Xi Zeyu, Han Jiuhui, Jin Zeyu, Hu Kailong, Qiu Hua-Jun, Ito Yoshikazu
Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, 305-8573, Japan.
Tianjin Key Laboratory of Advanced Functional Porous Materials, Institute for New Energy Materials and Low-Carbon Technologies, Tianjin University of Technology, Tianjin, 300384, China.
Small. 2024 Feb;20(8):e2308045. doi: 10.1002/smll.202308045. Epub 2023 Oct 12.
Nitrogen (N) doping of graphene with a three-dimensional (3D) porous structure, high flexibility, and low cost exhibits potential for developing metal-air batteries to power electric/electronic devices. The optimization of N-doping into graphene and the design of interconnected and monolithic graphene-based 3D porous structures are crucial for mass/ion diffusion and the final oxygen reduction reaction (ORR)/battery performance. Aqueous-type and all-solid-state primary Mg-air batteries using N-doped nanoporous graphene as air cathodes are assembled. N-doped nanoporous graphene with 50-150 nm pores and ≈99% porosity is found to exhibit a Pt-comparable ORR performance, along with satisfactory durability in both neutral and alkaline media. Remarkably, the all-solid-state battery exhibits a peak power density of 72.1 mW cm ; this value is higher than that of a battery using Pt/carbon cathodes (54.3 mW cm ) owing to the enhanced catalytic activity induced by N-doping and rapid air breathing in the 3D porous structure. Additionally, the all-solid-state battery demonstrates better performances than the aqueous-type battery owing to slow corrosion of the Mg anode by solid electrolytes. This study sheds light on the design of free-standing and catalytically active 3D nanoporous graphene that enhances the performance of both Mg-air batteries and various carbon-neutral-technologies using neutral electrolytes.
具有三维（3D）多孔结构、高柔韧性和低成本的氮（N）掺杂石墨烯在开发用于为电气/电子设备供电的金属空气电池方面展现出潜力。优化石墨烯中的氮掺杂以及设计相互连接的整体式石墨烯基3D多孔结构对于质量/离子扩散以及最终的氧还原反应（ORR）/电池性能至关重要。使用氮掺杂纳米多孔石墨烯作为空气阴极组装了水基型和全固态一次镁空气电池。发现具有50 - 150纳米孔径和约99%孔隙率的氮掺杂纳米多孔石墨烯表现出与铂相当的ORR性能，并且在中性和碱性介质中都具有令人满意的耐久性。值得注意的是，全固态电池的峰值功率密度为72.1毫瓦/平方厘米；由于氮掺杂诱导的催化活性增强以及3D多孔结构中的快速透气，该值高于使用铂/碳阴极的电池（54.3毫瓦/平方厘米）。此外，由于固体电解质对镁阳极的腐蚀较慢，全固态电池表现出比水基型电池更好的性能。这项研究为独立且具有催化活性的3D纳米多孔石墨烯的设计提供了思路，这种石墨烯可提高镁空气电池以及使用中性电解质的各种碳中和技术的性能。
