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(III) 和 (IV) 甲基-甲基酸盐复合物

Benjamin L L Réant^1,2, John A Seed^1,2, George F S Whitehead²

¹Centre for Radiochemistry Research, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.

Inorganic chemistry

|February 7, 2025

概括

这项研究合成和表征了新型的复合物,其中包括重的m-terphenylthiolate连接体. 这些复合物,包括罕见的nido-metalloboranes,提供了关于-硫结合相互作用的见解.

科学领域:

有机金属化学有机金属化学
化学的化学
协调化学协调化学

背景情况:

复合物因其独特的电子特性和潜在应用而引起人们的兴趣.
新型连接体系统的开发对于控制化合物的反应性和结构至关重要.
庞大的配体可以稳定不寻常的氧化状态和协调几何形状.

研究的目的:

为了合成和描述由庞大的m-terphenylthiolate连接体系统支持的新的晶体复合物,S.Ar.
在各种条件下研究前体与SAR联体的反应性.
探索这些新复合物的结构多样性和结合特性.

主要方法:

使用各种前体 (UCl4,U(BH4) 4,U(BH3) 3 ((toluene)) 和SAr配体 (KSAr,HSAr)) 合成复合物.
包括单晶和粉末X射线衍射,多核NMR,IR,UV-Vis-NIR光谱,SQUID磁力测量和元素分析在内的表征技术.
量子化学计算以阐明U-S结合相互作用.

主要成果:

成功合成了五个晶体复合物 (1-5),具有不同的氧化状态 (U(IV) 和U(III)) 和联体协调.
[UIV(SAr) 2 ((Cl) 2) (1),[UIV(μ-SAr) 4 ((BH4) 2 ((μ-BH4) 3 ((μ-BH4) K)) 2 (2),[UIII(H3B·SAr κS,H,H) 4 ((BH4) 2) 3) 的分离,以及[UIII(SAr) 2 ((μ-B2H6}) ] (4a) 和[UIII(SAr) 4 (BH4) ] (4b) 和[UIII(SAr) 2BH4) ] (5) 的混合物.
识别了复合物4b作为一种罕见的nido-metalloborane的例子.
综合复合物的结构性,光谱性,磁性和电子性质的详细描述.
计算分析提供了对-硫键的性质的见解.

结论:

庞大的SAr配体有效地支持不同氧化状态的多种复合物的合成.
这项研究证明了前体在与甲酸联体的反应中的多功能性.
这些复合物的特征,包括nido-metalloborane,扩大了对协调化学和结合的理解.
量子化学计算是解释复杂系统中的结合的宝贵工具.

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