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          我所焚燒源高毒性氯代芳構化合物生成機制研究取得新進展

            近日,我所生態環境評價與分析研究組(103組)陳吉平研究員和張海軍研究員團隊,在焚燒煙氣中高毒性氯代芳構化合物的氯化生成機制研究中取得新進展,相關研究成果以全文的形式發表于《環境科學與技術》(Environmental Science & Technology)雜志上。該工作被期刊選為當期的Supplementary Cover。

            固體廢棄物焚燒和鐵礦石冶煉等燃燒過程會產生大量的芳構化合物,如苯、酚、聯苯、多環芳烴及類似物等,并伴有氯化物(金屬氯鹽和HCl)、Cl2和氯自由基(Cl·)的生成和揮發。這些芳構化合物和含氯粒子在煙氣中可發生復雜化學反應生成氯代芳構化合物,如二噁英、多氯聯苯、多氯萘和氯代多環芳烴等(Chemosphere,2019)。這些氯代化合物具有強烈的“致癌、致畸和致突變”毒性,被聯合國環境署列入持久性有機污染物名錄,為環保領域重點監控污染物。芳烴氯化反應是控制焚燒煙氣中氯代芳構化合物生成的關鍵步驟。由于參與反應的物質極其復雜,并且涉及的基元反應眾多,長期以來人們對焚燒過程中高毒性氯代芳構化合物的氯化生成機制缺乏系統深入的認知,這在一定程度上限制了相應減排控制技術的發展。

            在本工作中,該團隊通過模擬焚燒煙氣反應氛圍,以萘為模式化合物,研究了焚燒煙氣中可能存在的Cu、Fe、Mn、Cr、Co、Ni、Al、Ti、Pb和Zn的氧化物和氯化物對芳構化和物親電氯化的影響,發現銅(Ⅱ和Ⅰ)和鐵(Ⅲ和Ⅱ)的氯化物是促進萘氯化的關鍵活性物質。結合銅鐵粒子晶型結構變化分析,首次揭示了煙氣中銅和鐵粒子通過脫氯-氧氯化循環驅動芳構化合物親電氯化的反應機制。氯化銅(Ⅱ)和氯化鐵(Ⅲ)可作為氯化劑直接誘導芳構化合物氯化。在銅粒子的脫氯-氧氯化循環中,由氯化銅(Ⅱ)誘導的直接氯化是芳構化合物氯化的主要機制;在鐵粒子的脫氯-氧氯化循環中,直接氯化和催化氯化發揮的作用相當。萘的親電氯化符合電子云密度函數理論,1和4位點優先發生氯取代反應。

            基于對焚燒過程氯代芳構化合物氯化生成機制的深入認識,該團隊已研發出焚燒源二噁英等氯代芳構化合物生成抑制技術,目前已在3家大型城市生活垃圾焚燒發電廠應用示范。

            上述研究工作得到我所科研創新基金、國家自然科學基金面上項目和國家重點基礎研究發展計劃(973計劃)的資助。(文/圖 王丹 張海軍)

          版權所有 © 中國科學院大連化學物理研究所 本站內容如涉及知識產權問題請聯系我們 備案號:遼ICP備05000861號 遼公網安備21020402000367號
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