Abstract
Rechargeable Li-O2 batteries have attracted considerable interests because of their exceptional energy density. However, the short lifetime still remained as one of the bottle-neck obstacles for the practical application of rechargeable Li-O2 batteries. The development of efficient cathode catalyst is highly desirable to reduce the energy barrier of Li-O2 reaction and electrode failure. In this work, we report a facile strategy for the fabrication of a high-performance cathode catalyst for rechargeable Li-O2 batteries by the encapsulation of high content of active Fe nanorods into N-doped carbon nanotubes with high stability (denoted as Fe@NCNTs). First-principles calculations reveal that the synergistic charge transfer and redistribution between the interface of Fe nanorods, the CNT walls and the active N dopants greatly facilitate the chemisorption and subsequent dissociation of O2 molecules into the epoxy intermediates on the carbon surface, which benefits the uniform growth of nanosized discharge products on CNT surface and thus boosts the reversibility of Li-O2 reactions. As a result, the cathode with Fe@NCNT catalyst exhibits long cycling stability with high capacities (1000 mA h g−1 for 160 cycles and 600 mA h g−1 for 270 cycles). Based on the total mass of Fe@NCNTs + Li2O2, high gravimetric energy densities of 2120–2600 W h kg−1 can be achieved at the power densities of 50–795 W kg−1.
摘要
锂-空气二次电池是当前能量密度最高的二次电池体系之一, 高效阴极催化剂的创制构筑是构筑高性能锂-空气电池的关键技术之一. 本文基于简便易行的全固相热解反应, 设计构筑了一种具有纳米电缆结构的新型铁-碳纳米管电化学催化剂. 第一性原理计算表明碳纳米 管与其内部包覆的铁纳米棒之间的电荷迁移与协同分布效应可有效促进氧气在碳纳米管表面的化学吸附与转化. 得益于此, 基于其的锂- 空气电池在限制比容量为600 mA h g−1时, 循环寿命可达270次, 基于此催化剂与固态放电产物(Li2O2)总质量的电极比能量可达2120–2600 W h kg−1. 本研究为锂-空气二次电池用高性能阴极催化剂的开发提供了有效途径.
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Acknowledgments
This work was supported by the National Natural Science Foundation of China (NSFC, 51522203), Fok Ying Tung Education Foundation (151047), the Recruitment Program of Global Youth Experts (2014) and Xinghai Scholarship of Dalian University of Technology. Wang Z and Zhou T also acknowledge the support by the Opening Project of State Key Lab of Polymer Materials Engineering, China (Sklpme2015-4-25).
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Mengzhou Yu received her MSc degree from Dalian University of Technology (DUT) in 2016. Currently, she is a PhD candidate at the School of Chemical Engineering in DUT. Her research mainly focuses on the development of high-performance electrocatalysts for oxygen reduction/evolution reactions.
Si Zhou received her PhD degree from the School of Physics at Georgia Institute of Technology in 2014. She is currently an associate professor at DUT. Her research interests focus on computational design of advanced materials for electronics and energy storage and conversion devices.
Zhiyu Wang received his PhD degree fromthe School of Chemical Engineering at DUT in China. Currently he is a professor of the School of Chemical Engineering in DUT. His research focuses on the design and synthesis of functional hybrid nanomaterials for energy storage/conversion applications. Jieshan
Jieshan Qiu received his PhD degree from the School of Chemical Engineering at DUT in China. He was appointed to a Cheung-Kong Distinguished Professor in 2009. He is a professor of the School of Chemical Engineering and director of the Carbon Research Laboratory at DUT. His research focuses on the development of new methodologies for the synthesis of functional carbon materials, as well as their applications in catalysis, energy conversion/storage and environment protection.
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Long life rechargeable Li-O2 batteries enabled by enhanced charge transfer in nanocable-like Fe@N-doped carbon nanotube catalyst
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Yu, M., Zhou, S., Liu, Y. et al. Long life rechargeable Li-O2 batteries enabled by enhanced charge transfer in nanocable-like Fe@N-doped carbon nanotube catalyst. Sci. China Mater. 60, 415–426 (2017). https://doi.org/10.1007/s40843-017-9021-6
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DOI: https://doi.org/10.1007/s40843-017-9021-6