First Eu(II)/Ln(III) Mixed Complex with High Oxidative Stability

Wei Yongqin; Wang Gaoji; Wu Kechen

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First Eu(II)/Ln(III) Mixed Complex with High Oxidative Stability

机译：具有高氧化稳定性的第一个Eu（II）/ Ln（III）混合配合物

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Due to the instability of divalent europium ions, the heterometallic Eu(II)/Ln(III) complex has not yet been reported. By utilizing coordination chemistry principles, a macrocyclic ligand, N,N',N '',N '''-tetra(2-hydroxy-3-methoxy-5-methylbenzyl)-1,4,7,10-tetra-azacyclododecae (H4L), has been rationally designed to encapsulate Eu2+ and to enable direct formation of the first mixed Eu(II)/Ln(III) complexes, namely, Eu(2)(II)Ln(4)(III)(OH)(4)(NIC)(4)L-2 (Ln = Sm, Eu, Tb; HNIC = nicotinic acid). Two divalent europium ions are trapped within the macrocydic cavities of designed ligands L and are further isolated from the environment by outside phenyl rings and the tetrahedral 4Ln(III) cluster, resulting in the enhanced stability of Eu2+. Cyclic voltammetry experiments showed that the oxidation potential of Eu2+ in the heterovalent 2Eu(II)/4Ln(III) cluster is larger than that for the ferrocene/ferrocenium redox couple, which has never been reported previously for Eu2+-containing complexes. Further development of Eu(II) complexes has been limited because Eu2+ could be easily oxidized to Eu3+. The dramatic oxidative stability of as-synthesized complexes not only verifies the synthetic feasibility but also highlights the prospective applications of mixed Eu(II)/Ln(III) coordination complexes.

机译：由于二价euro离子的不稳定性，尚未报道杂金属的Eu（II）/ Ln（III）配合物。利用配位化学原理，制备大环配体N，N'，N''，N'''-四（2-羟基-3-甲氧基-5-甲基苄基）-1,4,7,10-四氮杂环十二烷（H4L）经过合理设计，可以包封Eu2 +并能够直接形成第一个Eu（II）/ Ln（III）混合复合物，即Eu（2）（II）Ln（4）（III）（OH）（4）（NIC）（4）L-2（Ln = Sm，Eu，Tb; HNIC =烟酸）。两个二价euro离子被困在设计的配体L的大环腔内，并通过外部苯环和四面体4Ln（III）簇与环境进一步隔离，从而增强了Eu2 +的稳定性。循环伏安法实验表明，异价2Eu（II）/ 4Ln（III）簇中Eu2 +的氧化电位大于二茂铁/二茂铁氧化还原对的氧化电位，以前从未对含Eu2 +的络合物进行过报道。 Eu（II）配合物的进一步开发受到限制，因为Eu2 +容易被氧化成Eu3 +。合成后的复合物具有惊人的氧化稳定性，不仅验证了合成可行性，而且突出了混合的Eu（II）/ Ln（III）配位复合物的预期应用。

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《Crystal growth & design》 |2015年第11期|共5页
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Wei Yongqin; Wang Gaoji; Wu Kechen;
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1. First Eu(II)/Ln(III) Mixed Complex with High Oxidative Stability [J] . Wei Yongqin, Wang Gaoji, Wu Kechen Crystal growth & design . 2015,第11期

机译：具有高氧化稳定性的第一个Eu（II）/ Ln（III）混合配合物
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First Eu(II)/Ln(III) Mixed Complex with High Oxidative Stability

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