Yu Ao, Peng Zhiyao, Li Yaozhou, Zhu Longtao, Peng Ping, Li Fang-Fang
State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, 1037 Luoyu Road, Wuhan 430074, P. R. China.
ACS Appl Mater Interfaces. 2022 Sep 21;14(37):42337-42346. doi: 10.1021/acsami.2c10387. Epub 2022 Sep 12.
Carbon-based materials with superior electrochemical performances have been prepared from fullerenes by releasing their intrinsic advantages such as pentagon defects and π-electron carbons. To the best of our knowledge, fullerene-derived carbon nanotubes (CNTs) and their electrochemical behavior have not been experimentally investigated. In this work, in situ growth of CNT composites from fullerene is realized via a self-catalyzed process by employing an Fe-decorated fullerene (ferrocenylpyrrolidine C) as the precursor and NH as the pyrolysis atmosphere. The results show that the in situ Fe doping in fullerene, the self-assembly of fullerene molecules, the pyrolysis temperature, and the NH flow play essential roles in the generation of CNTs. The as-prepared MN7-10/3 CNT composite exhibits efficient oxygen reduction performance with = 0.82 V and = 1.02 V vs the RHE. The flexible solid-state Zn-air battery constructed based on MN7-10/3 exhibits a superior power density (109.3 mW cm at 180.9 mA cm) and long-term durability (the voltage remains at 95.6% of the initial value after discharging for 5000 s) compared with the benchmark Pt/C catalyst. The transformation of the Fe-decorated fullerene to CNTs reveals a new function of fullerenes and demonstrates a new solid-state synthetic method for CNTs.
通过释放富勒烯的内在优势，如五边形缺陷和π电子碳，已经制备出具有优异电化学性能的碳基材料。据我们所知，尚未对富勒烯衍生的碳纳米管（CNTs）及其电化学行为进行实验研究。在这项工作中，通过使用铁修饰的富勒烯（二茂铁基吡咯烷C）作为前驱体，以NH作为热解气氛，通过自催化过程实现了从富勒烯原位生长CNT复合材料。结果表明，富勒烯中的原位铁掺杂、富勒烯分子的自组装、热解温度和NH流量在CNTs的生成中起着至关重要的作用。所制备的MN7-10/3 CNT复合材料表现出高效的氧还原性能，相对于可逆氢电极（RHE），其E1/2 = 0.82 V，Eonset = 1.02 V。与基准Pt/C催化剂相比，基于MN7-10/3构建的柔性固态锌空气电池表现出优异的功率密度（在180.9 mA cm-2时为109.3 mW cm-2）和长期耐久性（放电5000 s后电压保持在初始值的95.6%）。铁修饰的富勒烯向CNTs的转变揭示了富勒烯的一种新功能，并展示了一种用于CNTs的新型固态合成方法。
