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《中国化学会第九届全国无机化学学术会议论文集——B配位化学》2015年
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Proton Tuned Spin-Crossover for a Mononuclear Iron(Ⅱ) Complex With Amino Group

Qing-Ling Liu  Li-Jing Yang  Yang-Hui Luo  Bai-Wang Sun  
【摘要】:A new iron(Ⅱ)complex based on dihydrobis(1-pyrazolyl)borate{[Fe(H2Bpz2)2(bipy-NH2)]·CH3OH,1}(bipy-NH2=4,4’-diaamino-2,2’-bipyridine)was prepared.1,2 The crystal structure of 1 is made up of mononuclear neutral species where the positive charge of iron(Ⅱ)is neutralized through the coordination of two H2Bpz2 anions,and the bipy-NH2 neutral ligands are used to fill the iron(Ⅱ)coordination sphere,the neutral iron(Ⅱ)species are stacked throughπ‐‐‐πcontacts between the interdigitated bipy-NH2 chelate ligands.The lattice methanol molecules are bind the iron(Ⅱ)species with the amino group through hydrogen bonding contacts.SQUID measurements of 1in solid state revealed the high-spin electron state of this iron(Ⅱ)species,which may attribute to the existence of the hydrogen bonding contacts.The responses of spin-state for compound 1 to the addition of H+have been investigated in butyronitrile solution through the measurement of UV spectrum,by using CF3SO3H.Results revealed that the UV band of metal-ligand charge transfer(MLCT)3 for this iron(Ⅱ)species has increased with the addition of H+(from 1:0 to 1:1),accompanied by color change from light yellow to pink,which means that the low-spin state has been obtained with one amino group on bipy-NH2 ligand been protonated.What’s more,this protonation must occur on the amino group which participant in the formation of hydrogen bond and lead to break of this contact.For this 1:1 state,the MLCT energy between iron(Ⅱ)and bipy-NH2+has decreased by about 0.11ev.While,the protonation of the both amino group lead to the decomposition of this iron(Ⅱ)species.We further investigated the temperature-dependent UV spectrum of this 1:1(complex:CF3SO3H)solution,which revealed the room-temperature spin-crossover form HS to LS in the region 303-273K,with transition temperature T1/2≈297K.To the best of our knowledge,this is the first example of H+tuned spin-crossover.
【作者单位】:School of Chemistry and Chemical Engineering,Southeast University
【分类号】:O641.3

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