Developing high-power Li||S batteries via transition metal/carbon nanocomposite electrocatalyst engineering
Date
2024
Authors
Li, H.
Meng, R.
Ye, C.
Tadich, A.
Hua, W.
Gu, Q.
Johannessen, B.
Chen, X.
Davey, K.
Qiao, S.-Z.
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Journal article
Citation
Nature Nanotechnology, 2024; 19(6):792-799
Statement of Responsibility
Huan Li, Rongwei Meng, Chao Ye, Anton Tadich, Wuxing Hua, Qinfen Gu, Bernt Johannessen, Xiao Chen, Kenneth Davey, Shi-Zhang Qiao
Conference Name
Abstract
The activity of electrocatalysts for the sulfur reduction reaction (SRR) can be represented using volcano plots, which describe specific thermodynamic trends. However, a kinetic trend that describes the SRR at high current rates is not yet available, limiting our understanding of kinetics variations and hindering the development of high-power Li||S batteries. Here, using Le Chatelier’s principle as a guideline, we establish an SRR kinetic trend that correlates polysulfide concentrations with kinetic currents. Synchrotron X-ray adsorption spectroscopy measurements and molecular orbital computations reveal the role of orbital occupancy in transition metal-based catalysts in determining polysulfide concentrations and thus SRR kinetic predictions. Using the kinetic trend, we design a nanocomposite electrocatalyst that comprises a carbon material and CoZn clusters. When the electrocatalyst is used in a sulfur-based positive electrode (5 mg cm⁻² of S loading), the corresponding Li||S coin cell (with an electrolyte:S mass ratio of 4.8) can be cycled for 1,000 cycles at 8 C (that is, 13.4 A gS⁻¹, based on the mass of sulfur) and 25 °C. This cell demonstrates a discharge capacity retention of about 75% (final discharge capacity of 500 mAh gS⁻¹) corresponding to an initial specific power of 26,120 W kgS⁻¹ and specific energy of 1,306 Wh kgS⁻¹.
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Dissertation Note
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Published online: 16 February 2024
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© The Author(s), under exclusive licence to Springer Nature Limited 2024