摘要
在水热条件下,成功合成了一例过渡金属钴修饰的有机-无机杂化Dawson型三维超分子多金属磷钨酸簇合物[Co(dap)_3]_2[H_2P_2W_(18)O_(62)]·11H_2O (1)(dap=1,2-丙二胺),采用X射线单晶衍射、元素分析、红外光谱及热重分析对化合物进行了结构分析和基本表征.化合物1属于正交晶系,Pnma空间群,单胞参数为a=2.688 92(7) nm,b=2.176 67(6) nm,c=1.480 93(5) nm,α=β=γ=90°.从超分子化学的角度来看,化合物1中的饱和Dawson型簇阴离子和金属-有机复合物之间通过广泛的氢键作用,进而形成有趣的4,8-连接的三维超分子网络结构.
A new 3 D cobalt-substituted Dawson-type organic-inorganic hybrid supramolecular polyoxometalate, [Co(dap)_3]_2[H_2P_2W_(18)O_(62)]·11 H_2O(1)(dap = 1,2-diaminopropane), has been prepared under hydrothermal conditions and characterized by elemental analysis, IR spectroscopy, XRD, thermogravimetric(TG) analysis and X-ray single-crystal diffraction. It belongs to Orthorhombic and Pnma space group, and the cell parameters are a = 2.688 92(7) nm, b = 2.176 67(6) nm, c = 1.480 93(5) nm, α = β = γ = 90°. From the viewpoint of supramolecular chemistry, the saturated Dawson-type polyoxoanions and cobalt(II)-dap complexes in 1 can be further extended to interesting 4,8-connected 3-D frameworks via extensive hydrogen-bonding interactions.
引文
[1] MACDONALD L, RAUSCH B, SYMES M D. Selective hydrogenation of nitroarenes using an electrogenerated polyoxometalate redox mediator [J]. Chemical Communications, 2018, 54(9): 1093-1096.
[2] HAN Q, DING Y. Recent advances in the field of light-driven water oxidation catalyzed by transition-metal substituted polyoxometalates [J]. Dalton Transactions, 2018, 47(25): 8180-8188.
[3] 湛世霞, 张康, 李春艳, 等. 基于多金属氧酸盐和贵金属的纳米复合材料的研究进展[J]. 化学研究, 2018, 29(2): 125-130. ZHAN S X, ZHANG K, LI C Y, et al. Research progress of nanocomposites based on polyoxometallates and noble metals [J]. Chemical Research, 2018, 29(2): 125-130.
[4] TANG Y J, ZHANG A M, ZHU H J, et al. Polyoxometalate precursors for precisely controlling synthesis of bimetallic sulfide heterostructure through nucleation-doping competition [J]. Nanoscale, 2018, 10(18): 8404-8412.
[5] MIRAS H N, VILA-NADAL L, CRONIN L. Polyoxometalate based open-frameworks (POM-OFs) [J]. Chemical Society Reviews, 2014, 43(16): 5679-5699.
[6] DU D Y, QIN J S, LI S L, et al. Recent advances in porous polyoxometalate-based metal-organic framework materials [J]. Chemical Society Reviews, 2014, 43(13): 4615-4632.
[7] ZHANG Z, ZHAO J W, YANG G Y. Tri-ZrIV substituted sandwiched polyoxometalate with mixed trilacunary Keggin-/Dawson-type polyoxotungstate units [J]. European Journal of Inorganic Chemistry, 2017, 2017(26): 3244-3247.
[8] MOUSSAWI M A, LECLERC-LARONZE N, FLOQUET S, et al. Polyoxometalate, cationic cluster, and γ-cyclodextrin: from primary interactions to supramolecular hybrid materials [J]. Journal of the American Chemical Society, 2017, 139(36): 12793-12803.
[9] WANG G N, CHEN T T, LI S B, et al. A coordination polymer based on dinuclear (pyrazinyl tetrazolate) copper(II) cations and Wells-Dawson anions for high-performance supercapacitor electrodes [J]. Dalton Transactions, 2017, 46(40): 13897-13902.
[10] HUANG Q, WEI T, ZHANG M, et al. A highly stable polyoxometalate-based metal-organic framework with π-π stacking for enhancing lithium ion battery performance [J]. Journal of Materials Chemistry A, 2017, 5(18): 8477-8483.
[11] ZHAO H Y, DONG D P, YU N S, et al. Three new organic-inorganic hybrid di-copper-complex substituted monovacant phosphotungstates: Hydrothermal syntheses, structures and properties [J]. Inorganic Chemistry Communications, 2018, 88: 25-29.
[12] 王斌, 赵海燕, 董大朋, 等. 一种镍-取代型有机-无机杂化三维超分子多酸:合成、结构与表征[J]. 化学研究, 2018, 29(3): 245-252. WANG B, ZHAO H Y, DONG D P, et al. A 3D nickel-substituted organic-inorganic hybrid supramolecular polyoxometalate: synthesis, structure and characterization [J]. Chemical Research, 2018, 29(3): 245-252.
[13] ZHENG S T, YANG G Y. Recent advances in paramagnetic-TM-substituted polyoxometalates (TM = Mn, Fe, Co, Ni, Cu) [J]. Chemical Society Reviews, 2012, 41(22): 7623-7646.
[14] 王禹, 赵海燕, 董大朋, 等. 基于1,2-丙二胺配体构筑CuII-LaIII异金属修饰型磷钨酸化合物的合成与表征[J]. 化学研究, 2017, 28(5): 568-574. WANG Y, ZHAO H Y, DONG D P, et al. Synthesis and characterization of a CuII-LaIII heterometallic phosphotungstate containing 1,2-diaminopropane ligand [J]. Chemical Research, 2017, 28(5): 568-574.
[15] CONTANT R. Potassium octadecatungstodiphosphates(V) and related lacunary compounds [J]. Inorganic Syntheses, 1990, 27: 108-109.
[16] SHELDRICK G M. SADABS, Program for siemens area detector absorption corrections [M]. G?ttingen University of G?ttingen, 1990.
[17] SHELDRICK G M. SHELXL97, Program for crystal structure refinement [M]. G?ttingen University of G?ttingen, 1997.
[18] SHELDRICK G M. SHELXL97, Program for crystal structure solution [M]. G?ttingen University of G?ttingen, 1997.
[19] BROWN I D, ALTERMATT D. Bond-valance parameters obtained from a systematic analysis of the inorganic crystal structure database [J]. Acta Crystallographica Section B: Structural Science, 1985, 41(4): 244-247.