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通过基于基的氧化非无辜性产生和氧化反应的Ni (II) 超氧复合物

Andrew J McNeece¹, Kate A Jesse¹, Jiaze Xie¹

¹Department of Chemistry, University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States.

Journal of the American Chemical Society

|May 21, 2020

概括

含有氧化还原活性联体的复合物激活氧气进行氧化反应. 这种使用基电子转移的策略使能够进行通常在铁和铜中看到的氧化.

科学领域:

无机化学
有机金属化学
生物模拟化学

背景情况:

金属连接体的合作性对于激活O2至关重要,血红细胞中心是主要的生物学例子.
虽然Fe和Cu在有氧氧化中很常见,但由于具有挑战性的氧化还原潜力,基于Ni的系统不太常见.
一些Ni酶使用专门的配体调整Ni (II) /Ni (III) 氧化还原对,但存在替代策略.

研究的目的:

探索一种新的介导氧激活策略,使用基于基的还原剂.
合成和表征 Ni 复合物与氧化还原活性联体 2,5-bis (((2-t-butylhydrazono)) ((p-tolyl) methyl) -pyrrole (DHP).
证明这些复合物在激活O2和执行氧化反应的能力.

主要方法:

含有氧化还原活性DHP联体的Ni复合物的合成.
由此产生的Ni-superoxo物种的特征.
对超氧复合物在酒精和碳化合物的氧化中的催化活性进行评估.

主要成果:

通过Ni-DHP复合体成功激活O2,形成一个Ni(II) 超氧物种.
通过基于联体的电子转移产生超氧复合体.
超复合物在酒精和碳化合物的石化氧化方面表现出能力.

结论:

将基于联体的氧化还原活性与氧化还原无活性Ni中心相结合,为O2激活提供了新的途径.
这种方法使Ni能够调解通常与Fe和Cu相关的氧化转换.
这些发现为生物酶机制提供了合成先例,其中涉及基于体的电子转移以进行氧结合.

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