通过内层酸盐降解形成Ce (IV) 氧化物复合物
Peter L Damon1, Guang Wu1, Nikolas Kaltsoyannis2
1Department of Chemistry & Biochemistry, University of California , Santa Barbara, California 93106, United States.
Journal of the American Chemical Society
|September 14, 2016
概括
这项研究详细介绍了一种新型氧复合物的合成,[Li(12-crown-4][NN
科学领域:
- 有机金属化学
- 无机合成
- 兰化物化学
背景情况:
- 复合物在催化和材料科学中具有价值.
- 了解氧物种的结合和反应性对于开发新合成方法至关重要.
研究的目的:
- 合成和描述一个新的氧复合物.
- 研究氧联体的反应性和电子结构.
- 将-氧结合与类似的系统进行比较.
主要方法:
- 在12-crown-4的存在下,酸与胺基发生反应.
- 氧复合物和酸盐中间体的分离和表征.
- 复合物与化的反应以探测联体的核友性.
- 使用自然键轨道 (NBO) 和分子中的原子量子理论 (QTAIM) 方法进行计算分析.
主要成果:
- 在36%的产量中通过内部球酸盐的减少合成[Li{12-crown-4) ][NN' 3) Ce{O) ].
- 形成一个Ce(III) 酸盐中间体,[Li(12-crown-4) ][(NN' 3) Ce(κ 2-O 2NO) ] (2).
- 通过与化反应形成 (NN' 3) Ce(OSi tBuMe 2) 的核性质的确认 (3).
- 根据NBO和QTAIM的分析,Ce-O债券具有类似于U-O债券的重大共价性.
结论:
- 一种新型的氧复合物成功合成和特征化.
- 氧联体表现出核友性行为,使其进一步功能化.
- Ce-O 键的电子结构具有重要的共价性质,与系统可比,为 f 元素键提供了洞察力.
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