中间成功

IF 44.6 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2025-06-25 DOI:10.1038/s41929-025-01373-y

Eren Peterson

引用次数: 0

摘要

合成的镍配合物由三氮杂环烷大环连接，类似于ACS a簇中镍活性位点的三坐标几何结构。从那里，为了分离出代表催化循环每一步的不同络合物，研究人员将金属中心还原并甲基化，从而得到Ni(III) -CH3络合物。甲基化的配合物随后与CO反应，形成Ni(II)（甲基）（CO）。随后，CO插入到Ni(II) -CH3键中，形成Ni(II) -COCH3。重要的是，已经提出了完全分离的Ni（甲基）（CO）中间体，但尚未观察到。Ni（甲基）（CO）的分离为研究CO迁移插入（一种基本的有机金属转化）提供了一个平台。通过用同位素标记的配合物重复这一合成过程，研究小组能够观察到13CO的跳跃，支持假设的可逆初始CO结合，以及可逆迁移插入到Ni(II) -甲基键中。最后，通过首先合成Ni(I) -CO物种然后甲基化，他们确定了结合顺序（甲基对CO）对催化循环无关紧要。Mirica和同事成功地生成了催化机制中的所有关键中间体，包括甲基化、羰基化和硫解，最终生成乙酰辅酶a硫酯。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.