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首页> 外文期刊>ACS catalysis >Tuning the Product Selectivity of the alpha-Alkylation of Ketones with Primary Alcohols using Oxidized Titanium Nitride Photocatalysts and Visible Light
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Tuning the Product Selectivity of the alpha-Alkylation of Ketones with Primary Alcohols using Oxidized Titanium Nitride Photocatalysts and Visible Light

机译：使用氧化钛氮化钛光催化剂和可见光调节酮烷基烷基化酮烷基化的产品选择性

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摘要

The direct alpha-alkylation of ketones with alcohol to synthesize important alpha-alkylated ketones and enones is an attractive procedure for C-C bond formation. High reaction temperatures are always needed for heterogeneous catalysis using non-noble metals, and switching product selectivity in one catalysis system remains a great challenge. In the present study, a visible-light-driven procedure for this reaction is proposed, using oxidized TiN photocatalysts under mild conditions, whereby the product selectivity can be well-tuned. Oxidized TiN photocatalysts with tunable surface N/O ratios were successfully synthesized through the facile and flexible thermal oxidation treatment of low-cost TiN nanopowder. The alpha-alkylation of acetophenone with benzyl alcohol to form the two important compounds chalcone and dihydrochalcone occurred even at room temperature and almost complete conversion was achieved at 100 degrees C under visible light. The proportion of the two products can be well-tuned by switching the surface N/O ratio of the synthesized photocatalysts. Visible light is demonstrated to affect the surface N/O ratio of the photocatalysts and contribute to tuning the product selectivity. Light intensity and action spectrum study proves that the generation of energetic charge carriers results in the observed activities under visible light, based on interband transitions of TiN or the ligand-to-metal charge transfer (LMCT) effect of the surface complex formed on TiO2. Thermal energy can be coupled with light energy within this photocatalytic system, which will facilitate the full use of solar energy. Different sequential reaction mechanisms on TiN and TiO2 are proposed to be responsible for the tunable product selectivity. The wide reaction scope, the fine conversion at a low light intensity, and the favorable reusability of photocatalysts prove the great application potential of this visible-light-driven procedure for the alpha-alkylation of ketones with primary alcohols.
机译：酮与醇的直接α-烷基化合成重要的α-烷基化酮和氧酮是C-C键形成的吸引方法。使用非贵金属的异质催化始终需要高反应温度，并且在一个催化系统中切换产品选择性仍然是一个巨大的挑战。在本研究中，提出了在温和条件下使用氧化锡光催化剂的该反应的可见光驱动的方法，从而可以良好地调整产品选择性。通过低成本锡纳米粉粉末的柔性和柔性的热氧化处理成功地合成了可调谐表面N / O比率的氧化锡光催化剂。苯乙酮与苄醇形成两个重要化合物的α-烷基化均匀地发生氯酮和二羟基酮酮，即使在室温下也发生了几乎完全转化，在100摄氏度下在可见光下实现。通过切换合成的光催化剂的表面N / O比可以良好地调整两种产品的比例。可以证明可见光以影响光催化剂的表面N / O比，并有助于调整产品选择性。光强度和动作谱研究证明了能量电荷载体的产生导致可见光下的观察到的活动，基于在TiO 2上形成的表面复合物的锡或配体 - 金属电荷转移（LMCT）效应的可见光转变。热能可以在该光催化系统内与光能相连，这将有助于充分利用太阳能。提出了锡和TiO 2上的不同顺序反应机制，负责可调产品选择性。宽反应范围，低光强度的细转化，光催化剂的有利可重用性证明了这种可见光驱动过程的巨大应用潜力，用于丙酮与伯醇的α-烷基化。

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