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Synthesis and Structure of Binary Copper/Silver-Arsenic Clusters Derived from zintl Ion As_(7)^(3-)

Chinese Journal of Chemistry 2022年第1期40卷 65-70页

作者： Wei-Qiang Zhang Nikolay V.Tkachenko Lei Qiao Alexander I.Boldyrev Zhong-Ming Sun State Key Laboratory of Elemento-Organic Chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of Chemistry and Biochemistry Utah State University 0300 Old Main HillLoganUT 84322-0300USA

Polyarsenides containing coinage metals,[As_(7)Cu(PPh_(3))]^(2-)(1)and[M_(2)As_(14)]^(4-)(M=Cu,2;Ag,3),were synthesized by reactions of the nominal composition K_(3)As_(7) with Group 11 metal *** possible intermediate,cluster 1,was isolated from the solution phase through subtle changes in reaction conditions in the formation process of complex ***,we establish the pathway of the bimetallic bridged clusters[Cu_(2)As_(14)]^(4-)by the oxidation of the[As_(7)Cu(PPh_(3))]^(2-).Quantum chemical calculations reveal the presence of metallophilic interaction in clusters 2 and 3.

关键词： Polyarsenide cluster Reaction mechanism zintl ions Covalently bound Metallophilic interaction

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Synthesis of a Nine-atom Germanium Cluster K_(0.5)[K(18-crown-6)]_(1.5)Ge_9·1.5en with Unprecedented “up” and “down” Chain Arrangement of Unit [-(Ge_9-K-Ge_9)^(3-)-]

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Chinese Journal of Structural Chemistry 2014年第7期33卷 995-1000页

作者：王义秦茜桑瑞利徐立 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences Graduate School of the Chinese Academy of Sciences

A new complex K0.5[K（18-crown-6）]1.5Geg.1.5en （1） which contains unpreceden- ted ＂up＂ and ＂down＂ chain arrangement of unit [-（Ge9-K-Ge9）3-] has been prepared by the reaction of K4Ge9 with HgS in ethylenediamine （en） in the presence of 18-crown-6（1,4,7,10,13,16- hexaoxacyclooctadecane）, and characterized by X-ray structure analysis. The color of the title crystals （black）, which is darker than that of the reported three compounds with chains of germanium clusters, may result from the naked K＋ and their interactions with the chain. And the structure differences between 1 and the reported three compounds with chains of germanium have also been discussed.

关键词： zintl ions germanium clusters infinite chains comparison

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Synthesis and Crystal Structure of [K(18-Crown-6)]_3P_(11)·2en

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Chinese Journal of Structural Chemistry 2007年第1期26卷 45-48页

作者：戴枫荣徐立 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterThe Chinese Academy of Sciences

The undecaphosphide anion in ethylenediamine/18-crown-6 solution is isolated as [K（18-crown-6）]3P11·2en 1. The crystal structure has been determined by single-crystal X-ray diffraction. The crystal is of monoclinic, space group P21 with α = 13.4731（7）, b = 16.1123（6）, c = 16.5117（9） A, β = 112.133（2）°, Y = 3320.3（3） A3, Dc = 1.371 g/cm^3, C40H88K3N4O18P11, Mr = 1371.11, F（000） = 1444,μ = 0.532 mm^-1, Z= 2, R = 0.0544 and wR = 0.1326 for 11423 observed reflections （I 〉 20（I））. The ＂naked＂ P11^3- ion is stabilized by two partly sequestered potassiums, The third partly sequestered potassium does not interact with the P atom （P（6）） but with two solvent molecules.

关键词： zintl ions phosphorus crystal structure undeeaphosphide

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Synthesis and Crystal Structure of [K(2,2,2-crypt)]_3Sb_(11)

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Chinese Journal of Structural Chemistry 2011年第8期30卷 1091-1094页

作者：翟君徐立 Graduate School of the Chinese Academy of Sciences State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

The title complex [K（2,2,2-crypt）]3Sb11 has been prepared by the reaction of K3Cd2Sb with Cu-C≡CH in ethylenediamine in the presence of 2,2,2-crypt, and characterized by low temperature X-ray structure analysis. The crystal is of orthorhombic system, space group C2221 with a = 15.475（3）, b = 22.807（5）, c = 24.834（6）, V = 8765（3）3, Dc = 1.960 g/cm3, C54H108K3N6O18Sb11, Mr = 2586.01, F（000） = 4944, μ = 3.531 mm-1, Z = 4, R = 0.0442 and wR = 0.1053 for 10265 observed reflections （I 2σ（I））. The ＂naked＂ Sb113- anion is stable due to the completely sequestered alkali metal cations through ion-ion interactions.

关键词： zintl ions antimony crystal structure

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Symmetry Reduction upon Size Mismatch:The Non-lcosahedral Intermetalloid Cluster [Co@Ge12]^3-

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Chinese Journal of Chemistry 2018年第12期36卷 1165-1168页

作者： Chao Liu Lei-Jiao Li Ivan A.Popov Robert J.Wilson Cong-qiao Xu Jun Li Alexander I.Boldyrev Zhong-Ming Sun State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences5625 Renmin StreetChangchunJilin 130022China University of Chinese Academy of Sciences Beijing 100049China School of Materials Science and Engineering Research Center of Rare Earth and Inorganic Functional MaterialsNankai UniversityTianjin 300350China School of Chemistry & Environmental Engineering Chang chun University of Science & TechnologyChangchunJilin 130022China Department of Chemistry and Biochemistry Utah State University0300 Old Main HillLosanUtah84322-0300USA Fachbereich Chemie und Wissenschaftliches Zentrum fur Materialwissenschaften (WZMW) Philipps-Universtat MarburgHans-Meerwein-Straβe35043 MarburgGermany Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education Tsinghua UniversityBeijing 200084China

A new complex comprising [Co@Ge12]3- cluster core was synthesized through the reaction of CoMe(PMe3)4 and K4Ge9 in ethylenediamine solution. The pseudo‐D5d geometry of this cluster can be viewed as structurally derived from an icosahedral cage via Jahn‐Teller effect, leading to notable bonding differences from Ih‐[M@E12]q− clusters (E = Sn, Pb with q = 2, 3). The [Co@Ge12]3- cluster represents a structural conundrum. On the basis of the geometric considerations it could be viewed as a sandwich complex. However, chemical bonding analysis revealed that there is a direct covalent multicenter bonding between the two pentagons, thus indicating that the structure should be viewed as an elongated icosahedron. Further theoretical calculations on [M@Ge12]3− (M = Rh, Ir, Mt) indicate that similar compounds of larger‐size metal atoms can drive the complete transformation of [M@Ge12]3− clusters from icosahedron structure to a sandwich one.

关键词： zintl ions intermetalloid cluster icosahedron Sandwich complex

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