Photodeposition of Pd nanoparticles on ZnIn2S4 for efficient alkylation of amines and ketones’ α-H with alcohols under visible light
Photodeposition of Pd nanoparticles on ZnIn2S4 for efficient alkylation of amines and ketones’ α-H with alcohols under visible light
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DOI：
10.1016/j.apcatb.2018.06.067
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发表时间：
2018-12
期刊：
影响因子：
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通讯作者：
Bingqing Wang;Zirong Deng;Xianzhi Fu;Chaodi Xu;Z. Li
中科院分区：
文献类型：
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作者：
Bingqing Wang;Zirong Deng;Xianzhi Fu;Chaodi Xu;Z. Li
通过在znin2s4表面光还原Pd(CH3CN) 2cl2，在可见光下沉积了尺寸约为6 nm的Pd纳米颗粒。对合成的pd - znin2s4纳米复合材料进行了全面表征，并考察了其光诱导胺的n -烷基化和酮与醇的α-H烷基化的催化性能。通过将醇在znin2s4上的光催化脱氢与pd基加氢成功偶联，发现pd - znin2s4纳米复合材料对烷基化反应具有优异的催化活性。在串联烷基化反应中，通过同步不同反应步骤的速率，获得了在0.5 wt%以上的pd - znin2s4纳米复合材料的最佳性能。由于小尺寸的钯纳米粒子提供了更多活性的不饱和钯原子，通过光还原得到的Pd- znin2s4纳米复合材料比通过NaBH4化学还原得到的Pd/ znin2s4表现出更优越的性能。本研究为在可见光下实现酮类的胺和α-H与醇的高效稳定烷基化提供了一条有效途径。该研究还强调了构建光诱导有机合成多功能催化剂的巨大潜力。
Pd nanoparticles with a small size of ca. 6 nm were deposited on the surface of ZnIn2S4via photoreduction of Pd(CH3CN)2Cl2over ZnIn2S4under visible light. The resultant Pd-ZnIn2S4nanocomposites were fully characterized and their catalytic performance for light induced N-alkylation of amines and α-H alkylation of ketones with alcohols were investigated. It was found that Pd-ZnIn2S4nanocomposites show superior catalytic activity for the alkylation reactions via a successful coupling of the photocatalytic dehydrogenation of alcohols over ZnIn2S4with Pd-based hydrogenation. An optimum performance was realized over 0.5 wt% Pd-ZnIn2S4nanocomposites by synchronization of the rates of different reaction steps in the tandem alkylation reaction. Ascribed to the small sized Pd nanoparticles, which provide more active unsaturated Pd atoms, Pd-ZnIn2S4nanocomposites obtained via photoreduction show superior performance as compared to Pd/ZnIn2S4obtained via a chemical reduction using NaBH4. This study provides an efficient way to realize a highly efficient and stable alkylation of amines and α-H of ketones with alcohols under visible light. This study also highlights the great potential of construction of multifunctional catalysts for light induced organic syntheses.