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N-doped carbon nanoflower-supported Fe-N4 motifs for high-efficiency reduction of oxygen in both alkaline and acid
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-05-21 , DOI: 10.1016/j.cej.2021.130401
Danni Wang , Yinglong Wu , Zongge Li , Hao Pan , Yaqun Wang , Miaosen Yang , Guoxin Zhang

Simultaneously improving the loading and accessibility of atomically dispersed metal sites to achieve high-activity and high-throughput electrocatalysis is important yet challenging. Herein, a simple method based on formamide chemistry was developed for the efficient synthesis of 3D flower-like N-doped carbons decorated with highly loaded atomic Fe-N4 motifs. Approximately twice as much atomic Fe (6.84 wt%) was loaded due to the introduction of 2,1,3-benzothiadiazole (Bz) as additional ligands in the preparation of formamide-derived binary ZnFe-NC (f-ZnFe-NC). Meanwhile, with the promotion of Bz, the f-ZnFe-NC precursor also showed improved 3D flower structure that could be robustly inherited into the formation of flower-like Fe-NC product after high-temperature treatment, leading to the obtainment of rich open pores for exposing more atomic Fe sites (site density of 26.6 umol g−1 and turnover of frequency of 1.73 s−1) for oxygen reduction electrocatalysis. Electrochemical measurements showed that the Bz-promoted synthesized Fe-NC (referred to as Bz-Fe1-NC) possessed superior onset potential (1.04 V) and half-wave potential (0.94 V), and its assembled Al-air battery provided a very large specific power of 238.2 mW cm−2 along with high-rate capability and good long-term stability.



中文翻译:

N掺杂的碳纳米花支持的Fe-N 4图案,可高效减少碱性和酸性条件下的氧气

同时改善原子分散的金属位点的负载和可及性以实现高活性和高通量电催化是重要但具有挑战性的。本文中,开发了一种基于甲酰胺化学的简单方法,用于高效合成装饰有高负载原子Fe-N 4的3D花状N掺杂碳。图案。由于在制备甲酰胺衍生的二元ZnFe-NC(f-ZnFe-NC)中引入了2,1,3-苯并噻二唑(Bz)作为额外的配体,因此负载了约两倍的原子铁(6.84 wt%)。同时,随着Bz的促进,f-ZnFe-NC前体也显示出改进的3D花结构,经过高温处理后可以牢固地遗传为花状Fe-NC产品的形成,从而获得丰富的开放孔,用于暴露更多的原子铁位点(位点密度为26.6 umol g -1,频率转换为1.73 s -1),用于氧还原电催化。电化学测量表明,Bz促进了合成Fe-NC(简称Bz-Fe 1-NC)具有较高的起始电势(1.04 V)和半波电势(0.94 V),并且其组装好的Al-air电池可提供238.2 mW cm -2的非常大的比功率,并具有高倍率性能和良好的长续航能力。长期稳定性。

更新日期:2021-05-25
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