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[MIII2MII3]基于抗磁性和顺磁性金属配体的三角双锥笼。

[MIII2MII3] trigonal bipyramidal cages based on diamagnetic and paramagnetic metalloligands.

作者信息

Sanz S, O'Connor H M, Martí-Centelles V, Comar P, Pitak M B, Coles S J, Lorusso G, Palacios E, Evangelisti M, Baldansuren A, Chilton N F, Weihe H, McInnes E J L, Lusby P J, Piligkos S, Brechin E K

机构信息

EaStCHEM School of Chemistry , The University of Edinburgh , David Brewster Road , Edinburgh , EH9 3FJ , UK . Email:

UK National Crystallography Service , Chemistry , University of Southampton , Highfield Campus , Southampton , SO17 1BJ , UK.

出版信息

Chem Sci. 2017 Aug 1;8(8):5526-5535. doi: 10.1039/c7sc00487g. Epub 2017 May 19.

DOI:10.1039/c7sc00487g
PMID:28970932
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5618769/
Abstract

A family of five [MIII2MII3] trigonal bipyramidal cages (M = Fe, Cr and Al; M = Co, Zn and Pd; = 0 for and = 6 for ) of formulae [FeCoLCl] (), [FeZnLBr] (), [CrZnLBr] (), CrPdL(dppp) () and AlPdL(dppp) () (where HL is 1-(4-pyridyl)butane-1,3-dione and dppp is 1,3-bis(diphenylphosphino)propane) are reported. Neutral cages were synthesised using the tritopic [ML] metalloligand in combination with the salts CoCl and ZnBr, which both act as tetrahedral linkers. The assembly of the -protected [Pd(dppp)(OTf)] with [ML] afforded the anionic cages of general formula MIII2PdII3. The metallic skeleton of all cages describes a trigonal bipyramid with the M ions occupying the two axial sites and the M ions sitting in the three equatorial positions. Direct current (DC) magnetic susceptibility, magnetisation and heat capacity measurements on reveal weak antiferromagnetic exchange between the Fe and Co ions. EPR spectroscopy demonstrates that the distortion imposed on the {MO} coordination sphere of [ML] by complexation in the {MIII2MII3} supramolecules results in a small, but measurable, increase of the zero field splitting at M. Complete active space self-consistent field (CASSCF) calculations on the three unique Co sites of suggest ≈ -14 cm and / ≈ 0.1, consistent with the magnetothermal and spectroscopic data.

摘要

报道了一族五个[MIII2MII3]三角双锥笼（M = Fe、Cr和Al；M = Co、Zn和Pd；对于 ， = 0，对于 ， = 6），其化学式分别为[FeCoLCl]（）、[FeZnLBr]（）、[CrZnLBr]（）、CrPdL(dppp)（）和AlPdL(dppp)（）（其中HL是1-(4-吡啶基)丁烷-1,3-二酮，dppp是1,3-双(二苯基膦基)丙烷）。中性笼 使用三齿[ML]金属配体与盐CoCl和ZnBr合成，二者均作为四面体连接体。受 -保护的[Pd(dppp)(OTf)]与[ML]组装得到通式为MIII2PdII3的阴离子笼 。所有笼的金属骨架均描述为一个三角双锥，其中M离子占据两个轴向位置，M离子位于三个赤道位置。对 的直流（DC）磁化率、磁化强度和热容量测量表明Fe和Co离子之间存在弱反铁磁交换。电子顺磁共振（EPR）光谱表明，在{MIII2MII3}超分子中络合对[ML]的{MO}配位球施加的畸变导致M处零场分裂有小但可测量的增加。对 的三个独特Co位点进行的完全活性空间自洽场（CASSCF）计算表明 ≈ -14 cm且 / ≈ 0.1，与磁热和光谱数据一致。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/3135365e21e1/c7sc00487g-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/1b5f45e3b097/c7sc00487g-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/c9b4cf8ba199/c7sc00487g-f2.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/a141b7af64b5/c7sc00487g-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/8a8f45f465f6/c7sc00487g-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/cf506fa4ed9e/c7sc00487g-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/3d627c25d650/c7sc00487g-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/3135365e21e1/c7sc00487g-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/1b5f45e3b097/c7sc00487g-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/c9b4cf8ba199/c7sc00487g-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/6dd9cb4559a7/c7sc00487g-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/90a79032787e/c7sc00487g-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/a141b7af64b5/c7sc00487g-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/8a8f45f465f6/c7sc00487g-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/cf506fa4ed9e/c7sc00487g-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/3d627c25d650/c7sc00487g-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cc2b/5618769/3135365e21e1/c7sc00487g-f9.jpg

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