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Highly efficient Co single-atom catalyst for epoxidation of plant oils

机译:高效的CO单原子催化剂,用于植物油的环氧化

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摘要

Epoxidation of bio-derived plant oils is a sustainable route to manufacturing plasticizers, additives in lubricants, and other chemicals. The traditional synthetic approaches suffer from the employment of corrosive mineral acid or expensive peroxides (e.g., H2O2). In this work, we report the epoxidation of plant oils using O-2 as the terminal oxidant catalyzed by Co-N-C/SiO2 single-atom catalyst. The single-atom dispersion of cobalt is confirmed by high-angle annular dark field-STEM and x-ray absorption fine structure techniques. In the epoxidation of methyl oleate under mild reaction conditions (35 degrees C, 0.1 MPa O-2), 99% selectivity to the desired product is achieved at full conversion. Even for crude oils, Co-N-C/SiO2 is also effective and good yields of the corresponding epoxides are obtained. In addition, the catalyst is easily recovered and can be reused five times without obvious decay in catalytic activity/selectivity. A superoxide radical involved reaction mechanism is proposed on the basis of kinetic study and EPR experiment.
机译:生物衍生植物油的环氧化是制造增塑剂、润滑剂添加剂和其他化学品的可持续途径。传统的合成方法因使用腐蚀性矿物酸或昂贵的过氧化物(如H2O2)而受到影响。在这项工作中,我们报道了用Co-N-C/SiO2单原子催化剂催化O-2作为末端氧化剂的植物油环氧化反应。利用高角度环形暗场和x射线吸收精细结构技术证实了钴的单原子色散。在温和的反应条件下(35摄氏度,0.1MPa O-2),油酸甲酯的环氧化反应,在完全转化时,对所需产物的选择性达到99%。即使对于原油,Co-N-C/SiO2也是有效的,并且相应的环氧化合物的产率也很高。此外,催化剂易于回收,可重复使用五次,且催化活性/选择性没有明显衰减。在动力学研究和EPR实验的基础上,提出了超氧自由基参与的反应机理。

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  • 来源
    《The Journal of Chemical Physics》 |2021年第13期|共6页
  • 作者单位

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys CAS Key Lab Sci &

    Technol Appl Catalysis Dalian 116023 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 物理化学(理论化学)、化学物理学;
  • 关键词

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