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    首頁» 圖片新聞» 吳凱課題組在表面非對稱反應研究中取得進展

    吳凱課題組在表面非對稱反應研究中取得進展

    合成化學和材料科學的快速發展得益于豐富的化學反應“工具箱”。它既包括了多種多樣的化學反應類型,也包括了不斷擴充的反應調控方法學——后者對于提高反應效率和精準程度至關重要。一類重要的反應調控方法被稱為非對稱反應,即通過對反應過程的精細控制,從而在同一分子中多個等價的反應活性位點上分別實現不同的化學反應。借助這類方法,可以從簡單的前驅體出發合成結構復雜的產物。然而,在傳統的濕法合成化學中,受限于反應環境的均一性和不可控性,非對稱反應很難實現。

    針對這一問題,北京大學化學與分子工程學院吳凱課題組進行了相關研究,通過對反應過程的精準控制,在固體表面實現了非對稱反應。研究成果發表在最新一期《自然-通訊》雜志上(Jing Liu, Qiwei Chen, Kang Cai, Jie Li, Yaru Li, Xiao Yang, Yajie Zhang, Yongfeng Wang,* Hao Tang, Dahui Zhao* and Kai Wu,* Stepwise On-Surface Dissymmetric Reaction to Construct Binodal Organometallic Network, Nat. Commun. 2019, 10, 2545)。

    該研究利用1,4-二溴-2,5-二乙炔基苯這一雙官能團分子作為反應前驅體。掃描隧道顯微鏡研究表明,前驅體分子吸附在Ag(111)表面后,兩個等價溴代位點在不同溫度下分步活化,并參與不同的反應:室溫(300 K)下,分子首先選擇性地脫去一個溴原子,脫溴位點與氫原子反應;同時,分子中的炔基發生分子間反應,形成由炔--炔節點連接而成的一維有機金屬鏈狀結構。分子中另一個溴原子的活化需要更高的溫度(320~450 K),形成的脫溴位點則與表面銀增原子反應生成分子間的有機金屬連接,最終得到由炔--炔和炔--苯兩種有機金屬節點有序排列而成的二維結構。密度泛函理論計算進一步揭示了非對稱反應的機理:分子中兩個溴原子解離勢壘的差異導致了二者在不同溫度下分步活化。較低溫度下,炔基的反應提供大量氫原子,促進了脫溴位點與氫的不可逆結合;更高溫度下,表面氫原子耗盡,穩定的分子間有機金屬產物的形成拉動了脫溴位點與銀的反應向右進行。該研究為制備復雜的分子納米結構和高分子提供了新思路。

     

    本文的第一作者為吳凱課題組已畢業的劉婧博士。該工作是與北京大學信息科學技術學院王永鋒課題組、化學與分子工程學院趙達慧課題組以及法國國家科研中心材料制造與結構研究中心(CEMES-CNES)唐浩課題組合作完成的,并得到了國家自然科學基金委員會、科技部以及北京分子科學國家研究中心的經費支持。

    原文鏈接:https://www.nature.com/articles/s41467-019-10522-4

     

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