催化作用
电催化剂
X射线光电子能谱
质子交换膜燃料电池
碳纤维
X射线吸收光谱法
无机化学
过渡金属
化学
氧气
材料科学
吸收光谱法
物理化学
电化学
化学工程
电极
有机化学
复合材料
工程类
物理
复合数
量子力学
作者
Xiudong Shi,Zonghua Pu,Bin Chi,Siyan Yu,Jingsong Hu,Shuhui Sun,Shijun Liao
出处
期刊:Small
[Wiley]
日期:2023-11-09
卷期号:20 (12)
被引量:2
标识
DOI:10.1002/smll.202307011
摘要
Abstract It is crucial to rationally design and synthesize atomic‐scale transition metal‐doped carbon catalysts with high electrocatalytic activity to achieve a high‐efficient oxygen reduction reaction (ORR). Herein, an electrocatalyst comprised of Fe–Fe dual atom pairs and N‐doped concave carbon are reported (N‐CC@Fe DA) that achieves ultrahigh electrocatalytic ORR activity. The catalyst is prepared by a gaseous doping approach, with zeolitic imidazolate framework‐8 (ZIF‐8) as the carbon framework precursor and cyclopentadienyliron dicarbonyl dimer as the Fe–Fe atom pair precursor. The catalyst exhibits high cathodic ORR catalytic performance in an alkaline Zn/air battery and proton exchange membrane fuel cell (PEMFC), yielding peak power densities of 241 mW cm −2 and 724 mW cm −2 , respectively, compared to 127 mW cm −2 and 1.20 W cm −2 with conventional Pt/C catalysts as cathodes. The presence of Fe atom pairs coordinate with N atoms is revealed by X‐ray photoelectron spectroscopy (XPS) and X‐ray absorption spectroscopy (XAS) analysis, and Density Functional Theory (DFT) calculation results show that the Fe–Fe pair structure is beneficial for adsorbing oxygen molecules, activating the O─O bond, and desorbing OH * intermediates formed during oxygen reduction, resulting in a more efficient oxygen reaction. The findings may provide a new pathway for preparing ultra‐high‐performance doped carbon catalysts with Fe–Fe atom pair structures.
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