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Unveiling the Essential Nature of Lewis Basicity in Thermodynamically and Dynamically Promoted Nitrogen Fixation

机译：揭示热力学和动态促进氮固定的Lewis碱性的基本性质

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摘要

Electrochemical N(2)reduction provides a promising alternative to the Haber-Bosch process for sustainable ammonia production but enhancing its selectivity and activity remains a significant challenge. Here, this issue is tackled by triggering strong Lewis basicity within the catalyst, which boosts ambient ammonia synthesis from both thermodynamic and dynamic viewpoints. The enhanced pi back donation induced by the Lewis base as the electron donor is first confirmed by first-principle calculations, which greatly activates the N(sic)N bond and promotes its dissociation. Moreover, as suggested by molecular dynamics simulations, such abundant Lewis base would contribute to more surface heterogeneity and thus enhanced van der Waals interactions between nitrogen and the catalyst. Localized high concentration of N(2)molecules can be realized at the catalyst surface, enabling efficient N(2)delivery with a high flux and benefiting the following reaction process. As expected, the proof-of-concept metal-free catalyst achieves a Faradaic efficiency of 62.9% and ammonia yield rate of 41.1 mu g h(-1)mg(-1)at -0.2 V versus reversible hydrogen electrode. With this Lewis base-assisted strategy, the superior efficiency would greatly reduce the energy loss of the system and cut down the fundamental cost, thus contributing to future practical applications.
机译：电化学N（2）减少为可持续氨生产的Haber-Bosch工艺提供了有希望的替代品，但增强其选择性和活动仍然是一个重大挑战。在这里，通过触发催化剂内的强Lewis碱度来解决该问题，这使得从热力学和动态观点促进了环境氨合成。由Lewis碱基引起的作为电子给体引起的增强的PI回捐赠由第一原理计算证实，这极大地激活N（SiC）N键并促进其解离。此外，如分子动力学模拟所提出的，这种丰富的路易斯碱将有助于更多的表面异质性，因此增强了氮气与催化剂之间的相互作用。局部高浓度的N（2）分子可以在催化剂表面实现，使得能够用高通量提供高效的N（2）递送并有利于以下反应过程。如所预期的，概念证明的无金属催化剂在-0.2V与可逆氢电极的情况下实现了62.9％，氨屈服率为41.1μg（-1）mg（-1）的氨屈服率。借鉴了这一刘易斯辅助战略，卓越的效率将大大降低系统的能量损失，减少基本成本，从而有助于未来的实际应用。

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  • 来源
    《Advanced Functional Materials》 |2020年第32期|2001244.1-2001244.7|共7页
  • 作者

    Wang Mengfan; Liu Sisi; Ji Haoqing; Liu Jie; Yan Chenglin; Qian Tao;

  • 作者单位

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

    Soochow Univ Coll Energy Key Lab Adv Carbon Mat & Wearable Energy Technol Suzhou 215006 Peoples R China;

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

    ammonia synthesis; Lewis base; metal-free catalyst; nitrogen fixation; thermodynamics;

    机译：氨合成;路易斯碱;无金属催化剂;氮固定;热力学;

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