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首页> 外文期刊>ACS applied materials & interfaces >Covalent Entrapment of Cobalt-Iron Sulfides in N-Doped Mesoporous Carbon: Extraordinary Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions
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Covalent Entrapment of Cobalt-Iron Sulfides in N-Doped Mesoporous Carbon: Extraordinary Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions

机译：N掺杂介孔碳中钴铁硫化物的共价捕集：氧还原和演化反应的非常规双功能电催化剂

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摘要

To alleviate the kinetic barriers associated with ORR (oxygen reduction reaction) and OER (oxygen evolution reaction) in electrochemical systems, efficient nonprecious electrocatalysts are urgently required. Here we report a facile soft-template mediated approach for fabrication of nanostructured cobaltiron double sulfides that are covalently entrapped in nitrogen-doped mesoporous graphitic carbon (Co(0.5)Fe(0.)5S@N-MC). Notably, with a positive half-wave potential (0.808 V) and a high diffusion-limiting current density, the composite material delivers unprecedentedly striking ORR electrocatalytic activity among recently reported nonprecious late transition metal chalcogenide materials in alkaline medium. Various characterization techniques, including X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, are conducted to elucidate the correlation between structural features and catalytic activities of the composite. Moderate substitution and well-dispersion of iron in bimetallic sulfide composites are believed to have positive effect on the adsorption and activation of oxygen-containing species, thus leading to conspicuous ORR and OER catalytic enhancement compared to their monometallic counterparts. Besides, the covalent bridge between active sulfide particles and mesoporous carbon shells provides facile pathways for electron and mass transport. Beneficially, the intimate coupling interaction renders prolonged electrocatalytic performances to the composite. Our results may possibly lend a new impetus to the rational design of bi- or multimetallic sulfides encapsulated in porous carbon with improved performance for electrocatalysis and energy storage applications.
机译：为了减轻与电化学系统中的ORR（氧还原反应）和OER（氧释放反应）有关的动力学障碍，迫切需要有效的非贵金属电催化剂。在这里，我们报告了一种易于制造的软模板介导的方法，该方法用于共价掺杂在氮掺杂的介孔石墨碳（Co（0.5）Fe（0.）5S @ N-MC）中的纳米结构钴铁双硫化物的制造。值得注意的是，复合材料具有正的半波电势（0.808 V）和高的扩散限制电流密度，在碱性介质中，这种材料在最近报道的非贵重的后过渡金属硫属元素化物材料中提供了前所未有的惊人的ORR电催化活性。进行了各种表征技术，包括X射线吸收光谱，X射线光电子能谱和X射线衍射，以阐明复合材料的结构特征与催化活性之间的关系。铁在双金属硫化物复合物中的适度取代和良好分散被认为对含氧物质的吸附和活化具有积极作用，因此与单金属对应物相比，导致显着的ORR和OER催化增强。此外，活性硫化物颗粒和中孔碳壳之间的共价桥为电子和质量传输提供了便捷的途径。有利地，紧密的偶联相互作用使复合物具有延长的电催化性能。我们的研究结果可能为合理设计设计在多孔碳中的双金属或多金属硫化物提供了新的动力，该双金属或多金属硫化物具有改进的性能，可用于电催化和储能应用。

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