金原子簇与Lewis酸协同催化醛类加氢
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- 英文论文题名：Experimental and Mechanistic Understanding of Aldehyde Hydrogenation by Gold Cluster with Lewis-Acids: Unique Catalytic Sites
- 论文作者：李志敏 ; 李杲
- 英文论文作者：Zhimin Li ; Gao Li ; Gold Catalysis Research Center ; Dalian Institute of Chemical Physics ; CAS
- 年：2016
- 作者机构：中国科学院大连化学物理研究所;
- 论文关键词：金原子簇 ; 醛类加氢 ; Lewis酸 ; Au_(25)
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十七分会：纳米催化
- 语种：中文
- 分类号：O621.251
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十七分会 ; 纳米催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：354k
- 原文格式：D
- 会议级别：全国
摘要
近十年来,金原子簇以独特的量子效应,使其在纳米科学及纳米技术方面应用受到了广泛关注~([1])。金原子簇在Lewis酸(如Cu~+、Cu~(2+)、Ni~(2+)和Co~(2+)等)协同下对醛类加氢反应表现出很高的催化活性及选择性~([2])。在Au25(SR)_(18)/CeO_2催化剂催化乙醛及其衍生物加氢反应过程中,Lewis酸的加入能够显著提高其催化活性(见左图)。为进一步探索其机理,我们通过MALDI、ESI质谱图及UV-vis光谱图证明了新物种Au_(25-n)(SR)_(18-n)(n=1-4)的产生,并通过DFT计算对Au_(25)(SR)_(18)/CeO_2催化剂在Lewis酸协同下催化醛类加氢反应的机理提出了合理的说明(见右图)。
Over the last decade,atomically precise gold clusters have emerged as a novel and promising nanomaterial in nanoscience and nanotechnology.The addition of a Lewis acid is found to significantly promote the catalytic activity of Au_(25)(SR)_(18) in the hydrogenation of benzaldehyde and a number of its derivatives.The MALDI and ESI mass spectrometry in conjunction with UV-vis spectroscopy confirm the generation of new species,Au_(25-n)(SR)_(18-n)(n = 1-4),in the presence of a Lewis acid.The pathways for the speciation of Au_(24)(SR)_(17) from its parent Au_(25)(SR)_(18) nanocluster as well as its structure are investigated via the DFT method.
Over the last decade,atomically precise gold clusters have emerged as a novel and promising nanomaterial in nanoscience and nanotechnology.The addition of a Lewis acid is found to significantly promote the catalytic activity of Au_(25)(SR)_(18) in the hydrogenation of benzaldehyde and a number of its derivatives.The MALDI and ESI mass spectrometry in conjunction with UV-vis spectroscopy confirm the generation of new species,Au_(25-n)(SR)_(18-n)(n = 1-4),in the presence of a Lewis acid.The pathways for the speciation of Au_(24)(SR)_(17) from its parent Au_(25)(SR)_(18) nanocluster as well as its structure are investigated via the DFT method.
引文
[1]Li,G.;Jin,R.Acc.Chem.Res.2012,46:1749.
[2]Li,G.;Abroshan,H.;Chen,Y.;Jin,R.;Kim,H.J.J.Am.Chem.Soc.2015,137:14295.
[2]Li,G.;Abroshan,H.;Chen,Y.;Jin,R.;Kim,H.J.J.Am.Chem.Soc.2015,137:14295.