Terphenyl-Tricarboxylate Coordination Polymers: From Hydrothermal Assembly to Structural Diversity and Catalytic Application

IF 4.3 3区材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC

ACS Applied Electronic Materials Pub Date : 2024-10-09 DOI:10.1021/acs.cgd.4c0122110.1021/acs.cgd.4c01221

Hongrui Zhang, Jinzhong Gu*, Marina V. Kirillova and Alexander M. Kirillov*,

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Abstract

An aromatic tricarboxylic acid building block, [1,1′:3′,1″-terphenyl]-4,4″,5′-tricarboxylic acid (H₃tptca), was used as a versatile linker for assembling, under hydrothermal conditions, a series of 12 new coordination polymers (CPs) in the presence of supporting N-donor ligands acting as mediators of crystallization. The obtained products were formulated as [Mn(μ-Htptca)(phen)₂]_n·nH₂O (1), [Zn(μ-Htptca)(2,2′-bipy)(H₂O)]_n·nH₂O (2), [Ni(μ₃-Htptca)(μ-4,4′-bipy)]_n·2nH₂O (3), [Co(μ₃-Htptca)(μ-bpe)]_n (4), [M₃(μ₃-tptca)₂(phen)₃(H₂O)₂]_n·2nH₂O (M = Co (5), Zn (6)), [Co₂(μ₄-tptca)(μ-OH)(2,2′-bipy)₂]_n (7), [Zn₃(μ₃-tptca)₂(2,2′-bipy)₃(H₂O)₂]_n·4nH₂O (8), {[Cd(H₂biim)₃][Cd₂(μ₃-tptca)(μ₅-tptca)]}_n (9), [Co₂(μ₄-tptca)(μ-bpa)(μ₃-OH)(H₂O)₂]_n·nH₂O (10), [Ni₃(μ₃-tptca)₂(μ-bpa)₃(H₂O)₄]_n·5nH₂O (11), and [Co₂(μ₄-tptca)(μ-bpb)(μ-OH)]_n (12), wherein phen, 2,2′-bipy, 4,4′-bipy, bpe, H₂biim, bpa, and bpb are 1,10-phenanthroline, 2,2′- and 4,4′-bipyridine, 1,2-di(4-pyridyl)ethane, 2,2′-biimidazole, bis(4-pyridyl)amine, and 1,4-bis(pyrid-4-yl)benzene, respectively. Crystal structures of CPs 1–12 reveal a broad diversity metal–organic networks that range from 1D chains (1, 2, 5, 6, and 8) to 2D layers (3, 4, 7, 9, and 11) and 3D nets (10 and 12), including the examples of interpenetrated, polycatenated, and topologically unique architectures. Structural features and catalytic properties of the obtained CPs were studied and discussed. In particular, a Zn(II) CP 8 acts as an efficient and recyclable heterogeneous catalyst for the mild cyanosilylation of benzaldehydes, leading to the formation of the corresponding cyanohydrin products in up to 99% yields. The obtained compounds widen a growing family of functional CPs driven by terphenyl-tricarboxylate linkers.

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三羧酸三联苯配位聚合物：从水热组装到结构多样性和催化应用

一种芳香族三羧酸结构单元--[1,1′:3′,1″-三联苯]-4,4″,5′-三羧酸（H3tptca），被用作一种多功能连接体，在水热条件下，在作为结晶介质的 N-供体配体的支持下，组装成一系列 12 种新型配位聚合物（CPs）。所得到的产物分别为[Mn(μ-Htptca)(phen)2]n-nH2O (1)、[Zn(μ-Htptca)(2,2′-bipy)(H2O)]n-nH2O (2)、[Ni(μ3-Htptca)(μ-4,4′-bipy)]n-2nH2O (3)、[Co(μ3-Htptca)(μ-bpe)]n (4)、[M3(μ3-ptca)2(phen)3(H2O)2]n-2nH2O（M = Co (5)、Zn (6)）、[Co2(μ4-ptca)(μ-OH)(2,2′-bipy)2]n (7)、[Zn3(μ3-ptca)2(2,2′-bipy)3(H2O)2]n-4nH2O (8)、{[Cd(H2biim)3][Cd2(μ3-ptca)(μ5-ptca)]}n (9)、[Co2(μ4-tptca)(μ-bpa)(μ3-OH)(H2O)2]n-nH2O（10）、[Ni3(μ3-tptca)2(μ-bpa)3(H2O)4]n-5nH2O（11）和[Co2(μ4-tptca)(μ-bpb)(μ-OH)]n（12），其中phen、2,2′-联吡、4,4′-联吡、bpe、H2biim、bpa 和 bpb 分别指 1,10-菲罗啉、2,2′- 和 4,4′-联吡啶、1,2-二（4-吡啶基）乙烷、2,2′-双咪唑、双（4-吡啶基）胺和 1,4-双（吡啶-4-基）苯。氯化石蜡 1-12 的晶体结构揭示了金属有机网络的广泛多样性，从一维链（1、2、5、6 和 8）到二维层（3、4、7、9 和 11）和三维网（10 和 12），包括互穿、多链和拓扑结构独特的例子。对所获得的氯化石蜡的结构特征和催化特性进行了研究和讨论。其中，Zn(II) CP 8 是一种高效、可回收的异相催化剂，可用于苯甲醛的温和氰基硅烷化反应，生成相应的氰醇产物，收率高达 99%。所获得的化合物拓宽了由三联苯三羧酸连接体驱动的功能性氯化石蜡家族。

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来源期刊

ACS Applied Electronic Materials Multiple-

CiteScore

7.20

自引率

4.30%

发文量

567