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NH3-Plasma pre-treated carbon supported active iron–nitrogen catalyst for oxygen reduction in acid and alkaline electrolytes
Catalysis Science & Technology ( IF 5 ) Pub Date : 2020/02/06 , DOI: 10.1039/c9cy02545f
Roopathy Mohan 1, 2, 3 , Arindam Modak 1, 2, 3 , Alex Schechter 1, 2, 3
Affiliation  

Metal–nitrogen–carbon (M–N–C) catalysts synthesized by a conventional high-temperature carbonization method are considered as promising electrocatalysts for the oxygen reduction reaction. Herein, we proposed a new approach for the preparation of M–N–C catalysts through NH3-plasma pretreatment of high surface area black pearl carbon. In this study, a pre-treated carbon support facilitated the formation of an Fe–N–C (FeNC/NH3–C) type model catalyst through pyrolysis, acid-treatment, and an additional pyrolysis step. In contrast to untreated FeNC/C, plasma pre-treated FeNC/NH3–C contains Fe3C and Fe–Nx as active catalytic sites. XPS confirms the presence of a high surface concentration of FeNx (43.6%) on FeNC/NH3–C that promotes low oxygen reduction overpotential (0.80 V vs. RHE in 0.5 M H2SO4 and 1.0 V vs. RHE in 0.1 M KOH). Hence plasma activates the surface and incorporates nitrogen, which forms stable Fe–N coordination for accelerating oxygen reduction. Importantly, FeNC/NH3–C shows a lower peroxide yield at 0.6 V vs. RHE (<1.0% in 0.5 M H2SO4 and <2% in 0.1 M KOH) that can reduce the detrimental effect of H2O2 on the catalyst support and exhibits high stability, as seen from thousands of potential cycling stability tests of FeNC/NH3–C in acid solutions. Thereby this plasma-based new synthetic approach can promote more active and stable non-precious metal catalysts.

中文翻译:

NH3-等离子体预处理的碳载活性铁-氮催化剂,用于还原酸性和碱性电解液中的氧气

通过常规的高温碳化方法合成的金属-氮-碳(MC)催化剂被认为是用于氧还原反应的有前途的电催化剂。本文中,我们提出了一种通过NH 3-等离子体预处理高表面积黑珍珠碳制备M–N–C催化剂的新方法。在这项研究中,经过预处理的碳载体通过热解,酸处理和额外的热解步骤促进了Fe–N–C(FeNC / NH 3 –C)型模型催化剂的形成。与未经处理的FeNC / C相比,经过等离子体预处理的FeNC / NH 3 –C包含Fe 3 C和Fe–N x作为活性催化位点。XPS证实存在高表面浓度的FeN x(43.6%)的FeNC / NH 3 -C可促进低氧还原超电势(0.5 MH 2 SO 4中的相对于RHE为0.80 V,0.1 M KOH中的相对于RHE为1.0 V )。因此,等离子体激活了表面并吸收了氮,氮形成了稳定的Fe-N配位,以加速氧的还原。重要的是,RHE相比,FeNC / NH 3 –C在0.6 V时显示出较低的过氧化物收率(在0.5 MH 2 SO 4中为<1.0%,在0.1 M KOH中为<2%),这可以减少H 2 O 2RHE的有害影响。从FeNC / NH的数千次潜在循环稳定性测试中可以看出,催化剂载体具有很高的稳定性。在酸性溶液中为3 –C。因此,这种基于等离子体的新合成方法可以促进活性和稳定性更高的非贵金属催化剂。
更新日期:2020-03-26
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