Electrochemical Synthesis of Poly(trisulfides)

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dc.contributor.authorPople, J.M.M.
dc.contributor.authorNicholls, T.P.
dc.contributor.authorPham, L.N.
dc.contributor.authorBloch, W.M.
dc.contributor.authorLisboa, L.S.
dc.contributor.authorPerkins, M.V.
dc.contributor.authorGibson, C.T.
dc.contributor.authorCoote, M.L.
dc.contributor.authorJia, Z.
dc.contributor.authorChalker, J.M.
dc.date.issued2023
dc.description.abstractWith increasing interest in high sulfur content polymers, there is a need to develop new methods for their synthesis that feature improved safety and control of structure. In this report, electrochemically initiated ring-opening polymerization of norbornene-based cyclic trisulfide monomers delivered well-defined, linear poly(trisulfides), which were solution processable. Electrochemistry provided a controlled initiation step that obviates the need for hazardous chemical initiators. The high temperatures required for inverse vulcanization are also avoided resulting in an improved safety profile. Density functional theory calculations revealed a reversible "self-correcting" mechanism that ensures trisulfide linkages between monomer units. This control over sulfur rank is a new benchmark for high sulfur content polymers and creates opportunities to better understand the effects of sulfur rank on polymer properties. Thermogravimetric analysis coupled with mass spectrometry revealed the ability to recycle the polymer to the cyclic trisulfide monomer by thermal depolymerization. The featured poly(trisulfide) is an effective gold sorbent, with potential applications in mining and electronic waste recycling. A water-soluble poly(trisulfide) containing a carboxylic acid group was also produced and found to be effective in the binding and recovery of copper from aqueous media.
dc.description.statementofresponsibilityJasmine M. M. Pople, Thomas P. Nicholls, Le Nhan Pham, Witold M. Bloch, Lynn S. Lisboa, Michael V. Perkins, Christopher T. Gibson, Michelle L. Coote, Zhongfan Jia, and Justin M. Chalker
dc.identifier.citationJournal of the American Chemical Society, 2023; 145(21):11798-11810
dc.identifier.doi10.1021/jacs.3c03239
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.orcidBloch, W.M. [0000-0003-1084-1287]
dc.identifier.orcidGibson, C.T. [0000-0003-3334-5059]
dc.identifier.urihttps://hdl.handle.net/2440/138806
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.granthttp://purl.org/au-research/grants/arc/DP200100090
dc.relation.granthttp://purl.org/au-research/grants/arc/DP210100025
dc.relation.granthttp://purl.org/au-research/grants/arc/LP200301660
dc.relation.granthttp://purl.org/au-research/grants/arc/LP200301661
dc.relation.granthttp://purl.org/au-research/grants/arc/DP230100587
dc.relation.granthttp://purl.org/au-research/grants/arc/FT220100054
dc.rights© 2023 American Chemical Society
dc.source.urihttps://doi.org/10.1021/jacs.3c03239
dc.titleElectrochemical Synthesis of Poly(trisulfides)
dc.typeJournal article
pubs.publication-statusPublished

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