高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (11): 2115.doi: 10.7503/cjcu20150601
收稿日期:
2015-07-31
出版日期:
2015-11-10
发布日期:
2015-10-13
作者简介:
联系人简介: 麥松威, 男, 博士, 教授, 博士生导师, 中国科学院院士, 主要从事结构化学、 无机合成、 超分子自组装及晶体工程研究. E-mail:基金资助:
Sam S. K. HAU1,2, Ting HU1,3, Dennis Y. S. TAM1, Thomas C. W. MAK1,*()
Received:
2015-07-31
Online:
2015-11-10
Published:
2015-10-13
Contact:
Thomas C. W. MAK
E-mail:tcwmak@cuhk.edu.hk
摘要:
总结了我们在新型炔银簇化合物研究方面的最新进展. 这些化合物分为以下几种类型: (a)1,3,5-己三炔基和1,3,5,7-辛四炔基; (b)1,5-己二炔基; (c)经膦酸配体组装的乙炔基和烷基乙炔基; (d)苯乙炔基、 环烷基乙炔基和含氮杂环基乙炔基结构单元的银簇化合物; (e)经不同类型的银-碳配位键连接, 并进一步通过分子内/分子间作用力稳固其配位网络的炔银化合物. 我们还进一步讨论了溶剂、 配体的位阻大小和辅助配体类型对于多维配位网络结构的影响.
中图分类号:
TrendMD:
侯俊傑, 胡婷, 譚耀新, 麥松威. 含全碳和多炔阴离子配体的银簇化合物的超分子组装及其结构研究. 高等学校化学学报, 2015, 36(11): 2115.
Sam S. K. HAU, Ting HU, Dennis Y. S. TAM, Thomas C. W. MAK. Assembly of Organosilver(I) Networks with Multinuclear Supramolecular Synthons Containing All-carbon and Carbon-rich Anionic Ligands. Chem. J. Chinese Universities, 2015, 36(11): 2115.
Fig.1 Coordination chain structure of Ag2C2·4AgCF3CO2·(bipyH)(CF3CO2)·H2O(A), discrete molecular structure of Ag2C2·7AgCF3CO2·(H3O)(CF3CO2)·2(bipyH2)(CF3CO2)2·3H2O(B), coordination chain structure of 2Ag2C2·8AgCF3CO2·6L1(L1=pyrazole)(C) and coordination chain structure of Ag2C2·10AgCF3CO2·2L2[L2=4,5-dihydro-3-(4-pyridinyl)-2H-benz(g)-indazole](D)
Fig.2 Ribbon-like coordination chain along b-axis formed by linkage of (C2)2@Ag15 units by bridging L3 ligands in [(Ag2C2)2(AgCF3COO)11(L3)(μ2-DMSO)3(DMSO)5]·1/4H2O
Fig.3 Discrete molecular structures of [(Ag2C4)(AgCF3CO2)6(L)6](L=2-cyanopyridine)(representative of 0D structure)(A), coordination chain structure of [(Ag2C4)2(AgCF3CO2)9(L)7(H2O)]n(L=3-chloropyridine)(representative of 1D structure)(B), coordination layer structure of [{(Ag2C4)0.5(AgNO3)3(L)}·H2O]n (L=3-chloropyridine)(representative of 2D structure)(C) and three-dimensional coordination network of [{(Ag2C4)(AgCF3CO2)5(L)1.5(H2O)2}·H2O]n(L=2-methylpyrazine)(representative of 3D structure)(D)
Fig.4 Coordination layer structure of Ag2C6·8AgCF3CO2·6H2O along c-axis(A) and ladder-like silver(I) double chain structure of 2.5(Ag2C8)·10AgCF3CO2·10DMSO(B)
Fig.5 Two typical coordination modes of C6H42- dianion (A) Agm?C6H4?Agn, anti “stretched-Z” conformation; (B) C6H4?Agn, gauche “arch-like” conformation.
