N, O-diatomic dopants activate catalytic activity of 3D self-standing graphene carbon aerogel for long-cycle and high-efficiency Li-CO2 batteries

气凝胶 石墨烯 催化作用 掺杂剂 材料科学 碳纤维 杂原子 纳米技术 化学工程 兴奋剂 化学 有机化学 复合材料 光电子学 复合数 工程类 戒指(化学)
作者
Wei Yu,Limin Liu,Yuxiao Yang,Na Li,Yuzhi Chen,Xiangkai Yin,Jinpen Niu,Jiuhong Wang,Shujiang Ding
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:465: 142787-142787 被引量:10
标识
DOI:10.1016/j.cej.2023.142787
摘要

Carbon-based metal-free materials are regarded as viable cathode catalysts for Li-CO2 batteries due to their low costs and lightweight. And heteroatom doping (such as N atom) has great potential to improve the catalytic activity of carbon-based catalysts. However, the underlying catalytic mechanism is yet unclear, which hinders the construction of high-efficiency catalysts and further improvements in electrochemical performance. Especially, the role of oxygen-containing groups prevalent in carbon-based catalysts has never been explored. In this work, guided by theoretical simulation, a self-standing N-doped graphene carbon aerogel with certain oxygenic groups was well-designed and synthesized by a straightforward, one-step thermal approach as the cathode catalyst. N dopant can effectively regulate the electronic structure of graphene and thus lower the free energy change of reactants/intermediate species. The intrinsic oxygen-containing functional groups still presented in graphene aerogel can further stabilize CO2-related intermediate species and improve the catalytic activity through a synergistic coupling effect with N dopant. This effect was originally discovered and clarified in the Li-CO2 battery system. Additionally, intriguing 3D hierarchical pores of as-obtained graphene carbon aerogel not only guarantee good conductivity but also offer a vast surface area to expose numerous accessible active sites. The resulting Li-CO2 batteries showed a significantly enhanced initial energy efficiency of approximately 78.46% and remarkable cyclic stability of more than 1500 h at 20 μA cm−2. This fundamental understanding of the structure-performance relationship gives new ideas for creating extremely effective carbon-based metal-free catalysts for Li-CO2 batteries.
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