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MOF-derived three-dimensional ordered porous carbon nanomaterial for efficient alkaline zinc-air batteries

金属有机框架衍生的三维有序多孔碳纳米材料用于高效碱性锌空气电池

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Abstract

The design and preparation of non-noble metal catalysts with high catalytic activity and robust stability are important in the research of metal-air batteries and fuel cells. Here, a three-dimensional (3D) hierarchically ordered porous carbon nanomaterial was conveniently synthesized with zeolite-imidazole framework (ZIF-8) carbonization using the silica-template method and carbon nanotube (CNT) growth. The addition of an iron source endows the porous mFeNC-CNT with Fe-based nanoparticles and abundant atomically dispersive Fe-Nx sites from its nitrogen-incorporated graphitic carbon matrix. As a result, the 3D porous structure reduces the charge transport resistance, and the iron and nitrogen codoped carbon exhibits excellent catalytic activity for oxygen reduction reaction (ORR) similar to that of commercial Pt/C. Meanwhile, the interwoven CNTs obtained under urea catalysis further shorten the ion and electron diffusion pathway. Experimental and theoretical analyses revealed that the optimized mFeNC-CNT has a high ORR activity with a half-wave potential of 0.908 V and a large open-circuit voltage (1.556 V) when applied on zinc-air batteries. This work provides a promising strategy for the rational design and facile synthesis of high-performing non-noble metal-based electrocatalysts for energy storage, conversion, and transport applications.

摘要

设计和制备高催化活性和高稳定性的非贵金属催化剂对金属-空气电池和燃料电池研究具有重要意义. 本文中, 我们通过二氧化硅模板法和碳纳米管(CNT)生长对金属有机框架ZIF-8进行碳化, 合成了一种分级三维有序多孔碳纳米材料. 进一步通过添加铁源, 高温热解获得的多孔mFeNC-CNT具有精细的Fe基纳米颗粒以及原子分散Fe-Nx位点. 三维多孔结构降低了电荷传输阻力, 使得铁、 氮共掺杂碳表现出与商业Pt/C相当的氧还原反应(ORR)性能. 同时, 在尿素催化下得到的交织CNT在电化学过程中进一步缩短了离子和电子的扩散途径. 实验和理论计算结果表明, 优化后的mFeNC-CNT在锌空气电池上表现出较高的ORR活性. 综上, 这项工作为用于能量存储、 转换和传输应用的高性能非贵金属基电催化剂的合理设计和简便合成提供了一种有前景的策略.

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Acknowledgements

This work was financially supported by the Basic Science and Technology Research Project of Wenzhou, Zhejiang Province (G20190007 and ZG2017027), the BUCT-WZU Joint Fund (KH2012031), and the State Key Laboratory of Structural Chemistry, Chinese Academy of Sciences (20190008).

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Authors and Affiliations

  1. Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, China

    Qiuhong Sun  (孙秋红), Kai Zhu  (朱楷), Xiangli Ji  (季湘丽), Dandan Chen  (陈丹丹), Cheng Han  (韩承), Yue Hu  (胡悦) & Jinjie Qian  (钱金杰)

  2. Research Center of Applied Solid State Chemistry, Ningbo University, Ningbo, 315211, China

    Ting-Ting Li  (黎挺挺) & Jinjie Qian  (钱金杰)

  3. School of Materials and Energy, Guangdong University of Technology, Guangzhou, 510006, China

    Shaoming Huang  (黄少铭)

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  1. Qiuhong Sun  (孙秋红)
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  2. Kai Zhu  (朱楷)
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  3. Xiangli Ji  (季湘丽)
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  5. Cheng Han  (韩承)
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  6. Ting-Ting Li  (黎挺挺)
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  7. Yue Hu  (胡悦)
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  8. Shaoming Huang  (黄少铭)
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  9. Jinjie Qian  (钱金杰)
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Contributions

Author contributions Qian J conceived the idea and supervised the project. Zhu K and Ji X contributed to the experiments. Chen D conducted the DFT calculations. The paper was primarily written by Qian J and Sun Q. All authors contributed to the general discussion.

Corresponding author

Correspondence to Jinjie Qian  (钱金杰).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Supporting data are available in the online version of the paper.

Qiuhong Sun received her bachelor’s degree from Wenzhou University in 2020, and now she is a graduate student at Wenzhou University. Her current research focuses on the design and synthesis of MOF-derived hierarchically porous materials using silica templates for electrochemical applications.

Jinjie Qian is an associate professor at the College of Chemistry and Materials Engineering, Wenzhou University. He received his PhD degree from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS), under the supervision of CAS Academician Maochun Hong. His current research focuses on the electrochemical research on carbon nanomaterials from metal-organic frameworks for energy storage and conversion.

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Sun, Q., Zhu, K., Ji, X. et al. MOF-derived three-dimensional ordered porous carbon nanomaterial for efficient alkaline zinc-air batteries. Sci. China Mater. 65, 1453–1462 (2022). https://doi.org/10.1007/s40843-021-1933-4

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  • DOI: https://doi.org/10.1007/s40843-021-1933-4

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