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Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation
dc.creator | Petit, Yann K. | |
dc.creator | Mourad, Eleonore | |
dc.creator | Prehal, Christian | |
dc.creator | Leypold, Christian | |
dc.creator | Windischbacher, Andreas | |
dc.creator | Mijailović, Daniel | |
dc.creator | Slugovc, Christian | |
dc.creator | Borisov, Sergey M. | |
dc.creator | Zojer, Egbert | |
dc.creator | Brutti, Sergio | |
dc.creator | Fontaine, Olivier | |
dc.creator | Freunberger, Stefan A. | |
dc.date.accessioned | 2022-03-04T11:23:09Z | |
dc.date.available | 2022-03-04T11:23:09Z | |
dc.date.issued | 2021 | |
dc.identifier.issn | 1755-4330 | |
dc.identifier.uri | http://TechnoRep.tmf.bg.ac.rs/handle/123456789/4903 | |
dc.description.abstract | Aprotic alkali metal-O-2 batteries face two major obstacles to their chemistry occurring efficiently, the insulating nature of the formed alkali superoxides/peroxides and parasitic reactions that are caused by the highly reactive singlet oxygen (O-1(2)). Redox mediators are recognized to be key for improving rechargeability. However, it is unclear how they affect O-1(2) formation, which hinders strategies for their improvement. Here we clarify the mechanism of mediated peroxide and superoxide oxidation and thus explain how redox mediators either enhance or suppress O-1(2) formation. We show that charging commences with peroxide oxidation to a superoxide intermediate and that redox potentials above similar to 3.5 V versus Li/Li+ drive O-1(2) evolution from superoxide oxidation, while disproportionation always generates some O-1(2). We find that O-1(2) suppression requires oxidation to be faster than the generation of O-1(2) from disproportionation. Oxidation rates decrease with growing driving force following Marcus inverted-region behaviour, establishing a region of maximum rate. | en |
dc.publisher | Nature Research | |
dc.relation | European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 636069) | |
dc.relation | French National Research Agency (STORE-EX Labex Project ANR-10-LABX-76-01) | |
dc.rights | restrictedAccess | |
dc.source | Nature Chemistry | |
dc.title | Mechanism of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation | en |
dc.type | article | |
dc.rights.license | ARR | |
dc.citation.epage | 471 | |
dc.citation.issue | 5 | |
dc.citation.other | 13(5): 465-+ | |
dc.citation.rank | aM21 | |
dc.citation.spage | 465 | |
dc.citation.volume | 13 | |
dc.identifier.doi | 10.1038/s41557-021-00643-z | |
dc.identifier.pmid | 33723377 | |
dc.identifier.scopus | 2-s2.0-85102822983 | |
dc.identifier.wos | 000629296400001 | |
dc.type.version | publishedVersion |