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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
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
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。