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首页> 外文期刊>ACS catalysis >Construction of Spatial Effect from Atomically Dispersed Co Anchoring on Subnanometer Ru Cluster for Enhanced N-2-to-NH3 Conversion
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Construction of Spatial Effect from Atomically Dispersed Co Anchoring on Subnanometer Ru Cluster for Enhanced N-2-to-NH3 Conversion

机译：从亚体仪ru簇锚定的空间效应构建增强N-2至NH3转换

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摘要

Simultaneously achieving a low activation barrier with weak binding of intermediates on a heterogeneous catalyst for the enhancement of catalytic performance under mild conditions remains a great challenge, especially for N-2-to-NH3 conversion. Herein, for the first time, we report a new strategy via integrating vacuum-freeze-drying and high-temperature pyrolysis technologies to design atomically dispersed Co deposits onto the surface of Ru tiny subnanoclusters (TCs). The special structure of this catalyst can generate a spatial effect and induce strong interelectronic interactions between Ru and Co. The outcome is simultaneous generation of the high-surface-unoccupied Co 3d charge and obvious upshifting of the Ru d-band center. With that, there is lowering of N-2 activation energy via strong electron "sigma-donation and pi-backdonation" between Ru and N-2 molecules. More importantly, our studies demonstrate that an appropriate Ru structure with tiny subnanoclusters rather than single Ru atoms or large Ru clusters could enable the repulsion to adsorption of the N-containing intermediates on the catalyst surface, resulting in weakening of the binding of NH3 and N(2)H(4)intermediates on the Co1Ru TC catalyst surface. In such a case, the scaling relation over Co1Ru TCs in NH3 synthesis was decoupled, and the developed Ba-promoted Co1Ru TC catalyst shows the highest NH3 synthesis rate (up to 21.90 mmol(NH3) g(-1) h(-1) at 360 degrees C and 3 MPa) among the Ru or Co-based catalysts ever reported.
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  • 来源
    《ACS catalysis》 |2021年第8期|共11页
  • 作者

    Zhang Yangyu; Li Jiejie; Cai Jihui; Yang Linlin; Zhang Tianhua; Lin Jianxin; Wang Xiuyun; Chen Chongqi; Zheng Lirong; Au Chak-tong; Yang Bo; Jiang Lilong;

  • 作者单位

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    ShanghaiTech Univ Sch Phys Sci &

    Technol Shanghai 201210 Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    Chinese Acad Sci Inst High Energy Phys Beijing 100049 Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian Peoples R China;

    ShanghaiTech Univ Sch Phys Sci &

    Technol Shanghai 201210 Peoples R China;

    Fuzhou Univ Natl Engn Res Ctr Chem Fertilizer Catalyst Fuzhou 350002 Fujian 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

    atomically dispersed; clusters; ammonia synthesis; electronic structure; spatial effect;

    机译：原子分散;簇;氨合成;电子结构;空间效果;

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