Manipulation of New Married Edge-Adjacent Fe2N5 Catalysts and Identification of Active Species for Oxygen Reduction in Wide pH Range,Advanced Functional Materials

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Manipulation of New Married Edge-Adjacent Fe2N5 Catalysts and Identification of Active Species for Oxygen Reduction in Wide pH Range
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-01-27 , DOI: 10.1002/adfm.202111835
Xingkun Wang ₁ , Zongkun Chen ₁ , Zhongkang Han ₂ , Huiyu Gai ₁ , Jian Zhou ₁ , Yurou Wang ₁ , Peixin Cui ₃ , Junjie Ge ₄ , Wei Xing _{4,

5} , Xusheng Zheng ₆ , Minghua Huang ₁ , Heqing Jiang ₅

Affiliation

Transition metal-nitrogen-carbon-based catalysts (M-N-C) serve as promising alternatives for oxygen reduction reaction (ORR). However, their synthesis generally involves complex pyrolysis reactions, resulting in their high structure heterogeneity and consequently making it difficult to distinguish the catalytic active sites. Herein, atomically dispersed Fe₂ on the hollow carbon spheres are synthesized as the model for insight into the active sites at the atomic level. By virtue of the systematic SCN⁻ poisoning experiments and theoretical calculations, the authors find that both edge-adjacent Fe₂N₅ and graphitic N sites exhibit the pH-dependent poisoning kinetics, beyond a simple and traditional “SCN⁻ poisoning M-N_x sites” notion, helping us to discriminate the edge-adjacent Fe₂N₅ structure and graphitic N species as the bi-active ORR sites in a wide pH range. Moreover, this is the first work to synthesize the new married edge-adjacent Fe₂N₅ structure in an experimental aspect. The original work offers an important insight to pinpoint the active species in different pH media, which can broaden the fundamental understanding to design M-N-C and metal-free-carbon-based catalysts for ORR.

中文翻译：

新型结合边相邻 Fe2N5 催化剂的操作和宽 pH 范围内氧还原活性物质的鉴定

过渡金属-氮-碳基催化剂 (MNC) 可作为氧还原反应 (ORR) 的有希望的替代品。然而，它们的合成通常涉及复杂的热解反应，导致它们的高度结构异质性，因此难以区分催化活性位点。在此，合成了在中空碳球上原子分散的 Fe ₂作为模型，用于深入了解原子水平的活性位点。通过系统的 SCN ^-中毒实验和理论计算，作者发现边缘相邻的 Fe ₂ N ₅和石墨 N 位点都表现出依赖于 pH 值的中毒动力学，超出了简单和传统的“SCN ^-中毒 MN _x位点”的概念，帮助我们将边缘相邻的 Fe ₂ N ₅结构和石墨 N 物种区分为在宽 pH 范围内的双活性 ORR 位点。此外，这是第一个在实验方面合成新结合的边缘相邻Fe ₂ N _{5结构的工作。}最初的工作为确定不同 pH 介质中的活性物质提供了重要的见解，这可以拓宽对设计用于 ORR 的 MNC 和无金属碳基催化剂的基本理解。

更新日期：2022-01-27

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