通过进入+II氧化状态并使其减少为U (I) 合成子的多电子氧化化学
Megan Keener1, R A Keerthi Shivaraam1, Thayalan Rajeshkumar2
1Group of Coordination Chemistry, Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Journal of the American Chemical Society
|July 13, 2023
概括
研究人员使用联联体合成了新的低价值复合物,包括U (I) 合成物. 这些复合体具有显著的多电子转移能力,为化学开辟了新的途径.
科学领域:
- 无机化学
- 有机金属化学
- 化学
背景情况:
- 低价值复合物的合成 (低于+3氧化状态) 是一个挑战.
- 这些复合物因其多电子转移反应性和电子结构而有意义.
研究的目的:
- 报告一个和两个电子减少的复合物的合成和特征.
- 研究这些低价值物种的电子结构和多电子转移能力.
主要方法:
- 通过与结合的三氧化物三脚连接体支持的复合物的合成.
- 使用EPR,UV/vis/NIR光谱,磁性测量,循环电压测量和计算研究进行表征.
- 与氧化基质 (亚和环乙烯) 的反应,以证明电子转移.
主要成果:
- 成功合成单降解II和二降解I复合物.
- 复杂的2-密码被描述为通过- δ-结合稳定的U{\displaystyle U} .
- 复合体3和3-crypt具有一个具有二基的U(III) 离子.
- 循环电压测量确定了三个氧化还原波,对应于U ((IV) /U ((III),U ((III) /U ((II) 和U ((II) /U ((III) - ((arene) 双.
- 复合体2和3分别表现出两个和三个电子传输能力.
结论:
- 连接的三氧化物三脚联体是访问低价值化学的有效平台.
- 合成的复合物显示出显著的多电子转移途径.
- 这项研究提供了第三个U (I) 合成的例子,推进了低价值化学领域.
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