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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Bis[1,1'-N,N'-(2-picolyl)aminomethyl]ferrocene as a redox sensor for transition metal ions
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Bis[1,1'-N,N'-(2-picolyl)aminomethyl]ferrocene as a redox sensor for transition metal ions

机译：双[1,1'-N，N'-（2-吡啶甲基）氨基甲基]二茂铁作为过渡金属离子的氧化还原传感器

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摘要

The compound bis[1,1'-N,N'-(2-picolyl)aminomethyl]ferrocene, L~1, was synthesized. The protonation constants of this ligand and the stability constants of its complexes with Ni~(2+), Cu~(2+), Zn~(2+), Cd~(2+) and Pb~(2+) were determined in aqueous solution by potentiometric methods at 25 ℃ and at ionic strength 0.10 mol dm~(-3) in KNO_3. The compound L~1 forms only 1:1 (M:L) complexes with Pb~(2+) and Cd~(2+) while with Ni~(2+) and Cu~(2+) species of 2:1 ratio were also found. The complexing behaviour of L~1 is regulated by the constraint imposed by the ferrocene in its backbone, leading to lower values of stability constants for complexes of the divalent first row transition metals when compared with related ligands. However, the differences in stability are smaller for the larger metal ions. The structure of the copper complex with L~1 was determined by single-crystal X-ray diffraction and shows that a species of 2:2 ratio is formed. The two copper centres display distorted octahedral geometries and are linked through the two L~1 bridges at a long distance of 8.781(10) A. The electrochemical behaviour of L~1 was studied in the presence of Ni~(2+), Cu~(2+), Zn~(2+), Cd~(2+) and Pb~(2+), showing that upon complexation the ferrocene-ferrocenium half-wave potential shifts anodically in relation to that of the free ligand. The maximum electrochemical shift (ΔE_(1/2)) of 268 mV was found in the presence of Pb~(2+), followed by Cu~(2+) (218 mV), Ni~(2+) (152 mV), Zn~(2+) (111 mV) and Cd~(2+) (110 mV). Moreover, L~1 is able to electrochemically and selectively sense Cu~(2+) in the presence of a large excess of the other transition metal cations studied.
机译：合成了双[1,1'-N，N'-（2-吡啶甲基）氨基甲基]二茂铁L〜1。确定了该配体的质子化常数及其与Ni〜（2 +），Cu〜（2 +），Zn〜（2 +），Cd〜（2+）和Pb〜（2+）的配合物的稳定性常数。在25℃和KNO_3中离子强度为0.10 mol dm〜（-3）的电位法测定水溶液中的铜离子含量。化合物L〜1与Pb〜（2+）和Cd〜（2+）仅形成1：1（M：L）配合物，而Ni〜（2+）和Cu〜（2+）物种为2：1还发现比率。 L〜1的络合行为受二茂铁在其主链中施加的约束条件调节，导致与相关配体相比，二价第一行过渡金属络合物的稳定常数值较低。但是，对于较大的金属离子，稳定性差异较小。通过单晶X射线衍射确定具有L〜1的铜络合物的结构，并显示形成了2：2比率的物种。两个铜中心显示扭曲的八面体几何形状，并通过两个L〜1桥以8.781（10）A的长距离连接。在Ni〜（2 +），Cu的存在下研究L〜1的电化学行为〜（2 +），Zn〜（2 +），Cd〜（2+）和Pb〜（2+），表明在络合时，二茂铁-二茂铁an的半波电势相对于游离配体的电势发生阳极移位。在Pb〜（2+）存在下发现最大电化学位移（ΔE_（1/2））为268 mV，其次是Cu〜（2+）（218 mV），Ni〜（2+）（152 mV） ），Zn〜（2+）（111 mV）和Cd〜（2+）（110 mV）。此外，在大量研究的其他过渡金属阳离子存在下，L〜1能够电化学和选择性地感测Cu〜（2+）。

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