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年度	110	專案性質	實驗性質
專案類別	研究專案	研究主題	調查
申請機構	國立臺灣大學	申請系所	食品安全與健康研究所
專案主持人	陳玟伶	職等/職稱	助理教授
專案中文名稱	沼液再利用對土壤中非目標新興污染物分布之影響
中文關鍵字	沼液, 土壤, 新興污染物, 高解析質譜, 化學輪廓
專案英文名稱	Effects of biogas slurry reuse on the distribution of emerging contaminants in soil
英文關鍵字	biogas slurry, soil, emerging contaminants, high-resolution mass spectrometry, chemical profiles
執行金額	920,000元
執行期間	2021/3/19 至 2022/2/28
計畫中文摘要	沼液可部分取代化學合成肥料、增加土壤肥份。然而動物用藥等新興污染物，可能隨著沼液灌溉而進入農地土壤。傳統之目標物分析法難以發現非預期的環境問題，非目標分析法不預設立場地收集化學資訊，有利於偵測未知污染物、提前發現不斷推陳出新的新興污染物。本計畫利用非目標分析法，探討利用沼液灌溉農地對土壤中新興污染物分布的影響。 本計畫進行田間試驗，分析在實際栽種作物（青江菜）之情境下的土壤。試驗田分為三組，分別是施灌正常量（每年每公頃不超過400公噸）與過量沼液（正常量的三倍）兩組實驗組、以及不施灌沼液的空白組。我們採集試驗開始前的背景土壤（500 g，n=9）及三期作物採收時的表層土壤（每期每組n=6），分析其物理化學性質、肥力、重金屬、微生物活性。土壤樣本另經過萃取與淨化，以高解析質譜法擷取所有非目標小分子（m/z 70−1100）的訊號，並從所有小分子中篩查與鑑定新興污染物。重金屬與新興污染物以多變量分析比較它們在實驗組與對照組中之整體分布；並以單變量分析之統計檢定結果判斷個別金屬元素與新興污染物是否隨沼液施灌量增加而在土壤中增加，藉以發掘與施灌沼液有關的特徵新興污染物。此外，我們也採集每批施灌農地的沼液，分析酸鹼度、飽和電導度、重金屬含量、並篩查新興污染物，以了解其特性。 本計畫成功完成栽種三期作物的田間試驗與土壤及沼液分析。研究結果發現試驗田之各組土壤重金屬濃度均符合農地管制標準。但是施灌過量沼液，使磷、鉀、鎂、錳、銅、鋅、鈉在土壤中濃度顯著增加 (p < 0.05)，可能造成營養鹽累積；所幸並未發現鉛、鎘等有毒重金屬因施灌沼液而增加之趨勢。微生物活性分析結果顯示：施灌沼液使土壤微生物相改變，尤其好氧菌活性下降（最低活性強度為2），可能有較多厭氧菌隨沼液進入土壤，並長期存活於土壤中。非目標分析結果，在土壤和沼液共發現146種新興污染物，其中有24種化合物只出現於施灌沼液的土壤樣本。半定量結果發現，包括畜牧業常用之抗生素 (lincomycin、tiamulin、tilmicosin和oxytetracycline)、殺真菌劑、鎮痛解熱劑、藥品保存劑在內，共有11種新興污染物在施灌沼液的土壤中濃度較高（至少1.49倍，p < 0.05），且有6種污染物隨施灌量增加而增加。所幸季節比較結果顯示這些特徵新興污染物並未隨著重複施灌沼液而增加，應無長期累積之趨勢。 依據本計畫研究結果，建議收集動物停藥時之糞尿為沼液原料、針對藥物研發處理技術、鼓勵合理化施肥、以及持續監測常用動物用藥在沼液與土壤中的分布。期望透過這些對策，使畜牧糞尿資源化政策之推動更臻完善，促進農牧產業與環境生態永續發展。
計畫英文摘要	Biogas slurry can partially replace synthetic fertilizers and increase soil fertility. However, emerging contaminants such as veterinary drugs may enter the agricultural soil through irrigating biogas slurry. Conventional targeted analyses would fail to discover unexpected environmental issues. Untargeted analyses enabled the unbiased collection of chemical information, facilitating the identification of unknown contaminants and the early detection of emerging contaminants. In this project, untargeted analysis was employed to investigate the effect of biogas slurry irrigation on the distribution of emerging contaminants in the agricultural soil. Field experiments were conducted in this project. We analyzed the soil under the actual crop planting circumstance. Three groups were included, which were two experimental groups, irrigating with a normal amount (≤ 400 mt/ha/year) and excessive (three times the normal) biogas slurry, and a blank group without biogas slurry. The background soil (500 g, n=9) sampled before the experiment and the topsoil at the three harvests (n=6 in each group) was collected and analyzed for physicochemical properties, fertility, heavy metals, and microbial activity. Further, After sample extraction and cleanup, untargeted small molecules (m/z 70−1100) in the soil were acquired using high-resolution mass spectrometry. The emerging contaminants were screened and identified from all the small molecules. The overall distribution of heavy metals and emerging contaminants among the control and experimental groups were compared using multivariate analysis. Univariate statistical tests were employed to evaluate the differences in the distribution of individual metals and emerging contaminants, uncovering emerging contaminants relevant to biogas slurry irrigation. In addition, we analyzed the pH, saturation conductivity, and heavy metal content, and screened the emerging contaminants in each batch of biogas slurry to understand its characteristics. Three field harvests, as well as soil and biogas slurry analyses, were completed in this project. The results demonstrated that the concentrations of heavy metals in the soils were all in line with the agricultural land control standards. However, excessive application of biogas slurry significantly increased the concentrations of phosphorus, potassium, magnesium, manganese, copper, zinc, and sodium in the soil (p < 0.05), which may cause nutrient accumulation. Fortunately, the increase in hazardous metals such as lead and cadmium was not found. The application of biogas slurry changed the microbiota in soil, resulting in a decrease in aerobic bacteria activity (minimum activity intensity as low as 2), indicating the existence of more anaerobic bacteria in the soil. Untargeted analysis facilitated the identification of 146 emerging contaminants in soil and biogas slurry, of which 24 only occurred in soil samples irrigated with biogas slurry. Further, the relative concentrations of 11 emerging contaminants were higher in the soil irrigated with biogas slurry (at least 1.49 times, p < 0.05), including antibiotics commonly used in animal husbandry (lincomycin, tiamulin, tilmicosin and oxytetracycline), fungicides, analgesics, and a pharmaceutical preservative. Six emerging contaminants increased with the amount of biogas slurry applied. Fortunately, the seasonal comparison results demonstrated that those marker emerging contaminants did not increase with repeated application of biogas slurry, and long-term accumulation was not observed. According to the research results of this project, we suggest collecting animal urine and manure during withdrawal as the raw materials of biogas slurry, developing veterinary drug treatment techniques, encouraging rational fertilization, and regular monitoring of commonly used veterinary drugs in biogas slurry and soil. We anticipate that these countermeasures will integrate the recycling of animal manure and urine and promote the sustainable development of agriculture and livestock industry and the environment and ecology.