Fig.6 3D coordination network of Ag2C6H4·2AgNO3·2AgL1 constructed by linking silver layers by pillar-like nitrate groups(A) and Ag2C6H4·4AgNO3·2L5 with coordination layers linked by weak N—H…O hydrogen bonds involving imidazole ligands and nitrate groups to form a 3D supramole-cular framework(B) and 3D supramolecular framework of Ag2C6H4·4AgNO3·2L6 with each coordination layer constructed by cross-linkage of silver chains by nitrate ligands
Fig.7 Infinite-chain structure of Ag2C6H4·5AgCF3CO2·3L5(A), two-dimensional coordination layer in 3Ag2C6H4·10AgCF3CO2·4L1(B) and three-dimensional coordination network of Ag2C6H4·3AgCF3CO2·2AgL7·H2O(C)
Fig.8 Top-down view of centrosymmetric Ag16 cluster in {(NO3)2@Ag16(PhC≡≡C)4[(tBuPO3)4V4O8]2·(DMF)6(NO3)2}(A) and top-down view of the core structure of pseudo-C3 Ag43 cluster in {[(O2)V2O6]3@Ag43(PhC≡≡C)19[(tBuPO3)4V4O8]3(DMF)6} For enhanced visibility, the three independent encapsulated [(O2)V2O6]4- species are represented by gray, turquoise, and blue semi-transparent polyhedra with V atoms included.
Fig.9 Core skeleton of one of the two nearly identical Ag28 clusters in [{Ag5(NO3@Ag18)Ag5}(tBuC≡≡C)16·(tBuPO3)4(H2O)4]·3SiF6·4.5H2O·3.5MeOH(A) and Cl@Ag22 cluster skeleton in[{Ag8(Cl@Ag14)}(tBuC≡≡C)14(tBuPO3)2F2·(H2O)2]BF4·3.5H2O, lying on a crystallographic C2 axis(B)
Fig.11 Layer structure of compound 1 viewed along the a-axis, in which the C2@Ag9 cages are linked by phosphonate groups(A) and three-dimensional architecture of compound 7 generated from the cross-linkage of silver chains by coordination bonding with aqua ligands(B)
Fig.12 Perspective views of argentophilic layer structure in [AgC≡≡CPh·AgNO3](A), silver(I) chain in [2AgC≡≡CPh·5CF3CO2Ag·4DMSO](B) and thick silver coordination column in [10AgC≡≡CPh·2AgOTf·AgNO3·3DMSO](C)
Fig.13 Perspective views of argentophilic silver(I) layer structure in 12[Ag(4-MeC6H4C≡≡C)]·7AgNO3(A) and the silver layer structure in 2[Ag(4-PhC6H4C≡≡C)]·AgNO3(B)
Fig.14 Argentophilic silver(I) structures in complexes generated with halophenylethynide ligands (A, D, G) Cl; (B, E, H) Br; (C, F, I) I; (A, B, C) para position; (D, E, F) meta position; (G, H, I) ortho position.
Fig.15 Different coordination modes of anionic tridentate L8 ligands in Ag11 and Ag12 aggregates(A) and coordination mode of L9 in [(AgL9)·(AgCF3CO2)5·(H2O)3][L9=1-chloro-2-(prop-2-ynyloxy)benzene]
Fig.16 Perspective views of a portion of an infinite silver-organic chain in the crystal packing of AgL11·3AgCF3CO2·3H2O(L11=2-ethynylquinoline)(A) and Ag8 aggregate in [(AgL12)·(AgCF3CO2)3](L12=2-ethynyl-4,6-dimethylpyrimidine)(B)
Fig.17 Coordination modes of independent L13 ligands in double salt(Ag2L13)·9AgCF3CO2·3H2O·3CH3CN(A) and perspective view of the linkage between metallocycles in the infinite-chain structure of (Ag2L13)2·9AgCF3CO2·11H2O(B)
Fig.18 Perspective view of the silver(I) atoms and ethynide groups in (Ag2L15)·8AgCF3CO2·6DMSO(A) and coordination environment of the silver(I) atoms and ethynide groups in (Ag2L19)·5AgCF3CO2·2H2O(B)
Fig.19 Coordination environment of the silver(I) atoms and ethynide groups in complex 11(A) and perspective view of the coordination silver-organic chain with L24 and Ag(I) aggregates in complex 12(B)
Fig.20 Perspective view of coordination geometry in double salt 2(Ag2L25)·7AgCF3CO2·3CH3CN(A) and perspective view of crystal packing in 3(Ag2L30)·14AgCF3CO2·[Ag2(CH3CN)3]·(CF3CO2)2·4H2O·6CH3CN(B)
Scheme 6 A series of ten ligands containing an aromatic core with a rigid/flexible terminal ethynyl group, an internal ethynyl group, and a vinyl substituent at various positions on an aromatic ring
Fig.22 Coordination modes of the anionic ligands in their corresponding silver complexes, in which part (J) illustrates the presence of all the four kinds of silver-carbon binding interactions in AgL44·6AgCF3CO2·H2O·MeOH
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