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Coordination Polymers from an Amino-Functionalized Terphenyl-Tetracarboxylate Linker: Structural Multiplicity and Catalytic Properties
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-10-17 , DOI: 10.1021/acs.inorgchem.3c01905 Xiaoxiang Fan 1 , Hongyu Wang 1 , Jinzhong Gu 1 , Dongyu Lv 1 , Bo Zhang 1 , Jijun Xue 1 , Marina V Kirillova 2 , Alexander M Kirillov 2
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-10-17 , DOI: 10.1021/acs.inorgchem.3c01905 Xiaoxiang Fan 1 , Hongyu Wang 1 , Jinzhong Gu 1 , Dongyu Lv 1 , Bo Zhang 1 , Jijun Xue 1 , Marina V Kirillova 2 , Alexander M Kirillov 2
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An amino-functionalized terphenyl-tetracarboxylic acid, 2′-amino-[1,1′:4′,1″-terphenyl]-3,3″,5,5″-tetracarboxylic acid (H4tpta), was used as an adaptable linker to synthesize, under hydrothermal conditions, eight coordination polymers (CPs). The obtained products were formulated as [Co(μ6-H2tpta)]n (1), [Co(μ3-H2tpta)(2,2′-bipy)]n (2), [M3(μ6-Htpta)2(2,2′-bipy)2]n (M = Mn (3), Cd (4)), [Ni2(μ4-tpta)(phen)2(H2O)4]n (5), [Zn2(μ6-tpta)(phen)2]n (6), {[Zn2(μ6-tpta)(μ-4,4′-bipy)]·H2O}n (7), and [Zn2(μ6-tpta)(μ-H2biim)(H2O)2]n (8), wherein 2,2′-bipyridine (2,2′-bipy), 4,4′-bipyridine (4,4′-bipy), 1,10-phenanthroline (phen), or 2,2′-biimidazole (H2biim) are present as additional stabilizing ligands. The structural types of 1–8 vary from one-dimensional (1D) (2, 5) and two-dimensional (2D) (3, 4, 6) CPs to three-dimensional (3D) metal–organic frameworks (MOFs) (1, 7, and 8) with a diversity of topologies. The products 1–8 were investigated as catalysts in the Knoevenagel condensation involving aldehydes and active methylene derivatives (malononitrile, ethyl cyanoacetate, or tert-butyl cyanoacetate), leading to high condensation product yields (up to 99%) under optimized conditions. Various reaction conditions, substrate scope, and catalyst recycling were investigated. This work broadens the application of H4tpta as a versatile tetracarboxylate linker for the generation of diverse CPs/MOFs.
中文翻译：
氨基官能化三联苯四羧酸酯连接体的配位聚合物：结构多重性和催化性能
氨基官能化的三联苯四甲酸，2'-氨基-[1,1':4',1"-三联苯]-3,3",5,5"-四甲酸(H 4 tpta)，被用作一种适应性强的接头，可在水热条件下合成八种配位聚合物（CP）。得到的产物被配制为[Co(μ 6 -H 2 tpta)] n ( 1 ), [Co(μ 3 -H 2 tpta)(2,2'-bipy)] n ( 2 ), [M 3 ( μ 6 -Htpta) 2 (2,2′-bipy) 2 ] n (M = Mn ( 3 ), Cd ( 4 )), [Ni 2 (μ 4 -tpta)(phen) 2 (H 2 O) 4 ] n ( 5 ), [Zn 2 (μ 6 -tpta)(phen) 2 ] n ( 6 ), {[Zn 2 (μ 6 -tpta)(μ-4,4′-bipy)]·H 2 O } n ( 7 )和[Zn 2 (μ 6 -tpta)(μ-H 2 biim)(H 2 O) 2 ] n ( 8 )，其中2，2'-联吡啶(2，2'-联吡啶) 、4,4'-联吡啶 (4,4'-bipy)、1,10-菲咯啉 (phen) 或 2,2'-联咪唑 (H 2 biim) 作为额外的稳定配体存在。1 – 8的结构类型从一维 (1D) ( 2 , 5 ) 和二维 (2D) ( 3 , 4 , 6 ) CP 到三维 (3D) 金属有机框架 (MOF) ( 1、7和8 ）具有多种拓扑结构。研究了产物1 – 8作为涉及醛和活性亚甲基衍生物（丙二腈、氰基乙酸乙酯或氰基乙酸叔丁酯）的 Knoevenagel 缩合反应中的催化剂，在优化条件下产生了高缩合产物收率（高达 99%）。研究了各种反应条件、底物范围和催化剂回收。这项工作拓宽了 H 4 tpta 作为通用四羧酸酯连接体的应用，用于生成不同的 CP/MOF。
更新日期：2023-10-17
中文翻译：
氨基官能化三联苯四羧酸酯连接体的配位聚合物：结构多重性和催化性能
氨基官能化的三联苯四甲酸，2'-氨基-[1,1':4',1"-三联苯]-3,3",5,5"-四甲酸(H 4 tpta)，被用作一种适应性强的接头，可在水热条件下合成八种配位聚合物（CP）。得到的产物被配制为[Co(μ 6 -H 2 tpta)] n ( 1 ), [Co(μ 3 -H 2 tpta)(2,2'-bipy)] n ( 2 ), [M 3 ( μ 6 -Htpta) 2 (2,2′-bipy) 2 ] n (M = Mn ( 3 ), Cd ( 4 )), [Ni 2 (μ 4 -tpta)(phen) 2 (H 2 O) 4 ] n ( 5 ), [Zn 2 (μ 6 -tpta)(phen) 2 ] n ( 6 ), {[Zn 2 (μ 6 -tpta)(μ-4,4′-bipy)]·H 2 O } n ( 7 )和[Zn 2 (μ 6 -tpta)(μ-H 2 biim)(H 2 O) 2 ] n ( 8 )，其中2，2'-联吡啶(2，2'-联吡啶) 、4,4'-联吡啶 (4,4'-bipy)、1,10-菲咯啉 (phen) 或 2,2'-联咪唑 (H 2 biim) 作为额外的稳定配体存在。1 – 8的结构类型从一维 (1D) ( 2 , 5 ) 和二维 (2D) ( 3 , 4 , 6 ) CP 到三维 (3D) 金属有机框架 (MOF) ( 1、7和8 ）具有多种拓扑结构。研究了产物1 – 8作为涉及醛和活性亚甲基衍生物（丙二腈、氰基乙酸乙酯或氰基乙酸叔丁酯）的 Knoevenagel 缩合反应中的催化剂，在优化条件下产生了高缩合产物收率（高达 99%）。研究了各种反应条件、底物范围和催化剂回收。这项工作拓宽了 H 4 tpta 作为通用四羧酸酯连接体的应用，用于生成不同的 CP/MOF。
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