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A Discrete Tetrahedral Indium Cage as an Efficient Heterogeneous Catalyst for the Fixation of CO2 and the Strecker Reaction of Ketones.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-01-22 , DOI: 10.1021/acs.inorgchem.9b02763
Guang-Ming Liang 1, 2 , Peng Xiong 1 , Khan Azam 1 , Qing-Ling Ni 1 , Jian-Qiang Zeng 1 , Liu-Cheng Gui 1 , Xiu-Jian Wang 1
Affiliation  

A discrete tetrahedral indium cage, {[In12(μ3-OH)4(HCO2)24(tcma)4]} (In12-GL), was synthesized solvothermally by the reaction of indium nitrate with the tripodal tricarboxylic acid ligand N,N,N-tris{(2'-carboxy[1,1'-biphenyl]-4-yl)methyl}methylammonium chloride ([H3tcma]+Cl). This cage consists of four trimeric units [In3(μ3-OH)(μ2-CO2)3(μ2-HCO2)3] and four [tcma]2- ligands, which all perform as 3-connection nodes to bridge each other, resulting in a tetrahedral cage structure. The trimeric unit [In3(μ3-OH)(μ2-CO2)3(μ2-HCO2)3] is observed for the first time in the family of In-based metal-organic structures and can be considered as an evolution of a 6-connected [In3(μ3-O)(μ2-CO2)6] unit. Each In3+ is terminally coordinated by a μ1-HCO2 group. This cage contains potential Lewis acidic/basic active sites endowed by In3+ ions as Lewis acidic sites and the uncoordinated oxygen atoms of μ1-HCO2 moieties as Lewis basic sites and was explored as an effective heterogeneous catalyst in the cycloaddition of CO2 with epoxides and the Strecker reaction for amino nitriles. These catalytic reactions were deduced to happen on the surface of the In12-GL cage.

中文翻译:

离散的四面体铟笼作为一种高效多相催化剂,用于固定CO2和酮的Strecker反应。

通过硝酸铟与三脚架三羧酸配体N,N的溶剂热反应合成了离散的四面体铟笼{[In12(μ3-OH)4(HCO2)24(tcma)4]}(In12-GL)。 N-三({2'-羧基[1,1'-联苯] -4-基)甲基}甲基氯化铵([H3tcma] + Cl)。该笼由四个三聚体单元[In3(μ3-OH)(μ2-CO2)3(μ2-HCO2)3]和四个[tcma] 2-配体组成,它们均作为3个连接节点相互桥接,从而呈四面体的笼状结构。三聚体单元[In3(μ3-OH)(μ2-CO2)3(μ2-HCO2)3]首次在In基金属有机结构家族中观察到,可以看作是6 -连接的[In3(μ3-O)(μ2-CO2)6]单元。每个In3 +均通过μ1-HCO2基团进行末端协调。该笼包含潜在的路易斯酸性/碱性活性位点,该活性位点是In3 +离子赋予的路易斯酸性位点,而μ1-HCO2部分的未配位的氧原子则是路易斯碱性位点,被认为是有效的多相催化剂,用于环氧化物和Strecker的CO2环加成反应。反应为氨基腈。推测这些催化反应发生在In12-GL笼子的表面。
更新日期:2020-01-23
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