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  • 化學與材料學院劉春元教授課題組在Nat. Commun.發表重要研究成果并獲SCIENCE CHINA Chemistry亮點評述

    發布單位:人員機構 [2019-05-21 08:48:21] 打印此信息

    近日,化學與材料學院劉春元教授課題組在Nature子刊Nature Communications(IF:12.353)上發表了題為“Efficient electron transfer across hydrogen bond interfaces by proton-coupled and -uncoupled pathways”的原創性研究論文,我校為第一完成單位,劉春元教授為唯一通訊作者。

    (期刊截圖)

    氫鍵普遍存在于化學和生物體系,其強度介于化學鍵和范德華力之間,因此對相關體系的結構、性質和反應過程起著重要的調控作用。跨過氫鍵的電子轉移是一個重要的基礎科學問題,也是長期以來的一個非常活躍的研究領域。通過研究,在分子水平上建立電子和質子運動及相互作用的規律性認識,對于揭示生物體系內各種酶、蛋白及DNA內電子轉移過程有著重大意義。該領域研究的核心問題是電子轉移通過氫鍵界面的動力學過程和反應機理。

    該項研究利用鍵合雙鉬(Mo2)金屬配位單元作為電子給、受體構筑了氫鍵、p和s共價鍵三種類型的混價D-B-A體系,在Marcus電子轉移經典理論框架下,應用Hush譜學分析方法,獲得了體系長距離(~ 12 ?)通過氫鍵的電子偶合矩陣元(Hab)和熱誘導電子轉移速率(ket~1010s-1)。研究發現,氫鍵界面的熱誘導電子轉移速率與p共價鍵相近,但明顯大于s鍵;氫鍵強度和電子偶合程度兩種因素共同調控電子轉移的速率并決定反應機理。該研究既驗證了現存的PCET(proton-coupled electron transfer)理論,還發現電子轉移不引起質子遷移的現象,由此提出了質子未偶合電子轉移(Proton-uncoupled electron transfer,PUET)途徑。

    質子未偶合電子轉移(PUET)機理的提出突破了質子偶合電子轉移(PCET)理論的局限,開始從一個新透視角度探討通過氫鍵的電子轉移問題。由于PUET途徑不受質子移動時標的限制,電子通過氫鍵界面遷移速率可能更快,距離更長。PUET機理可用于闡述生物體復雜的電子轉移過程。例如,DNA光修復酶光活化過程中發生的連續多步長程電子轉移,但質子遷移發生在最后一步以滿足電荷平衡。接下來需要解決的問題是,在核量子效應和分子動力學層次深刻揭示氫鍵體系高效傳遞電子的內在因素,準確、定量地描述PUET動力學。

    這一研究成果被SCIENCE CHINA Chemistry期刊進行亮點評述(2019,DOI:org/10.1007/s11426-019-9496-x)。該研究工作得到了國家自然科學基金、廣東省自然科學基金和我校的資助。

    論文鏈接:https://www.nature.com/articles/s41467-019-09392-7

    (化學與材料學院)



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