Tuning Structural and Electronic Configuration of FeN4 via External S for Enhanced Oxygen Reduction Reaction,Energy & Environmental Materials

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Tuning Structural and Electronic Configuration of FeN4 via External S for Enhanced Oxygen Reduction Reaction
Energy & Environmental Materials ( IF 13.0 ) Pub Date : 2022-11-21 , DOI: 10.1002/eem2.12560
Shidong Li ₁ , Lixue Xia ₁ , Jiantao Li _{1,

2} , Zhuo Chen ₁ , Wei Zhang ₁ , Jiexin Zhu ₁ , Ruohan Yu ₃ , Fang Liu ₃ , Sungsik Lee ₄ , Yan Zhao _{5,

6} , Liang Zhou _{1,

7,

8} , Liqiang Mai _{1,

7,

8}

Affiliation

The Fe–N–C material represents an attractive oxygen reduction reaction electrocatalyst, and the FeN₄ moiety has been identified as a very competitive catalytic active site. Fine tuning of the coordination structure of FeN₄ has an essential impact on the catalytic performance. Herein, we construct a sulfur-modified Fe–N–C catalyst with controllable local coordination environment, where the Fe is coordinated with four in-plane N and an axial external S. The external S atom affects not only the electron distribution but also the spin state of Fe in the FeN₄ active site. The appearance of higher valence states and spin states for Fe demonstrates the increase in unpaired electrons. With the above characteristics, the adsorption and desorption of the reactants at FeN₄ active sites are optimized, thus promoting the oxygen reduction reaction activity. This work explores the key point in electronic configuration and coordination environment tuning of FeN₄ through S doping and provides new insight into the construction of M–N–C-based oxygen reduction reaction catalysts.

中文翻译：

通过外部 S 调整 FeN4 的结构和电子配置以增强氧还原反应

Fe-N-C材料代表了一种有吸引力的氧还原反应电催化剂，并且FeN ₄部分已被确定为非常有竞争力的催化活性位点。 FeN ₄配位结构的微调对催化性能具有重要影响。在此，我们构建了一种具有可控局部配位环境的硫改性Fe-N-C催化剂，其中Fe与四个面内N和轴向外部S配位。外部S原子不仅影响电子分布，还影响电子分布。 FeN ₄活性位点中 Fe 的自旋态。 Fe 较高价态和自旋态的出现表明不成对电子的增加。利用上述特性，优化了反应物在FeN ₄活性位点的吸附和解吸，从而促进了氧还原反应活性。这项工作探索了通过S掺杂调节FeN ₄的电子构型和配位环境的关键点，为构建基于M-N-C的氧还原反应催化剂提供了新的见解。

更新日期：2022-11-21

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