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Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc-Air Batteries

机译:了解钴单原子和小纳米颗粒的协同作用:增强氧气减少反应催化活性和锌空气电池的稳定性

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摘要

The development of earth-abundant oxygen reduction reaction (ORR) catalysts with high catalytic activity and good stability for practical metal-air batteries remains an enormous challenge. Herein, a highly efficient and durable ORR catalyst is reported, which consists of atomically dispersed Co single atoms (Co-SAs) in the form of Co-N4 moieties and small Co nanoparticles (Co-SNPs) co-anchored on nitrogen-doped porous carbon nanocage (Co-SAs/SNPs@NC). Benefiting from the synergistic effect of Co-SAs and Co-SNPs as well as the enhanced anticorrosion capability of the carbon matrix brought by its improved graphitization degree, the resultant Co-SAs/SNPs@NC catalyst exhibits outstanding ORR activity and remarkable stability in alkaline media, outperforming Co-SAs-based catalyst (Co-SAs@NC), and benchmark Pt/C catalyst. Density functional theory calculations reveal that the strong interaction between Co-SNPs and Co-N4 sites can increase the valence state of the active Co atoms in Co-SAs/SNPs@NC and moderate the adsorption free energy of ORR intermediates, thus facilitating the reduction of O-2. Moreover, the practical zinc-air battery assembled with Co-SAs/SNPs@NC catalyst demonstrates a maximum power density of 223.5 mW cm(-2), a high specific capacity of 742 W h kg(-1) at 50 mA cm(-2) and a superior cycling stability.
机译:具有高催化活性的地球丰氧还原反应(ORR)催化剂的发展仍然是实用金属电池的良好稳定性仍然是巨大的挑战。在此,报告了一种高效和耐用的ORR催化剂,其包括以共n4部分和小CO纳米粒子(CO-SNP)的形式的原子分散的CO单个原子(CO-SAS)在氮气掺杂的多孔上锚定碳纳米载(CO-SAS / SNPS @ NC)。受益于CO-SAS和CO-SNP的协同作用以及通过其改进的石墨化程度提高的碳基质的增强的防腐能力,所得的CO-SAS / SNPS @ NC催化剂在碱性的含量呈现出色的ORR活性和显着的稳定性培养基,优于基于CO-SAS的催化剂(CO-SAS @ NC)和基准PT / C催化剂。密度函数理论计算表明,CO-SNP和CO-N4位点之间的强相互作用可以增加CO-SAS / SNPS @ NC中活性CO原子的价态,并中间体中间体的吸附自由能量,从而便于减少O-2的。此外,用CO-SAS / SNPS @ NC催化剂组装的实用锌 - 空气电池显示出223.5 mW cm(-2)的最大功率密度,高特定容量为742Wh kg(-1),50 mA cm( -2)和优异的循环稳定性。

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  • 来源
    《Advanced Functional Materials》 |2021年第45期|2104735.1-2104735.11|共11页
  • 作者单位

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore;

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore;

    Nanyang Technol Univ Sch Phys & Math Sci 21 Nanyang Link Singapore 637371 Singapore;

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore;

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore;

    Univ Elect Sci & Technol China Inst Fundamental & Frontier Sci Chengdu 611731 Peoples R China|Univ Elect Sci & Technol China Yangtze Delta Reg Inst Huzhou Huzhou 313002 Peoples R China;

    Hainan Univ State Key Lab Marine Resource Utilizat South Chin Haikou 570228 Hainan Peoples R China|Jilin Univ State Key Lab Inorgan Synth & Preparat Chem Coll Chem Changchun 130012 Jilin Peoples R China;

    Jilin Univ State Key Lab Inorgan Synth & Preparat Chem Coll Chem Changchun 130012 Jilin Peoples R China;

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore|Nanyang Technol Univ Sch Elect & Elect Engn Singapore 639798 Singapore|CINTRA CNRS NTU THALES UMI 13288 Res Techno Plaza So Nanyang Dr Border X Block Singapore 637553 Singapore;

    Nanyang Technol Univ Sch Mat Sci & Engn 50 Nanyang Ave Singapore 639798 Singapore;

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

    nanoparticles; nitrogen-doped carbon; oxygen reduction reaction; single atom catalyst; zinc-air batteries;

    机译:纳米颗粒;氮掺杂碳;氧还原反应;单原子催化剂;锌 - 空气电池;

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