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Electrochemical probing into the active sites of graphitic-layer encapsulated iron oxygen reduction reaction electrocatalysts
Science Bulletin ( IF 18.9 ) Pub Date : 2017-11-24 , DOI: 10.1016/j.scib.2017.11.017
Lijie Zhong 1 , Jens Oluf Jensen 1 , Lars Nilausen Cleemann 1 , Chao Pan 1 , Qingfeng Li 1
Affiliation  

The graphitic-layer encapsulated iron-containing nanoparticles ([email protected]) have been proposed as a potential type of active and stable non-precious metal electrocatalysts (NPMCs) for the oxygen reduction reaction (ORR). However, the contribution of the encapsulated components to the ORR activity is still unclear compared with the well-recognized surface coordinated FeNx/C structure. Using the strong complexing effect of the iron component with anions, cyanide (CN) in alkaline and thiocyanate (SCN) in acidic media, the metal containing active sites are electrochemically probed. Three representative catalysts are chosen for a comparison including the as-prepared encapsulated [email protected], commercial Fe/N/C catalyst with iron–nitrogen coordinated surface functionalities and molecular iron phthalocyanine (FePc) containing well-defined structures and compositions. It was found that all samples showed significant shifts of half-wave potentials indicating that surface Fe coordinated sites in all cases. The [email protected] catalyst showed the weakest poisoning effect (the lowest shifts of half-wave potential) compared to the Fe/N/C and FePc catalysts in both electrolytes. These results could be explained that the encapsulated iron components influence the FeNx/C and/or NxC surface functionality.



中文翻译:

石墨层包封铁氧还原反应电催化剂活性位点的电化学研究

石墨层包封的含铁纳米颗粒([电子邮件保护])已被提议作为用于氧还原反应(ORR)的活性和稳定的非贵金属电催化剂(NPMC)的潜在类型。然而,与公认的表面配位 FeN x /C 结构相比,封装组分对 ORR 活性的贡献仍不清楚。利用铁成分与阴离子的强络合作用,碱中的氰化物(CN -)和硫氰酸盐(SCN -) 在酸性介质中,对含有活性位点的金属进行电化学探测。选择三种代表性催化剂进行比较,包括制备好的封装 [电子邮件保护]、具有铁氮配位表面功能的商用 Fe/N/C 催化剂和包含明确结构和组成的分子铁酞菁 (FePc)。发现所有样品都显示出半波电位的显着变化,表明在所有情况下表面 Fe 配位。与两种电解质中的 Fe/N/C 和 FePc 催化剂相比,[email protected] 催化剂表现出最弱的中毒效应(半波电位的最低偏移)。这些结果可以解释为封装的铁组分影响 FeN x /C 和/或 N xC面功能。

更新日期:2017-11-24
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