Design and Synthesis of Ir/Ru Pyrochlore Catalysts for the Oxygen Evolution Reaction Based on Their Bulk Thermodynamic Properties

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F19%3A00517197" target="_blank" >RIV/61388955:_____/19:00517197 - isvavai.cz</a>

Výsledek na webu

<a href="http://hdl.handle.net/11104/0302487" target="_blank" >http://hdl.handle.net/11104/0302487</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acsami.9b13220" target="_blank" >10.1021/acsami.9b13220</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Design and Synthesis of Ir/Ru Pyrochlore Catalysts for the Oxygen Evolution Reaction Based on Their Bulk Thermodynamic Properties

Popis výsledku v původním jazyce

Density functional theory (DFT) has proven to be an invaluable and effective tool for identifying highly active electrocatalysts for the oxygen evolution reaction (OER). Herein, we take a computational approach to first identify a series of rare-earth pyrochlore oxides based on Ir and Ru as potential OER catalysts. The DFT-based phase diagrams, Pourbaix diagrams (E vs pH), projected density of states, and band energy diagrams were used to identify prospective OER catalysts based on rare-earth Ir and Ru pyrochlores. The predicted materials were synthesized using the spray-freeze freeze-drying approach to afford nanoparticulate oxides conforming to the pyrochlore structural type A(2)B(2)O(7) where A = Nd, Gd, or Yb and B = Ir or Ru. In agreement with the computed Pourbaix diagrams, the materials were found to be moderately stable under OER conditions. All prepared materials show higher stability as compared to the benchmark IrO2 catalyst, and the OER mass activity of Yb2Ir2O7 and the ruthenate pyrochlores (Nd2Ru2O7, Gd2Ru2O7, and Yb2Ru2O7) were also found to exceed those of the benchmark IrO2 catalyst. We find that the OER activity of each pyrochlore series (i.e., iridate or ruthenate) generally improves as the size of the A-site cation decreases, indicating that maintaining control over the structure can be used to influence the electrocatalytic properties.

Název v anglickém jazyce

Design and Synthesis of Ir/Ru Pyrochlore Catalysts for the Oxygen Evolution Reaction Based on Their Bulk Thermodynamic Properties

Popis výsledku anglicky

Density functional theory (DFT) has proven to be an invaluable and effective tool for identifying highly active electrocatalysts for the oxygen evolution reaction (OER). Herein, we take a computational approach to first identify a series of rare-earth pyrochlore oxides based on Ir and Ru as potential OER catalysts. The DFT-based phase diagrams, Pourbaix diagrams (E vs pH), projected density of states, and band energy diagrams were used to identify prospective OER catalysts based on rare-earth Ir and Ru pyrochlores. The predicted materials were synthesized using the spray-freeze freeze-drying approach to afford nanoparticulate oxides conforming to the pyrochlore structural type A(2)B(2)O(7) where A = Nd, Gd, or Yb and B = Ir or Ru. In agreement with the computed Pourbaix diagrams, the materials were found to be moderately stable under OER conditions. All prepared materials show higher stability as compared to the benchmark IrO2 catalyst, and the OER mass activity of Yb2Ir2O7 and the ruthenate pyrochlores (Nd2Ru2O7, Gd2Ru2O7, and Yb2Ru2O7) were also found to exceed those of the benchmark IrO2 catalyst. We find that the OER activity of each pyrochlore series (i.e., iridate or ruthenate) generally improves as the size of the A-site cation decreases, indicating that maintaining control over the structure can be used to influence the electrocatalytic properties.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10405 - Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis)

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2019

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ACS Applied Materials and Interfaces

ISSN

1944-8244

e-ISSN

—

Svazek periodika

11

Číslo periodika v rámci svazku

41

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

13

Strana od-do

37748-37760

Kód UT WoS článku

000491219700037

EID výsledku v databázi Scopus

2-s2.0-85073160623