Suzuki-Miyaura coupling reactions using novel metal oxide supported ionic palladium catalysts

IF 5.062

Journal of Molecular Catalysis A: Chemical Pub Date : 2017-01-01 DOI:10.1016/j.molcata.2016.10.033

G.J. Lichtenegger , M. Maier , M. Hackl , J.G. Khinast , W. Gössler , T. Griesser , V.S.Phani Kumar , H. Gruber-Woelfler , P.A. Deshpande

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引用次数: 17

Abstract

Palladium substituted CeO₂, SnO₂ and their mixed oxides have been synthesized in quantitative yields out of non-toxic and inexpensive precursors using a simple and rapid single step solution combustion method. The resulting oxides, especially the mixed oxides Ce_0.79Sn_0.20Pd_0.01O_2-δ, Sn_0.79Ce_0.20Pd_0.01O_2-δ and Sn_0.99Pd_0.01O_2-δ proved to be highly active (TOF > 12,000 h⁻¹) for Suzuki-Miyaura cross-couplings of phenylboronic acid with various bromoarenes. The reactions were carried out in ambient air at moderate temperatures using environmentally friendly aqueous ethanol solutions as reaction solvents. Minimal amounts of palladium in the product solution ( < 0.14 mg/L), the reaction kinetics as well as catalyst poisoning tests support the thesis that the reaction proceeds via dissolved palladium species in a homogeneous reaction mechanism. Nevertheless, the synthesized catalysts could be reused for at least five times with only minor changes in activity and no changes in the crystal structure, indicating the high potential of the investigated catalysts as quasi-heterogeneous CC coupling catalysts.

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新型金属氧化物负载离子钯催化剂的Suzuki-Miyaura偶联反应

采用简单、快速的单步溶液燃烧法，以无毒、廉价的前驱物为原料，定量合成了钯取代CeO2、SnO2及其混合氧化物。所得到的氧化物，特别是混合氧化物ce0.79 sn0.20 pd0.010 o2 -δ， sn0.79 ce0.20 pd0.010 o2 -δ和sn0.99 pd0.010 o2 -δ被证明是高活性的(TOF >苯硼酸与各种溴芳烃的Suzuki-Miyaura交叉偶联反应为12,000 h−1)。反应以环境友好型乙醇水溶液为溶剂，在室温下进行。产品溶液中钯的最小量(<0.14 mg/L)，反应动力学和催化剂中毒试验支持了反应通过溶解的钯在均相反应机制下进行的论点。然而，合成的催化剂可以重复使用至少5次，而活性变化很小，晶体结构没有变化，表明所研究的催化剂作为准非均相CC偶联催化剂具有很高的潜力。

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来源期刊

Journal of Molecular Catalysis A: Chemical 化学-物理化学

自引率

0.00%

发文量

审稿时长

2.8 months

期刊介绍： The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.