Publication detail

Mechanisms of Degradation of Na2Ni[Fe(CN)(6)] Functional Electrodes in Aqueous Media: A Combined Theoretical and Experimental Study

Lamprecht, X. Evazzade, I. Ungerer, I. Hromadko, L. Macak, J.M. Bandarenka, A.S. Alexandrov, V.

Original Title

Mechanisms of Degradation of Na2Ni[Fe(CN)(6)] Functional Electrodes in Aqueous Media: A Combined Theoretical and Experimental Study

Type

journal article in Web of Science

Language

English

Original Abstract

Prussian blue analogues (PBAs) are versatile functional materials with numerous applications ranging from electrocatalysis and batteries to sensors and electrochromic devices. stability strongly depends on the electrolyte composition. In this work, we use density functional theory calculations and experiments to elucidate the mechanisms of degradation of model Na2Ni[Fe(CN)(6)] functional electrodes in aqueous electrolytes. Next to the solution pH and cation concentration, we identify anion adsorption as a major driving force for electrode dissolution. Notably, the nature of adsorbed anions can control the mass and charge transfer mechanisms during metal cation intercalation as well as the electrode degradation rate. We find that weakly adsorbing anions, such as NO3-, impede the degradation, while strongly adsorbing anions, such as SO42-, accelerate it. The results of this study provide practical guidelines for electrolyte optimization and can likely be extrapolated to the whole family of PBAs operating in aqueous media.

Keywords

PRUSSIAN BLUE ANALOGS; GENERALIZED GRADIENT APPROXIMATION; TOTAL-ENERGY CALCULATIONS; THIN-FILMS; INTERCALATION; ELECTROCHEMISTRY; STABILITY; SODIUM; XPS

Authors

Lamprecht, X.; Evazzade, I.; Ungerer, I.; Hromadko, L.; Macak, J.M.; Bandarenka, A.S.; Alexandrov, V.

Released

9. 2. 2023

Publisher

American Chemical Society

Location

WASHINGTON

ISBN

1932-7455

Periodical

Journal of Physical Chemistry C (web)

Year of study

127

Number

5

State

United States of America

Pages from

2204

Pages to

2214

Pages count

11

URL

https://pubs.acs.org/doi/full/10.1021/acs.jpcc.2c08222

BibTex

@article{BUT183969,
  author="Lamprecht, X. and Evazzade, I. and Ungerer, I. and Hromadko, L. and Macak, J.M. and Bandarenka, A.S. and Alexandrov, V.",
  title="Mechanisms of Degradation of Na2Ni[Fe(CN)(6)] Functional Electrodes in Aqueous Media: A Combined Theoretical and Experimental Study",
  journal="Journal of Physical Chemistry C (web)",
  year="2023",
  volume="127",
  number="5",
  pages="2204--2214",
  doi="10.1021/acs.jpcc.2c08222",
  issn="1932-7455",
  url="https://pubs.acs.org/doi/full/10.1021/acs.jpcc.2c08222"
}