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Hierarchical Carbon-Nitrogen Architectures with Both Mesopores and Macrochannels as Excellent Cathodes for Rechargeable Li-O_2 Batteries

机译：具有中孔和大通道的分层碳氮体系结构是可充电Li-O_2电池的出色阴极

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摘要

Lithium-oxygen batteries are attracting more and more interest; however, their poor rechargeability and low efficiency remain critical barriers to practical applications. Herein, hierarchical carbon-nitrogen architectures with both macrochannels and mesopores are prepared through an economical and environmentally benign sol-gel route, showing high electrocatalytic activity and stable cyclability over 160 cycles as cathodes for Li-O_2 batteries. Such good performance owes to the coexistence of macrochannels and mesopores in C-N hierarchical architectures, which greatly facilitate the Li~+ diffusion and electrolyte immersion, as well as provide an effective space for O_2 diffusion and O_2/Li_2O_2 conversion. Additionally, the mechanism of oxygen reduction reactions is discussed with the N-rich carbon materials through first-principles computations. The lithiated pyridinic N provides excellent O_2 adsorption and activation sites, and thus catalyzes the electrode processes. Therefore, hierarchical carbon-nitrogen architectures with both macrochannels and mesopores are promising cathodes for Li-O_2 batteries.
机译：锂氧电池吸引了越来越多的兴趣。但是，它们的可充电性差和效率低仍然是实际应用的关键障碍。在此，通过经济且对环境无害的溶胶-凝胶途径制备了具有大通道和中孔的分级碳氮结构，显示出高的电催化活性和超过160个循环的稳定循环性，可作为Li-O_2电池的阴极。这种良好的性能归因于C-N层次结构中大通道和中孔的共存，这极大地促进了Li〜+的扩散和电解质的浸入，并为O_2的扩散和O_2 / Li_2O_2的转化提供了有效的空间。此外，通过第一性原理计算，对富氮碳材料讨论了氧还原反应的机理。锂化吡啶二氮具有出色的O_2吸附和活化位点，因此可以催化电极过程。因此，具有大通道和中孔的分层碳氮结构是有希望的Li-O_2电池阴极。

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  • 来源
    《Advanced Functional Materials》 |2014年第43期|6826-6833|共8页
  • 作者

    Zhang Zhang; Jie Bao; Chen He; Yanan Chen; Jinping Wei; Zhen Zhou;

  • 作者单位

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

    Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Computational Centre for Molecular Science Institute of New Energy Material Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071, P. R. China;

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