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A Thorium Chalcogenolate Series Generated by Atom Insertion into Thorium-Carbon Bonds

机译:通过原子插入Thor-碳键中生成的Thor硫属元素化物系列

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摘要

A new thorium monoalkyl complex, Th-(CH_2SiMe_3)(L_3) (L = MeC(N~iPr)_2) (2), undergoes insertion of chalcogen atoms resulting in a series of thorium chalcogenolate complexes, Th(ECH_2SiMe_3)(L_3) (E = S, SS, Se, Te; 5-8). Complex 6 represents the first alkyl disulfide thorium species and illustrates the ability of 2 to undergo controllable, stoichiometric atom insertion. All complexes have been characterized by ~lH and ~(13)C NMR spectroscopy, FTIR, EA, and melting point, and in the case of 1, 2, and 4-8, X-ray crystallography. Insertion was achieved by balancing the thermodynamic driving force of chalcogenolate formation versus the BDE of the pnictogen-chalcogen bond in the transfer reagent. Utilizing Me_3NO as an oxygen atom transfer reagent led to C-H activation and SiMe_4 extrusion rather than oxygen atom insertion, resulting in the alkoxide complex Th(OCH_2NMe_2)(L_3) (4).
机译:一种新的mono单烷基络合物Th-(CH_2SiMe_3)(L_3)(L = MeC(N〜iPr)_2)(2)经历硫族元素原子的插入,生成一系列硫族cha酸or络合物Th(ECH_2SiMe_3)(L_3) (E = S,SS,Se,Te; 5-8)。配合物6代表第一个烷基二硫化th物种,并说明2进行可控的化学计量原子插入的能力。所有配合物的特征在于1H和〜(13)C NMR光谱,FTIR,EA和熔点,以及在1、2和4-8情况下的X射线晶体学。通过平衡硫属元素化物形成的热力学驱动力与转移剂中光原-硫属元素键的BDE平衡来实现插入。使用Me_3NO作为氧原子转移试剂会导致C-H活化和SiMe_4挤出而不是氧原子插入,从而生成醇盐配合物Th(OCH_2NMe_2)(L_3)(4)。

著录项

  • 来源
    《Journal of the American Chemical Society》 |2017年第17期|6261-6269|共9页
  • 作者单位

    Chemical Science Division, Lawrence Berkeley National Laboratory and Department of Chemistry, University of California, Berkeley, California 94720, United States;

    Chemical Science Division, Lawrence Berkeley National Laboratory and Department of Chemistry, University of California, Berkeley, California 94720, United States;

    Chemical Science Division, Lawrence Berkeley National Laboratory and Department of Chemistry, University of California, Berkeley, California 94720, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-18 03:07:57

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