塑膠食品接觸材料(Food Contact Material, FCM)由於其優異的性能及便利性，國際與國內生產及使用量皆逐年急遽增長，根據2021年歐洲塑膠市場研究小組(Plastics Europe Market Research Group, PEMRG)報告之統計，塑膠材需求量依序為PP（聚丙烯），其次為LDPE（低密度聚乙烯），再次之為HDPE（高密度聚乙烯），然而這些塑膠FCM使用後將造成大量的塑膠廢棄物，進而導致生態系統惡化衍生環境危害，為因應這些環境問題，循環經濟已成為各國推展的目標，其中將再生料替代原生料使用即為其中一項。此作法雖環保，但使用過之塑膠食品接觸材在回收、處理及再製過程中可能會比原生塑膠食品接觸材暴露更多危害物質，因此需確認回收再製過程能否去除這些可能的污染物質，避免造成人體危害。回收再製塑膠食品接觸材中，可能遷移的物質分為兩大類，即有意添加物質(Intentionally Added Substances, IAS)及非有意添加物質(Non-Intentionally Added Substances, NIAS)，其中IAS為塑膠回收再製時須添加之物質，而NIAS可能為添加劑之降解產物、製程之副產物或回收再製之污染物等，其存在無法預料，且可能為對人體有害之物質。有鑑於此，近年來，進行塑膠回收料中IAS及NIAS檢測之非目標物分析極受關注。目前各國研究已於使用塑膠回收料製造之FCM中測得多種IAS及NIAS，但其研究多集中為歐洲，使用之樣本大多也僅以回收PET為主，且僅針對最終成品進行量測，考量各國間塑膠回收料中存有物質可能不同、回收再製製程中各步驟對塑膠回收料成品中IAS與NIAS之影響，以及再製塑膠料PP及HDPE未來使用於塑膠FCM之可能性，本研究之目的為建立以氣相層析質譜儀(GC-MS)與液相層析四極柱串聯時間飛行式質譜儀(LC-QTOF)之非標的物分析流程，鑑別塑膠回收料PP（以下簡稱rPP）及HDPE（以下簡稱rHDPE）中IAS及NIAS之分析方法，確認我國rPP及rHDPE中IAS及NIAS化合物種類，探討回收製程各步驟中對去除IAS及NIAS之影響，並針對定性結果中優先測得之鄰苯二甲酸酯類、苯類、醛酮類、全氟烷基化合物，以及有機磷耐燃劑等物質進行定量分析，瞭解其濃度分布，最後進行歐盟之安全性評估，以確認rPP與rHDPE再製為FCM之妥適性。
本研究與國內一間回收廠進行合作，收集國內之回收食品接觸材HDPE牛奶瓶與PP飲料瓶，並於有去味與無去味兩種製程各別設置7個與6個採樣點，將樣本以二氯甲烷進行萃取後，吹氮濃縮並以甲醇回溶，過濾後以GC-MS及LC-QTOF各別上機分析，並配合NIST20質譜資料庫、MassBank質譜資料庫，以及自建質譜資料庫(In-house database)進行辨識，經過上述定性分析後，自結果中選定鄰苯二甲酸酯類、苯類、醛酮類、全氟烷基化合物，以及有機磷耐燃劑進行定量，最後進行歐盟之安全性評估，藉由其中挑戰測試所得之擬似污染物殘留濃度，計算再製製程之去污效率，並與模擬殘留濃度比較。
本研究共採集rPP與rHDPE各39份樣本，於GC-MS定性分析結果中共測得10個IAS及1034個NIAS，其中物質種類以Hydrocarbon（碳氫化合物）為最多，Esters（酯類）次之，Alcohol（醇類）佔居第三，以Total peak area為去污指標來看該再製製程對rPP材質及rHDPE材質中物質含量之影響，可發現兩種材質之Total peak area於造粒前之清洗整體呈上升趨勢，但於造粒後皆有明顯下降趨勢，LC-QTOF定性分析結果中共測得8個IAS及2533個NIAS，物質種類以Esters（酯類）為最多，Ketone（酮類）及Acid（酸類）次之，rPP材質及rHDPE材質之Total peak area於造粒前之清洗與造粒後整體皆呈下降趨勢。
定量結果顯示，鄰苯二甲酸酯類以DINP有較高的檢出率及濃度，在解包後樣本以DINP平均濃度最高(4.46 μg/g)；瓶片樣本以DINP平均濃度最高(7.29 μg/g)；酯粒樣本以DINP平均濃度最高(0.74 μg/g)，將其進行Mann-Whitney U檢定，清洗前瓶片相對清洗後瓶片樣本中DINP濃度並無統計上差異，於清洗前瓶片相對酯粒樣本則有顯著差異，平均去污效率為83.39%。苯類檢出率及濃度較高之物質為toluene，在解包後樣本以toluene平均濃度最高(0.28 μg/g)；瓶片樣本以toluene平均濃度最高(0.36 μg/g)；酯粒樣本以toluene平均濃度最高(0.27 μg/g)，toluene於清洗前瓶片相對清洗後瓶片樣本以及酯粒樣本之濃度皆無統計上的差異，表示再製製程對於苯類雖不具明顯清洗效果，但於最終產物中最高濃度之苯類化合物toluene平均濃度也遠低於1μg/g。醛酮類以acetaldehyde有較高的檢出率及濃度，在解包後樣本acetaldehyde平均濃度最高(6.08 μg/g)；瓶片樣本以acetaldehyde平均濃度最高(1.18 μg/g)；酯粒樣本以acetaldehyde平均濃度最高(0.65 μg/g)，於清洗前瓶片相對清洗後瓶片樣本以及酯粒樣本，acetaldehyde濃度皆具顯著差異，其去污效率分別為80.68%與89.27%。全氟烷基化合物檢出率及濃度較高之物質為PFODA，解包後樣本以PFODA平均濃度最高(7.01 ng/g)；瓶片樣本以PFODA平均濃度最高(6.63 ng/g)；酯粒樣本以PFODA平均濃度最高(7.88 ng/g)，PFODA於清洗前瓶片相對清洗後瓶片樣本以及酯粒樣本之濃度皆無統計上的差異，代表再製製程對於全氟烷基化合物雖無明顯清洗效力，但最終產物中最高濃度之全氟烷基化合物PFODA平均濃度也低於10 ng/g。有機磷耐燃劑檢出率及濃度較高之物質為TBOEP，解包後樣本以TBOEP平均濃度最高(10.54 ng/g)；瓶片樣本以TNBP平均濃度最高(2.15 ng/g)；酯粒樣本以EHDPP平均濃度最高(0.68 ng/g)，TBOEP於清洗前瓶片相對清洗後瓶片樣本中濃度並無統計上差異，於清洗前瓶片相對酯粒濃度則具顯著差異，其平均去污效率為 93.9%，綜上所述，由結果可知造粒於再製製程中確實有其必要性。
