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首页> 外文期刊>RSC Advances >Design strategies for the development of a Pd-based acetylene hydrochlorination catalyst: improvement of catalyst stability by nitrogen-containing ligands
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Design strategies for the development of a Pd-based acetylene hydrochlorination catalyst: improvement of catalyst stability by nitrogen-containing ligands

机译：基于PD乙炔氢氯化催化剂的开发的设计策略：通过含氮配体改善催化剂稳定性

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摘要

Acetylene hydrochlorination is an attractive chemical reaction for the manufacture of polyvinyl chloride (PVC), and the development efforts are focused on the search for non-mercury catalyst systems. Supported Pd-based catalysts have relatively high activity in the catalytic hydrochlorination of acetylene but are still deactivated rather quickly. Herein, we demonstrated that the atomically dispersed (NH4)(2)PdCl4 complex, distributed on activated carbon, enabled the highly active and stable production of the vinyl chloride monomer (VCM) through acetylene hydrochlorination under low temperature conditions. We found that the presence of nitrogen-containing ligands in the structure of the active center could remarkably improve the stability of the Pd-based catalysts when compared with the case of the conventional PdCl2 catalyst. Further analyses via X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and temperature-programmed reduction (TPR) show that the variations in the Pd dispersion, chemical state and reduction property are caused by the nitrogen-containing ligands. Temperature-programmed desorption (TPD) characterizations illustrated that the N-containing ligands over the (NH4)(2)PdCl4/AC catalyst might enhance the adsorption of HCl. These findings suggest that in addition to strategies that target the doping modification of support materials, optimization of the structure of the active center complexes provides a new path for the design of highly active and stable Pd-based catalysts.
机译：乙炔氢氯化是一种有吸引力的化学反应，用于制造聚氯乙烯（PVC），开发努力集中在寻找非汞催化剂体系上。支持的Pd基催化剂在乙炔的催化氢氯化物中具有相对高的活性，但仍然仍然迅速消失。在此，我们证明，在活性炭上分布的原子分散（NH 4）（2）PdCl4配合物，使氯乙烯单体（VCM）的高活性和稳定地产生通过在低温条件下乙炔氢氯化物。我们发现，与常规PDCl2催化剂的情况相比，活性中心结构中的含氮配体的存在在活性中心的结构中可以显着提高Pd基催化剂的稳定性。通过X射线衍射（XRD）进一步分析，透射电子显微镜（TEM），X射线光电子能谱（XPS）和温度编程的减少（TPR）表明PD分散，化学状态和减少特性的变化是引起的通过含氮配体。温度编程的解吸（TPD）表明（TPD）表明（NH 4）（2）PDCl4 / AC催化剂上含N的配体可能增强HCl的吸附。这些发现表明，除了靶向掺杂磷酸盐改性的策略之外，活性中心复合物的结构的优化提供了一种高活性和稳定的Pd基催化剂的新路径。

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  • 来源
    《RSC Advances》 |2019年第37期|共7页
  • 作者

    He Haihua; Zhao Jia; Wang Bolin; Yue Yuxue; Sheng Gangfeng; Wang Qingtao; Yu Lu; Hu Zhong-Ting; Li Xiaonian;

  • 作者单位

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Coll Environm Hangzhou 310014 Zhejiang Peoples R China;

    Zhejiang Univ Technol Ind Catalysis Inst Lab Breeding Base Green Chem Synth Technol Hangzhou 310014 Zhejiang Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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