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Subnanometer iron clusters confined in a porous carbon matrix for highly efficient zinc–air batteries
Nanoscale Horizons ( IF 9.7 ) Pub Date : 2019/10/08 , DOI: 10.1039/c9nh00510b
Xin Wu 1, 2, 3, 4, 5 , Juncai Dong 3, 5, 6, 7, 8 , Mei Qiu 5, 9, 10, 11 , Yang Li 1, 2, 3, 4, 5 , Yongfan Zhang 5, 12, 13, 14 , Huabin Zhang 1, 2, 3, 4, 5 , Jian Zhang 1, 2, 3, 4, 5
Affiliation  

At the molecular level, metal coordinates are crucial for stabilizing an appropriate electronic configuration for high-efficiency oxygen reduction reaction (ORR) electrocatalysts. In this work, an excellent platform to realize the decoration of Fe coordinates at the subnanometer scale into nitrogen-doped carbon networks (designated as Fe–Fe@NC) is provided. X-ray absorption spectroscopy confirmed the precise configuration of Fe coordinates with Fe–Fe and Fe–N coordinations at the molecular level. As a cathode catalyst, the newly developed Fe–Fe@NC exhibited superior ORR performance and a higher peak power density of 175 mW cm−2 in Zn–air batteries. Unlike most reported pristine Fe-based catalysts, Fe–Fe@NC also showed good oxygen evolution reaction (OER) activity, with a low operating potential (1.67 V vs. RHE) at a current density of 10 mA cm−2. Calculations based on density functional theory revealed that the Fe–Fe coordination in Fe subclusters favored the 4e transfer pathway and, thus, achieved highly active catalytic performance. This work reveals that iron clusters at the subnanometer scale provide an optimized electronic structure for enhanced ORR activity.

中文翻译:

纳米亚铁团簇被限制在多孔碳基质中,用于高效的锌-空气电池

在分子水平上,金属配位对于稳定高效氧还原反应(ORR)电催化剂的合适电子构型至关重要。在这项工作中,提供了一个极好的平台,可将亚纳米级的Fe坐标装饰成氮掺杂的碳网络(称为Fe–Fe @ NC)。X射线吸收光谱法证实了在分子水平上Fe配位与Fe–Fe和Fe–N配位的精确构型。作为阴极催化剂,新开发的Fe-Fe @ NC在锌-空气电池中表现出卓越的ORR性能和175 mW cm -2的更高峰值功率密度。与大多数报道的原始铁基催化剂不同,Fe–Fe @ NC还显示出良好的氧释放反应(OER)活性,且操作电位低(1.67 V相对于RHE)在10 mA cm -2的电流密度下。基于密度泛函理论计算表明,在铁子群集的铁-铁的协调青睐4E -传递路径,因此,实现了高活性的催化性能。这项工作揭示了亚纳米级的铁簇为提高ORR活性提供了优化的电子结构。
更新日期:2020-02-13
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