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氧化三脚连体作为稳定兰坦化物在+4氧化状态中的支架

Maxime Tricoire¹, Fang-Che Hsueh¹, Megan Keener¹

¹Group of Coordiantion Chemistry, Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL) 1015 Lausanne Switzerland marinella.mazzanti@epfl.ch.

Chemical science

|May 10, 2024

概括

研究人员开发了一种新的氧化物联体,以稳定难以捉摸的高价值兰坦化物复合物,特别是分离了第一个多牙 terbium (IV) 复合物. 这一突破推动了高价值兰坦化物化学的发展.

科学领域:

协调化学协调化学
有机金属化学有机金属化学
兰化物化学兰化物化学

背景情况:

除了之外,在+4氧化状态中分离胺复合物在合成上是具有挑战性的.
之前只报告了四种 (terbium) 复合物,这凸显了兰坦化物稳定较高氧化状态的困难.

研究的目的:

开发一种新型的合成策略,用于稳定高价值的化物复合物,特别是.
为了研究氧化联体对兰坦化复合物的氧化还原特性的影响.
通过强大的联结体设计,扩大高价值化物化学的范围.

主要方法:

使用具有不同电子性质的三脚三离子氧化连接体合成兰坦化 (III) 复合物.
电化学研究 (循环电压测量) 来确定Ln(III) /Ln(IV) 对的氧化还原潜力.
兰化物 (III) 复合物的化学氧化,以产生和分离兰化物 (IV) 种.
单独的兰坦化 (((IV) 复合物的晶体学特征.

主要成果:

与具有电子捐赠的基替代的氧化连接体的兰化 (III) 复合体,与具有三-丁氧化连接体的复合体相比,其氧化潜力呈现出阴极转移.
添加一个trifenylsiloxide连接体进一步促进了进入兰化物状态.
通过化学氧化分离和表征了第一个多牙 terbium ((IV) 复合物,[Tb^IV((OSiPh₂Ar) ₃-arene) ((OSiPh₃) ((MeCN) ₂.
通过使用开发的氧化平台,成功制备和表征 (IV) 复合物.

结论:

设计的氧化三脚三离子连接体有效地稳定了高价值的类离子,特别是Tb (IV).
氧化连接体和辅助连接体的电子调节显著影响Ln(III) /Ln(IV) 氧化还原潜力.
这项工作为访问和研究更广泛的高价值化物化学提供了一个多功能平台.

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