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Developing high-power Li||S batteries via transition metal/carbon nanocomposite electrocatalyst engineering

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dc.contributor.authorLi, H.
dc.contributor.authorMeng, R.
dc.contributor.authorYe, C.
dc.contributor.authorTadich, A.
dc.contributor.authorHua, W.
dc.contributor.authorGu, Q.
dc.contributor.authorJohannessen, B.
dc.contributor.authorChen, X.
dc.contributor.authorDavey, K.
dc.contributor.authorQiao, S.-Z.
dc.date.issued2024
dc.descriptionPublished online: 16 February 2024
dc.description.abstractThe 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.
dc.description.statementofresponsibilityHuan Li, Rongwei Meng, Chao Ye, Anton Tadich, Wuxing Hua, Qinfen Gu, Bernt Johannessen, Xiao Chen, Kenneth Davey, Shi-Zhang Qiao
dc.identifier.citationNature Nanotechnology, 2024; 19(6):792-799
dc.identifier.doi10.1038/s41565-024-01614-4
dc.identifier.issn1748-3387
dc.identifier.issn1748-3395
dc.identifier.orcidLi, H. [0000-0003-0662-6939]
dc.identifier.orcidDavey, K. [0000-0002-7623-9320]
dc.identifier.orcidQiao, S.-Z. [0000-0002-1220-1761] [0000-0002-4568-8422]
dc.identifier.urihttps://hdl.handle.net/2440/142161
dc.language.isoen
dc.publisherSpringer Nature
dc.relation.granthttp://purl.org/au-research/grants/arc/FL170100154
dc.relation.granthttp://purl.org/au-research/grants/arc/DP220102596
dc.rights© The Author(s), under exclusive licence to Springer Nature Limited 2024
dc.source.urihttp://dx.doi.org/10.1038/s41565-024-01614-4
dc.titleDeveloping high-power Li||S batteries via transition metal/carbon nanocomposite electrocatalyst engineering
dc.typeJournal article
pubs.publication-statusPublished

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