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首页> 外文期刊>Crystal growth & design >Enhanced Catalytic Performance for Oxygen Reduction Reaction Derived from Nitrogen-Rich Tetrazolate-Based Heterometallic Metal-Organic Frameworks
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Enhanced Catalytic Performance for Oxygen Reduction Reaction Derived from Nitrogen-Rich Tetrazolate-Based Heterometallic Metal-Organic Frameworks

机译：增强氧还原反应的催化性能，衍生自富含氮的四斋酸盐的杂核金属 - 有机框架

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摘要

Efficient non-noble metal catalysts for oxygen reduction reaction (ORR) have been highly attractive for the fabrication of cost-effective fuel cells. Metal-organic frameworks (MOFs) derived heteroatom-doped carbon-based (NC) electrocatalysts have exhibited comparable electrocatalytic activity for ORR as commercial Pt/C catalyst, which were highly dependent on their MOF precursor/template structures. In this particular work, two NC composites, NC-1100 and MnO@NC-1100 (NC, nitrogen-doped carbon), have been successfully synthesized, which were derived from novel nitrogen-rich tetrazolate-based metal-organic frameworks, [Cd-2(L)(OH)(H2O)] (1) and [Cd3Mn(L)(2)(OH)(2)(H2O)(2)] (2) (L, 5'-(4-(1H-tetrazol-5-y1)(benzamido)benzene-1,3-dioic acid), respectively. The structural differences between complexes 1 and 2 arose from the introduction of Mn(II) to complex 2, where the Cd(II) in 1 was partially replaced by Mn(II). Both complexes 1 and 2 possessed three-dimensional (3D) structures with one-dimensional (1D) open channels. The resultant MnO@NC-1100 from the pyrolysis of complex 2 at 1100 degrees C under Ar atmosphere has indicated much better electrocatalystic behavior for ORR over the NC-1100 from complex 1, due to the existence of additional active sites of cubic phase MnO particles. The presence of initial Cd(II) benefits the spatial isolation of Mn(II) and prevents the sintering of MnO during the pyrolysis for MnO@NC-1100. The evaporation of Cd(II) and the explosion of nitrogen-rich tetrazolate groups would also promote the surface area of the resulting catalysts. Our study further demonstrated that the multiple metal centers of MOF could be the rational strategy to enhance the electrocatalytical performance. Compared with NC-1100, MnO@NC-1100 exhibited the enhanced electrocatalytic activity with an onset potential (E-onset) of 0.90 V and a half-wave potential (Ehalf-wave) of 0.74 V, which provided an insight view of the structure property relationship.
机译：高效的用于氧还原反应（ORR）的非贵金属催化剂对制造成本有效的燃料电池具有高度吸引力。金属有机框架（MOF）衍生的杂原子掺杂的碳基（NC）电催化剂表现出与商业PT / C催化剂的可相当的电催化活性，其高度依赖于其MOF前体/模板结构。在这种特殊的工作中，已经成功地合成了两种NC复合材料，NC-1100和MNO @ NC-1100（NC，氮掺杂碳），其衍生自新富含富含氮的四唑基金属 - 有机骨架[CD -2（1）（OH）（H 2 O）]（1）和[CD3MN（1）（2）（2）（2）（2）（2）（2）（2））]（2）（L，5' - （4-（分别为1H-四唑-5-Y1）（苯甲酰氨基）苯-1,3-二酸）。复合物1和2之间的结构差异从引入Mn（II）至复合物2，其中CD（II）在1中被Mn（II）部分替换。复合物1和2都具有三维（3D）结构，其中一维（1D）开放通道。来自络合物2的热解2的得到的MNO @ NC-1100在1100度下由于立方相MNO颗粒的另外的活性位点存在，AR气氛下的C在AR气氛下表明ORR的电催化行为更好。初始CD（II）的存在有利于MN的空间隔离（ II）并防止烧结Mn o在MNO @ NC-1100的热解期间。 CD（II）的蒸发和富含氮的四唑基团的爆炸还将促进所得催化剂的表面积。我们的研究进一步证明了MOF的多种金属中心可以是增强电催化性能的合理策略。与NC-1100相比，MNO @ NC-1100表现出增强的电催化活性，具有0.90V的起始电位（E-ONSET）和0.74V的半波电位（EHALF波），其提供了洞察观点结构财产关系。

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  • 来源
    《Crystal growth & design》 |2019年第5期|共9页
  • 作者

    Ji Li-Qian; Yang Jing; Zhang Zi-You; Qian Yong; Su Zhi; Han Min; Liu Hong-Ke;

  • 作者单位

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Normal Univ Coll Chem &

    Mat Sci Jiangsu Collaborat Innovat Ctr Biomed Funct Mat Jiangsu Key Lab Biofunct Mat Nanjing 210046 Jiangsu Peoples R China;

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  • 正文语种 eng
  • 中图分类 晶体学;
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