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    北理工在氣相團簇化學領域取得重要進展

      近日,北理工化學與化工學院馬嘉璧副教授團隊通過質譜實驗、陰離子光電子能譜實驗和高精度量子化學計算相結合的方法對N2與Ta3N3H?和Ta3N3?氣相團簇的反應性及結構進行了深入研究,得到了首例能夠固定并完全活化N2分子的過渡金屬氮化物團簇,揭示了H配體在反應中的重要作用。相關成果以“Dinitrogen Fixation and Reduction by Ta3N3H0,1? Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity”為題,發表在國際重要期刊《Journal of the American Chemical Society 》(IF= 14.695,DOI:10.1021/jacs.9b03168)。化學與化工學院碩士生趙越為該論文的第一作者,馬嘉璧副教授、德國Fritz-Haber研究所的André Fielicke、西華大學的胡連瑞老師為論文的共同通訊作者。

      N2作為惰性分子,其活化和還原是化學中最具挑戰性的課題之一。研究N2的活化反應機制作為一種長期目標激發科研工作者們對各種試劑和氮氣的反應做了大量的實驗和理論研究。工業中N2還原為NH3需要極端的條件來削弱和破壞強 N≡N 鍵。為了克服這一挑戰,科研工作者們通常依靠過渡金屬化合物來提供電子弱化或將N≡N鍵裂解去提高N2的反應活性。除Haber法工業制氨工藝中的Fe催化劑可以活化N2之外,過渡金屬鉭氮、鉭氫化合物也能夠活化N2,其在活化N2時都與活化中心密切相關。在此背景下,研究N2的反應規律以及過渡金屬氮化物和氫化物在活化N2反應中的作用具有重要的科學意義。

    圖1. Ta3N3H0,1- 與N2的反應質譜圖以及355nm的激光波長下Ta3N3H?和產物Ta3N5H?的光電子能譜

      基于以上難點,我校化學與化工學院馬嘉璧副教授團隊利用先進的質譜實驗測量反應性,陰離子光電子能譜實驗研究結構,結合高精度量子化學計算的方法,揭示了Ta3N3H?團簇在N2活化反應中優異的反應性,以及H配體的重要性。實驗表明,Ta3N3H?和Ta3N3?團簇都能徹底活化1分子N2,生成吸附產物Ta3N5H?和Ta3N5?,而前者的反應速率比后者快5倍。深入的理論計算表明:Ta3N3H?和Ta3N3?團簇與N2的反應過程中發生了N2徹底解離現象;此外,2個和3個Ta原子分別是N2還原的活性位點,也是N2還原的電子供體。雖然Ta3N3H?中的氫原子不直接參與反應,但它改變了Ta3N3H?的電荷分布和幾何構型,提高了團簇的反應活性。

      這是室溫下氣相氮化物團簇陰離子完全活化N2的第一個例子,這項工作也突出了氫輔助反應的重要性,為用于N2固定和活化以及合成NH3設計催化劑提供了分子水平的見解。

    圖2. ScNH+ 陽離子與CO2的反應性研究

      此外,該團隊在過渡金屬氮化物陽離子團簇活化CO2方面也取得系列進展。經研究發現:ScNH+陽離子可以高效活化CO2,生成高附加值的有機物異腈酸(HNCO)。這是第一個通過氣相離子介導活化CO2形成HNCO的例子,而且率先在CO2活化中實現了C="N雙鍵的形成。該成果發表在The" Journal of Physical Chemistry A (2019, 123, 5762-5767)雜志上,而且被選為外封面(Front Cover,圖2)。這些工作為認識相關CO2催化反應機理提供了新方法和新思路。

      論文相關鏈接: https://pubs.acs.org/doi/10.1021/jacs.9b03168 https://pubs.acs.org/doi/10.1021/acs.jpca.9b02133

     

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