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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Non-innocent PNN ligand is important for CO oxidation by N2O catalyzed by a (PNN)Ru-H pincer complex: insights from DFT calculations
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Non-innocent PNN ligand is important for CO oxidation by N2O catalyzed by a (PNN)Ru-H pincer complex: insights from DFT calculations

机译：非innocent pnn配体对于通过（pnn）ru-h钳子复合物的N2O催化的N2O氧化是重要的：来自DFT计算的见解

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摘要

Milstein et al. developed an efficient and mild method for CO oxidation by N2O to give CO2 and N-2 catalyzed by a (PNN)Ru-H pincer complex. To gain mechanistic information on this catalytic transformation, the reaction mechanism has been studied using density functional theory (DFT) calculations. It was found that the catalytic cycle for CO oxidation by N2O proceeds in three stages: N2O activation to form a (PNN)Ru-OH intermediate, CO insertion into the Ru-OH bond to form a (PNN)Ru-COOH intermediate and CO2 release from (PNN)Ru-COOH. In the CO2 release stage, CO2 is not released via a -H elimination mechanism as proposed in experiments, instead it is released via a deprotonation mechanism. The calculations demonstrated that the Ru-H bond of the catalyst plays an important role in facilitating the activation of N2O, which is the rate-determining step for the whole catalytic cycle, and the non-innocent PNN ligand is very important for CO oxidation by N2O. Our theoretical results are consistent with the experimental observations and could help design highly efficient catalysts for N2O activation.
机译：Milstein等人。通过N 2 O开发了一种有效和温和的方法，通过N 2 O CO 2和N-2催化A（PNN）Ru-H钳子复合物催化。为了获得该催化转化的机械信息，研究了使用密度泛函理论（DFT）计算研究了反应机理。发现通过N2O共同氧化的催化循环在三个阶段进行：N 2 O活化以形成（PNN）Ru-OH中间体，Co插入Ru-OH键，形成（PNN）Ru-CoOH中间体和CO2从（PNN）Ru-CoOH释放。在CO2释放阶段，CO 2通过实验中提出的-H消除机制释放，而是通过去质子机制释放。该计算证明催化剂的RU-H键在促进N2O的激活方面发挥着重要作用，这是整个催化循环的速率确定步骤，并且非无辜的PNN配体对于CO氧化非常重要n2o。我们的理论结果与实验观察结果一致，可以帮助设计高效的N2O活化催化剂。

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    Xie Hujun; Zhang Yutong; Xiang Chuyue; Li Yang; Fan Ting; Lei Qunfang; Fang Wenjun;

  • 作者单位

    Zhejiang Gongshang Univ Dept Appl Chem Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Gongshang Univ Dept Appl Chem Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Gongshang Univ Dept Appl Chem Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Gongshang Univ Dept Appl Chem Hangzhou 310018 Zhejiang Peoples R China;

    South China Univ Technol Sch Chem &

    Chem Engn Guangzhou 510641 Guangdong Peoples R China;

    Zhejiang Univ Dept Chem Hangzhou 310027 Zhejiang Peoples R China;

    Zhejiang Univ Dept Chem Hangzhou 310027 Zhejiang Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;无机化学;
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