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          我所在Chem上發表甲烷溫和條件下直接催化轉化研究綜述

            近日,我所催化基礎國家重點實驗室鄧德會研究員和包信和院士團隊在Chem上發表綜述文章,系統總結并展望了熱催化、電催化、光催化技術在甲烷溫和條件下直接轉化方面的研究進展。

            甲烷是天然氣、頁巖氣、可燃冰等的主要成分,是一種豐富的自然資源,它不僅被大量用作燃料供給,也是眾多工業化學品的源頭原料。因此,甲烷的催化轉化在工業和學術界引起了廣泛的研究興趣。然而,甲烷分子的高度穩定性,以及高的C-H鍵能使其在溫和條件下的活化或轉化極具挑戰,甲烷的選擇活化和定向轉化也因此被認為是催化化學領域中的圣杯式課題。目前,工業上甲烷的轉化主要是經水蒸氣重整制備合成氣(Syngas,一氧化碳和氫氣的混合氣),以及合成氣后續進一步轉化成各類有機化學品。該路線中甲烷水蒸氣重整過程通常需要在高溫(700°C-1100°C)條件下進行,合成氣的后續轉化也通常需要高溫高壓等苛刻條件,這增加了該過程的經濟成本和環境壓力。因此,探索溫和條件下甲烷直接轉化制備高附加值的化學品的技術是一個迫切但又極具挑戰的課題。

            該綜述系統總結了熱催化、電催化、光催化在甲烷溫和條件下轉化的研究進展,尤其對其中具有優異C-H活化能力的催化劑進行了重點介紹,在催化劑設計、理論計算模擬、反應條件的選擇、產物精確定量等方面進行了詳細的論述。綜述展望了未來甲烷活化和轉化的發展方向,指出了將來開發低溫下利用氧氣進行甲烷轉化的迫切性,指出限域單中心活性位點以及多組元催化劑在未來甲烷低溫催化轉化方面的重要性,并提出采用多能(熱、電、光)耦合進行甲烷催化轉化將有利于集成各種活化方式的優勢以實現更加高效的甲烷轉化。綜述為未來開發更加高效的甲烷轉化新途徑提供了借鑒。

            鄧德會與包信和研究團隊長期聚焦于二維材料及其在能源小分子催化轉化方面的研究(Nature Nanotechnology,2016;Chemical Reviews,2019)。早在2015年,該研究團隊報道了石墨烯限域單鐵原子活性位用于室溫下復雜碳氫化合物的催化氧化(Science Advances,2015)。近期,該團隊發現這種石墨烯限域單鐵原子活性位甚至可以在室溫下催化氧化甲烷,并獲得高附加值的含氧有機化合物(Chem,2018)。這些結果表明二維材料限域活性中心體系在催化C-H鍵活化和轉化方面具有潛在的應用前景。

            以上研究得到了國家科技部重點研發計劃、國家自然科學基金重大項目、中科院前沿科學重點研究項目、中科院潔凈能源創新研究院合作基金項目等資助,這也是獻禮我所七十周年所慶文章之一。(文/圖 孟憲光、高鶴華)

          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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