Prussian Blue-Derived Atomic Fe/Fe3C@N-Doped C Catalysts Supported by Carbon Cloth as Integrated Air Cathode for Flexible Zn-Air Batteries.

IF 14.3 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zihan Wang, Jing Ren, Guoqiang Ling, Junjie Guo, Yongkang Lv, Rui-Peng Ren
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Abstract

The development of an integrated air cathode with superior oxygen reduction reaction (ORR) performance is fundamental to flexible zinc-air batteries (ZABs) for wearable electronics. Herein, a self-assembled metal-organic framework (MOF)-derived strategy is proposed to prepare a atomic Fe/Fe3C@N-doped C catalysts supported by carbon cloth (CC) catalyst for use as an air cathode of flexible ZABs. The Prussian Blue precursor, which self-assembles on the surface of the carbon cloth due to electrostatic attraction, is critical in achieving the uniform dispersion of catalysts with high density loading on carbon cloth substrates. The hollow cubic structure, N-doped carbon layer coating, and the integrated electrode design can provide more accessible active sites and facilitate a rapid electron transfer and mass transport. Density functional theory (DFT) calculation reveals that the electronic interactions between the Fe-N4 and Fe3C dual active sites can optimize the adsorption-desorption behavior of oxygen intermediates formed during the ORR. Consequently, the Fe/Fe3C@N-doped C/CC exhibits an excellent half wave potential (E1/2 = 0.903 V) and superior long-term cycling stability in alkaline environments. With excellent ORR performance, ZABs and flexible ZABs based on Fe/Fe3C@N-doped C/CC air cathode demonstrate excellent overall electrochemical performance in terms of open circuit voltage, maximum power density, flexibility, and cycling stability.

碳布支撑的普鲁士蓝衍生原子铁/Fe3C@N-掺杂 C 催化剂作为柔性锌-空气电池的集成空气阴极
开发具有优异氧还原反应(ORR)性能的集成空气阴极是柔性锌-空气电池(ZAB)用于可穿戴电子设备的基础。本文提出了一种自组装金属有机框架(MOF)衍生策略,以制备由碳布(CC)催化剂支持的原子铁/Fe3C@N掺杂C催化剂,用作柔性锌空气电池的空气阴极。普鲁士蓝前驱体由于静电吸引而在碳布表面自组装,这对于在碳布基底上实现高密度负载的催化剂的均匀分散至关重要。中空立方结构、掺杂 N 的碳层涂层和一体化电极设计可以提供更多可访问的活性位点,促进电子转移和质量传输的快速进行。密度泛函理论(DFT)计算表明,Fe-N4 和 Fe3C 双活性位点之间的电子相互作用可以优化 ORR 过程中形成的氧中间产物的吸附-解吸行为。因此,Fe/Fe3C@N 掺杂的 C/CC 具有出色的半波电位(E1/2 = 0.903 V)和在碱性环境中长期循环的稳定性。由于具有出色的 ORR 性能,基于掺杂 Fe/Fe3C@N 的 C/CC 空气阴极的 ZAB 和柔性 ZAB 在开路电压、最大功率密度、柔性和循环稳定性方面都表现出了出色的整体电化学性能。
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来源期刊
Advanced Science
Advanced Science CHEMISTRY, MULTIDISCIPLINARYNANOSCIENCE &-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
18.90
自引率
2.60%
发文量
1602
审稿时长
1.9 months
期刊介绍: Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.
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