一种依靠可极化的亚硝基镍枢纽的硫催化镍-镍配位聚合物

IF 3.5 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Dalton Transactions Pub Date : 2024-12-17 DOI:10.1039/d4dt03174a

Manish Jana, Michael B. Hall, Marcetta Y. Darensbourg

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引用次数: 0

摘要

重氮镍顺式二硫酸盐对三苯基膦金(I)的模板化特性产生了一种横向[Ni(N2S2)-2Au(PPh3)]复合物（T. A. Pinder, S. K. Montalvo, A. M. Lunsford, C.-H. Hsieh, J. H. Reibenspies and M. Y. Darensbour, Dalton Trans, 2014, 43, 138-144）。Heieh、J. H. Reibenspies 和 M. Y. Darensbourg，Dalton Trans.，2014, 43, 138-144）提出，d10-Au(I)的合适类似物，即{Ni(NO)}10，可以为[Ni(N2S2)-2Ni(NO)(X)]n 配位聚合物生成一个四面体镍节点。由 Feltham 的 [(Ph3P)2Ni(NO)(Cl)]（R. D. Feltham，Inorg.Chem.，1964，3，116-119）衍生的单体前驱体产生了失去 PPh3 的双齿/硫螯合 [Ni(N2S2)-Ni(NO)(X)]。在{Ni(NO)}10 合子中，叠氮化物 N3- 交换了 Cl-，从而平衡了 Ni(NO)的亲电性和非共价（H 键和范德华）相互作用，稳定了方形平面 NiII 和四面体 Ni（后者在电子和自旋定位的{Ni(NO)}10 系统中）之间的桥接硫延伸链。这项研究开辟了一条利用金属二硫酸盐制造配位聚合物的新途径，在这种情况下，配位聚合物的成功取决于高度极化的{Ni(NO)}10单元。

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A sulfur-templated Ni–Ni′ coordination polymer that relies on a polarizable nickel nitrosyl hub

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A sulfur-templated Ni–Ni′ coordination polymer that relies on a polarizable nickel nitrosyl hub

The templating properties of a diaza-nickel-cis-dithiolate towards triphenylphosphine gold(I), yielding a transoid [Ni(N₂S₂)·2Au(PPh₃)] complex (T. A. Pinder, S. K. Montalvo, A. M. Lunsford, C.-H. Hsieh, J. H. Reibenspies and M. Y. Darensbourg, Dalton Trans., 2014, 43, 138–144) suggested that a suitable analogue of d¹⁰-Au(I), i.e., {Ni(NO)}¹⁰, could generate a tetrahedral nickel node for a [Ni(N₂S₂)·2Ni(NO)(X)]_n coordination polymer. Monomeric precursors, derived from Feltham's [(Ph₃P)₂Ni(NO)(Cl)] (R. D. Feltham, Inorg. Chem., 1964, 3, 116–119) produced the bidentate/sulfur-chelated [Ni(N₂S₂)·Ni(NO)(X)] species with loss of PPh₃. Exchange of Cl⁻ by azide, N₃⁻, in the {Ni(NO)}¹⁰ synthon led to the balance of electrophilicity at Ni(NO) and non-covalent (H-bonding and van der Waals) interactions that stabilized the extended chain of bridging sulfurs, in transoid connectivities, between a square planar Ni^II and a tetrahedral Ni, the latter within the electronic and spin-delocalized {Ni(NO)}¹⁰ system. This study defines a new path that creates coordination polymers using metallodithiolates, the success of which, in this case, depends on the highly polarizable {Ni(NO)}¹⁰ unit.

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.