O-arylation reaction over lanthanide metal–organic framework: Synthesis, structure and catalytic reaction

IF 2.4 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Polyhedron Pub Date : 2024-08-14 DOI:10.1016/j.poly.2024.117177

Pameli Ghosh, Rakesh Debnath, Subratanath Koner

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Abstract

Two novel lanthanide based two-dimensional metal-organic framework (MOF) compounds [Tb(NDC)(NO₃)(DMA)₂]_n (MOF-1) and [Ho(NDC)(NO₃)(DMA)₂]_n (MOF-2) [H₂NDC=2,6-naphthalenedicarboxylic acid and DMA=N,N-dimethylacetamide] have been synthesized following solvothermal route and structurally characterized. Structural analysis reveals that both the compounds are crystallized in the orthorhombic crystal system with space group Pbca. MOFs feature a “paddle-wheel” (PW) type core building units which are constructed via carboxylato oxygen coordination with lanthanide atoms. 2D lanthanide based MOFs consist of paddle-wheel building block are rare in the literature. MOF-1 and MOF-2 possess an octa-coordinated metal center. Apart from carboxylato groups, oxygen atoms of DMA and NO₃⁻ ions are also coordinated to metal centers. Paddle-wheel cores are interconnected to each other to give rise to layered network structure in both the cases. 2D layers are propagated parallel to bc plane and layers are stacked one upon another along the crystallographic a axis. Notably, both MOF-1 and MOF-2 are capable to catalyze O-arylation reaction efficiently under heterogeneous medium. However, amongst them, catalytic efficacy of MOF-1 towards O-arylation reaction is found to be better than that of MOF-2.

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镧系金属有机框架上的 O-芳基化反应：合成、结构和催化反应

采用溶热法合成了两种新型镧系元素二维金属有机框架（MOF）化合物[Tb(NDC)(NO3)(DMA)2]n（MOF-1）和[Ho(NDC)(NO3)(DMA)2]n（MOF-2）[H2NDC=2,6-萘二甲酸和 DMA=N,N-二甲基乙酰胺]，并对其进行了结构表征。结构分析表明，这两种化合物都在正方晶系中结晶，空间群为 Pbca。MOFs 具有 "桨轮"（PW）型核心结构单元，它是通过羧基氧与镧系原子配位而构建的。由桨轮结构单元组成的二维镧系元素基 MOF 在文献中并不多见。MOF-1 和 MOF-2 具有八配位金属中心。除羧基外，DMA 和 NO3- 离子的氧原子也与金属中心配位。在这两种情况下，桨轮核相互连接，形成了层状网络结构。二维层平行于 bc 平面传播，沿晶体学 a 轴层层叠加。值得注意的是，MOF-1 和 MOF-2 都能在异质介质中高效催化 O-芳基化反应。不过，在这两种催化剂中，MOF-1 对 O-芳基化反应的催化效率要优于 MOF-2。

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来源期刊

Polyhedron 化学-晶体学

CiteScore

4.90

自引率

7.70%

发文量

515

审稿时长

2 months

期刊介绍： Polyhedron publishes original, fundamental, experimental and theoretical work of the highest quality in all the major areas of inorganic chemistry. This includes synthetic chemistry, coordination chemistry, organometallic chemistry, bioinorganic chemistry, and solid-state and materials chemistry. Papers should be significant pieces of work, and all new compounds must be appropriately characterized. The inclusion of single-crystal X-ray structural data is strongly encouraged, but papers reporting only the X-ray structure determination of a single compound will usually not be considered. Papers on solid-state or materials chemistry will be expected to have a significant molecular chemistry component (such as the synthesis and characterization of the molecular precursors and/or a systematic study of the use of different precursors or reaction conditions) or demonstrate a cutting-edge application (for example inorganic materials for energy applications). Papers dealing only with stability constants are not considered.