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Operando pH Measurements Decipher H⁺/Zn²⁺ Intercalation Chemistry in High-Performance Aqueous Zn/δ-V₂O₅ Batteries

Liu, Xu 1; Euchner, Holger; Zarrabeitia, Maider ORCID iD icon 1; Gao, Xinpei 1; Elia, Giuseppe Antonio 1; Groß, Axel 1; Passerini, Stefano 1
1 Karlsruher Institut für Technologie (KIT)

Abstract:

Vanadium oxides have been recognized to be among the most promising positive electrode materials for aqueous zinc metal batteries (AZMBs). However, their underlying intercalation mechanisms are still vigorously debated. To shed light on the intercalation mechanisms, high-performance δ-V2O5 is investigated as a model compound. Its structural and electrochemical behaviors in the designed cells with three different electrolytes, i.e., 3 m Zn(CF3SO3)2/water, 0.01 M H2SO4/water, and 1 M Zn(CF3SO3)2/acetonitrile, demonstrate that the conventional structural and elemental characterization methods cannot adequately clarify the separate roles of H+ and Zn2+ intercalations in the Zn(CF3SO3)2/water electrolyte. Thus, an operando pH determination method is developed and used toward Zn/δ-V2O5 AZMBs. This method indicates the intercalation of both H+ and Zn2+ into δ-V2O5 and uncovers an unusual H+/Zn2+-exchange intercalation–deintercalation mechanism. Density functional theory calculations further reveal that the H+/Zn2+ intercalation chemistry is a consequence of the variation of the electrochemical potential of Zn2+ and H+ during the electrochemical intercalation/release.


Verlagsausgabe §
DOI: 10.5445/IR/1000128542
Veröffentlicht am 22.08.2022
Originalveröffentlichung
DOI: 10.1021/acsenergylett.0c01767
Scopus
Zitationen: 122
Dimensions
Zitationen: 126
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 09.2020
Sprache Englisch
Identifikator ISSN: 2380-8195, 2380-8195
KITopen-ID: 1000128542
HGF-Programm 37.01.01 (POF III, LK 01) Fundamentals and Materials
Erschienen in ACS energy letters
Verlag American Chemical Society (ACS)
Band 5
Heft 9
Seiten 2979–2986
Vorab online veröffentlicht am 01.09.2020
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