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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Chemical Nature of Catalytic Active Sites for the Oxygen Reduction Reaction on Nitrogen-Doped Carbon-Supported Non-Noble Metal Catalysts
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Chemical Nature of Catalytic Active Sites for the Oxygen Reduction Reaction on Nitrogen-Doped Carbon-Supported Non-Noble Metal Catalysts

机译：氮掺杂碳载非贵金属催化剂上氧还原反应催化活性位的化学性质

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摘要

Much work has been devoted to synthesizing the non-noble metal catalyst such as nitrogen-doped carbon supported transition metal catalysts (denoted as metal-N-C catalyst) for the oxygen reduction reaction (ORR). However, the catalytic mechanisms and precise chemical nature of the active sites in this kind of catalyst are still controversial, which hinders the development and commercialization of this novel ORR catalyst. The objective of this work is to study the nature of active sites for ORR in the Fe-N-C catalysts. We synthesized a new family of nitrogen-doped carbon with iron catalysts (denoted as Fe-N-C catalysts) by pyrolyzing the mixtures with various ratios of a nitrogen-atom rich heterocycle compound, 1-ethyl-3-methylimidazolium dicyanamide (EMIM-dca), and iron chloride (FeCl3). The ORR activity (J(K) at 0.8 V vs RHE, in 0.1 M KOH solution) of a typical catalyst, Fe-15-N-C1000, in this family is 6.65 mA/mg, which is much higher than the values of the Fe-C (0.48 mA/mg) and N-C catalysts (0.25 mA/mg). The relationship between the ORR activity and the structures (the possible active sites in particular) of the catalysts was studied under different conditions. The active site in the catalyst is found to be the Fe-N species (most likely in the form of Fe3N). Metallic iron (Fe) particles, Fe3C species, and N-C species are not catalytically active sites, nor do these moieties interact with the Fe-N active sites during the catalysis of the ORB. High pyrolysis temperatures and increasing the Fe content during the synthesis favor the formation of the Fe-N active sites in the final catalyst. Our study opens up new synthetic control of parameters affecting the final structure and catalyst performance and allows modifying the unexplored avenues toward new multiply heteroatom doped nonprecious ORR catalysts.
机译：已经进行了许多工作来合成用于氧还原反应（ORR）的非贵金属催化剂，例如掺杂氮的碳负载的过渡金属催化剂（称为金属-N-C催化剂）。然而，这种催化剂的催化机理和活性部位的精确化学性质仍存在争议，这阻碍了这种新型ORR催化剂的开发和商业化。这项工作的目的是研究Fe-N-C催化剂中ORR活性位的性质。我们通过热解具有各种比例的富氮原子杂环化合物1-乙基-3-甲基咪唑二氰胺（EMIM-dca）的混合物，用铁催化剂（称为Fe-NC催化剂）合成了一个新的氮掺杂碳族。以及氯化铁（FeCl3）。典型催化剂Fe-15-N-C1000在该族中的ORR活性（相对于RHE在0.8V下的J（K），在0.1M KOH溶液中）为6.65 mA / mg，远高于其值Fe-C（0.48 mA / mg）和NC催化剂（0.25 mA / mg）。在不同条件下研究了ORR活性与催化剂的结构（特别是可能的活性部位）之间的关系。发现催化剂中的活性部位是Fe-N物种（最有可能以Fe3N的形式）。金属铁（Fe）颗粒，Fe3C物种和N-C物种不是催化活性位，在ORB催化过程中，这些部分也不与Fe-N活性位相互作用。合成过程中较高的热解温度和增加的Fe含量有助于最终催化剂中形成Fe-N活性位。我们的研究为影响最终结构和催化剂性能的参数开辟了新的合成控制方法，并允许修改未探索的方法，以开发新型的多杂原子掺杂的非贵金属ORR催化剂。

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