安全性評估中挑戰測試結果顯示，浸泡之四種擬似污染物甲苯、二苯酮、氯仿、二十四烷中，浸泡之四種擬似污染物甲苯、二苯酮、氯仿、二十四烷中，以甲苯於rHDPE及rPP之酯粒中具有較高的殘留濃度，且rPP酯粒之殘留濃度較rHDPE酯粒高出1-22倍，將結果套入去污效率之公式後，可得該再製製程對回收塑膠材rHDPE材質及rPP材質之去污效率皆達99％以上，最後將計算得之Cres，與本研究建立之四種擬似污染物於rPP材質及rHDPE材質中的Cmod進行比較，結果可發現所有物質之Cres皆遠低於Cmod，證明該再製製程具足夠之去污效果，其再製酯粒造成人體危害之機率甚微，同時也代表回收塑膠材rHDPE及rPP兩種材質再製為酯粒後，將其使用於FCM確實有其可行性。

In recent years, the use of plastic food contact materials (FCM) has increased, especially polyethylene (PE), polypropylene (PP), and polyethylene terephthalate (PET). Based on the concept of circular economy, recycled plastic should be used in plastic bottles following the regulation of the directive EU 2019/904 issued by European Union. However, these plastic FCMs made by recycled plastics may have a risk to harm human health because they may be contaminated by intentionally added substances (IAS) and non-intentionally added substances (NIAS) during the misuse or recycling process. These contaminants may migrate to the food. Therefore, the present research aimed to establish a method by conducting qualitative and quantitative analysis to identify IAS and NIAS in recycled plastic FCM by GC-MS and LC-QTOF. Moreover, the safety assessment was implemented to check the feasibility that recycled plastic materials could be used as FCM.
In the qualitative analysis of the material test, A total of 10 IAS and 1034 NIAS were detected by GC-MS, and Hydrocarbon was the most species of substances; while a total of 8 IAS and 2533 NIAS were detected by LC-QTOF, and the most species of substances was Esters. In the quantitative analysis of the material test, the highest concentration substances were TBOEP, PFODA, Acetaldehyde, Toluene, and DINP. Finally, through the challenge test, it shows that the decontamination efficiency of the recycling process for the rHDPE and rPP is above 99.9%, and the safety assessment confirms the feasibility that rPP and rHDPE could be used as FCMs.

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