4.6 Article

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

期刊

ACS ENERGY LETTERS
卷 5, 期 9, 页码 2979-2986

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c01767

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资金

  1. Helmholtz Association
  2. state of Baden-Wurttemberg through bwHPC
  3. German Research Foundation (DFG) [INST 40/467-1 FUGG]
  4. H2020 Programme (H2020-FETOPEN-2018-2019-2020) under, Project VIDICAT Versatile Ionomers for Divalent Calcium Batteries [828902]
  5. Ministry of Science, Research and the Arts Baden-Wurttemberg
  6. Federal Ministry of Education and Research
  7. China Scholarship Council (CSC)
  8. Basque Government

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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 delta-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 Zn2+/delta-V2O5 AZMBs. This method indicates the intercalation of both H+ and Zn2+ into delta-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 Zn and H+ during the electrochemical intercalation/release.

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