Journal
ACS NANO
Volume 15, Issue 9, Pages 14105-14115Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c04642
Keywords
single-atomic Co-N-x; Li-S batteries; dual-functional; polysulfide conversion; dendrite inhibition
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Funding
- National Natural Science Foundation of China [52073177]
- National Key Research and Development Program of China [2019YFA0708201]
- Key Project of Department of Education of Guangdong Province [2020KTSCX118]
- Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Suzhou, China
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A dual-functional fibrous skeleton implanted with single-atom Co-N-x dispersion is designed to regulate both electrodes of lithium-sulfur batteries. By converting the fibrous carbon skeleton from lithiophobic to lithiophilic and optimizing the electrocatalytic activity of the Co-N-x species, the integrated batteries demonstrate improved performance in terms of dendritic formation and electrochemical conversion kinetics of sulfur.
Although lithium-sulfur (Li-S) batteries have long been touted as next-generation energy storage devices, the rampant dendrite growth at the anode side and sluggish redox kinetics at the cathode side drastically impede their practical application. Herein, a dual-functional fibrous skeleton implanted with single-atom Co-N-x\ dispersion is devised as an advanced modificator to realize concurrent regulation of both electrodes. The rational integration of single-atomic Co-N-x sites could convert the fibrous carbon skeleton from lithiophobic to lithiophilic, helping assuage the dendritic formation for the Li anode. Meanwhile, the favorable electrocatalytic activity from the Co-N-x species affording a lightweight feature effectively enables expedited bidirectional conversion kinetics of sulfur electrochemistry, thereby inhibiting the polysulfide shuttle. Moreover, the interconnected porous framework endows the entire skeleton with good mechanical robustness and fast electron/ion transportation. Benefiting from the synergistic effects between atomically dispersed Co-Nx sites and three-dimensional conductive networks, the integrated Li-S full batteries can achieve a reversible areal capacity (>7.0 mAh cm(-2)) at a sulfur loading of 6.9 mg cm(-2). This work might be beneficial to the development of practically viable Li-S batteries harnessing single-atom mediators.
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