Spontaneous carbon dioxide fixation: a µ4-carbonate bridged tetranuclear zinc(II) complex of a heptadentate Schiff base

Journal of The Chemical Society-dalton Transactions Pub Date : 2002-12-09 DOI:10.1039/B209328F

M. Fondo, A. M. García-Deibe, M. R. Bermejo, J. Sanmartín, A. Llamas-Saiz

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引用次数: 40

Abstract

The electrochemical reaction of zinc and 2-(2-hydroxyphenyl)-1,3-bis[4-(2-hydroxyphenyl)-3-azabut-3-enyl]-1,3-imidazolidine (H3L1) in acetonitrile in air yields the tetranuclear zinc complex [(Zn2L)2(CO3)]·4H2O, which crystallises with different solvent molecules in two different systems: [(Zn2L)2(CO3)]·4H2O·2CH3CN 1a (monoclinic, Pn) and [(Zn2L)2(CO3)]·4H2O 1b (triclinic, P). The electrochemical reaction under a nitrogen stream leads to the isolation of crystals of [(Zn2L)2(CO3)]·0·25H2O·2CH3CN 1c (monoclinic P21/c). All structures demonstrate the striking ability of this system to spontaneously fix carbon dioxide. The crystals solution reveal a µ4-η2:η1:η1 binding mode for the carbonate group in all cases, leading to a tetranuclear complex by self-assembly of dinuclear units. Chemical reaction of Zn(CH3COO)2·2H2O with H3L yields [Zn2L(CH3COO)]·2H2O. Its recrystallisation allows isolating [Zn2L(CH3COO)]·2H2O·CH3OH 2. Reaction of [Zn2L(CH3COO)]·2H2O with (CH3)4NOH·5H2O leads, again, to the tetranuclear carbonate compound.

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自发二氧化碳固定:一个七齿希夫碱的4-碳酸盐桥接四核锌(II)配合物

在空气中，锌与2-(2-羟基苯基)-1,3-双[4-(2-羟基苯基)-3-氮杂基-3-烯基]-1,3-咪唑烷(H3L1)在乙腈中电化学反应生成四核锌配合物[(Zn2L)2(CO3)]·4H2O，该配合物在两种不同体系中以不同溶剂分子结晶:[(Zn2L)2(CO3)]·4H2O·2CH3CN 1a(单斜，Pn)和[(Zn2L)2(CO3)]·4H2O 1b(三斜，P).在氮气流下电化学反应可分离出[(Zn2L)2(CO3)]·0·25H2O·2CH3CN 1c(单斜P21/c)晶体。所有的结构都显示了这个系统自发固定二氧化碳的惊人能力。在所有情况下，晶体溶液中碳酸盐基团的结合模式均为μ 4-η2:η1:η1，通过双核单元的自组装形成四核配合物。Zn(CH3COO)2·2H2O与H3L的化学反应生成[Zn2L(CH3COO)]·2H2O。它的再结晶可以分离[Zn2L(CH3COO)]·2H2O·CH3OH 2。[Zn2L(CH3COO)]·2H2O与(CH3)4NOH·5H2O反应，再次生成四核碳酸盐化合物。

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Journal of The Chemical Society-dalton Transactions

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