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Spontaneous Atomic Ruthenium Doping in Mo_2CT_X Mxene Defects Enhances Electrocatalytic Activity for the Nitrogen Reduction Reaction

机译:在Mo_2ct_x mxene缺陷中掺杂的自发原子钌增强了用于氮还原反应的电催化活性

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摘要

The electrochemical nitrogen reduction reaction (NRR) process usually suffers extremely low Faradaic efficiency and ammonia yields due to sluggish N(sic)N dissociation. Herein, single-atomic ruthenium modified Mo2CTX MXene nanosheets as an efficient electrocatalyst for nitrogen fixation at ambient conditions are reported. The catalyst achieves a Faradaic efficiency of 25.77% and ammonia yield rate of 40.57 mu g h(-1) mg(-1) at -0.3 V versus the reversible hydrogen electrode in 0.5 m K2SO4 solution. Operando X-ray absorption spectroscopy studies and density functional theory calculations reveal that single-atomic Ru anchored on MXene nanosheets act as important electron back-donation centers for N-2 activation, which can not only promote nitrogen adsorption and activation behavior of the catalyst, but also lower the thermodynamic energy barrier of the first hydrogenation step. This work opens up a promising avenue to manipulate catalytic performance of electrocatalysts utilizing an atomic-level engineering strategy.
机译:电化学氮气还原反应(NRR)过程通常由于N(SiC)n解离而导致的野生效率极低,氨产率。这里,报道了单型原子钌改性的Mo2CTX MxEn纳米片作为环境条件下的用于氮固定的有效电催化剂。该催化剂在-0.3V的-0.3V中实现了25.77%,氨屈服率为40.57μg(-1)mg(-1)的氨屈服率为0.5M k2SO4溶液中的可逆氢电极。 Operando X射线吸收光谱研究和密度泛函理论计算揭示了锚定的单一原子ru在MXENE Nanoshs上充当N-2活化的重要电子回送中心,这不仅可以促进催化剂的氮吸附和活化行为,但也降低了第一氢化步骤的热力学能量屏障。这项工作开辟了一个有前途的途径,以利用原子级工程战略操纵电催化剂的催化性能。

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  • 来源
    《Advanced energy materials》 |2020年第25期|2001364.1-2001364.9|共9页
  • 作者单位

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

    Shanghai Polytech Univ Dept Phys Shanghai 201209 Peoples R China;

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

    Natl Synchrotron Radiat Res Ctr Hsinchu 300 Taiwan;

    Hunan Univ Coll Mat Sci & Engn Changsha 410082 Hunan Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    doping; electrocatalytic nitrogen reduction; MXene;

    机译:掺杂;电催化氮气减少;mxene;

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