4.7 Article

A highly efficient and free-standing copper single atoms anchored nitrogen-doped carbon nanofiber cathode toward reliable Li-CO2 batteries

Journal

MATERIALS TODAY ENERGY
Volume 25, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.mtener.2022.100967

Keywords

Cu-N-4 sites; Free-standing air cathode; Reversible Li-CO2 batteries; Long-life stability

Funding

  1. Natural Science Foundation of Jiangsu Province [BK20210616, BK20190413]
  2. National Natural Science Foundation of China [51602153]
  3. National Defense Technology Innovation Special Zone Spark Project [2016300TS00911901]
  4. China Postdoctoral Science Foundation [2019M661825]
  5. Jiangsu Key Laboratory of Electrochemical Energy-Storage Technologies [EEST2021-2]
  6. Funding of Research and Practice Innovation Program in NUAA [xcxjh20210605]
  7. Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)

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In this study, copper single atoms doped nitrogen-containing carbon nanofibers were developed as free-standing cathodes for Li-CO2 batteries. The electrochemical performances showed high specific capacity, low polarization, and long life stability of the Cu/NCNF material. The uniformly dispersed Cu-N-4 catalytic active centers promoted the adsorption and activation of CO2, as well as the decomposition of discharge products.
In recent years, lithium-carbon dioxide (Li-CO2) batteries have received extensive attention due to their high energy density and environmental friendliness. However, the high charging voltage makes it difficult to withstand a large current density, resulting in the low energy efficiency. Herein, nitrogendoped carbon nanofibers with copper single atoms (Cu/NCNF) were developed as free-standing cathodes for Li-CO2 batteries. The Cu/NCNF sample was prepared by electrospinning and two-step heat treatment along with a meteorological deposition method. The electrochemical performances show that the Li-CO2 battery with Cu/NCNF possesses a high specific capacity (14084 mAh/g at a current density of 100 mAh/g), a low polarization of 1.29 V, and a long-life stability of 133 cycles. We believe that the highly spatialized structure of the Cu/NCNF sample can provide considerable storage space for discharge products. The X-ray absorption fine structure spectroscopy further proves the existence of a Cu-N-4 catalytic active center, and the uniformly dispersed Cu-N-4 sites had a positive effect on the adsorption and activation of CO2 and could also promote the decomposition of discharge products as the reactive active site.

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