII
Contents IX
List of Tables XIII
List of Figures XV
Chapter 1 Introduction 1
1.1 Background Introduction 1
1.2 Objectives 3
Chapter 2 Literatures Review 5
2.1 POP Emissions from Combustion Sources 5
2.1.1 PCDD/F and PCBs Emissions 5
2.1.2 PBDE Emissions 8
2.1.3 PBDD/F Emissions 10
2.2 Sludge Issue in Asia 11
2.3 Southeast Asian Biomass Burning 14
Chapter 3 Material and Methods 17
3.1 Fuel Properties and Industrial Boiler 17
3.2 Atmospheric Sampling Sites 20
3.3 Sampling Procedures 24
3.3.1 Industrial Boiler Study 24
3.3.2 Atmospheric Transport Study 25
3.4 Analytical Procedures 27
3.5 Quality Assurance/Quality Control 29
3.5.1 Industrial Boiler Study 29
3.5.2 Atmospheric Transport Study 29
Chapter 4 Results and Discussion 35
4.1 Industrial Boiler Study 35
4.1.1 PBDD/F and PBDE Characterizations in the Boiler System 35
4.1.2 PBDD/F and PBDE Congener Profiles in the Input and Output Materials 41
4.1.3 Fates of PBDD/Fs and PBDEs in the Boiler 45
4.1.4 PBDD/F and PBDE Distributions in the Boiler 48
4.1.5 Boiler Efficiency and Sludge Treatment Cost 50
4.2 Atmospheric Transport Study in 2010 51
4-2-1 POP Concentrations in the Atmosphere of the Biomass Burning Sites 51
4.2.2 POP Congener Profiles in the Atmosphere of the Biomass Burning Sites 54
4.2.3 Influence of the Southeast Asian Biomass Burnings on the Atmospheric POPs at LABS 59
4.3 Atmospheric Transport Study in 2013 69
4.3.1 Effects of Biomass Burnings on the Atmospheric PM2.5 Concentrations 69
4.3.2 Characteristic of Atmospheric POPs at the Biomass Burning Sites 77
4.3.3 Characteristic of Atmospheric POPs at the Receptor Site 88
4.3.4 Relationship among the Combustion Originated POPs and PM2.5 91
Chapter 5 Conclusions and Suggestions 95
References 97
Curriculum Vitae 111

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