The low efficiency of the electrocatalytic oxidation of water to O2 (oxygen evolution reaction-OER) is considered as one of the major roadblocks for the storage of electricity from renewable sources in form of molecular fuels like H2 or hydrocarbons Especially in acidic environments, compatible with the powerful proton exchange membrane (PEM), an earth-abundant OER catalyst that combines high activity and high stability is still unknown Current PEM-compatible OER catalysts still rely mostly on Ir and/or Ru as active components, which are both very scarce elements of the platinum group Hence, the Ir and/or Ru amount in OER catalysts has to be strictly minimized Unfortunately, the OER mechanism, which is the most powerful tool for OER catalyst optimization, still remains unclear In this review, we first summarize the current state of our understanding of the OER mechanism on PEM-compatible heterogeneous electrocatalysts, before we compare and contrast that to the OER mechanism on homogenous catalysts Thereafter, an overview over monometallic OER catalysts is provided to obtain insights into structure-function relations followed by a review of current material optimization concepts and support materials Moreover, missing links required to complete the mechanistic picture as well as the most promising material optimization concepts are pointed out

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Electrocatalytic Oxygen Evolution Reaction in Acidic Environments – Reaction Mechanisms and Catalysts

The oxygen evolution reaction (OER) is of prime importance in multiple energy storage devices; however, deeper mechanistic understanding is required to design enhanced electrocatalysts for the reaction. Current understanding of the OER mechanism based on oxygen adsorption on a metallic surface site fails to fully explain the activity of iridium and ruthenium oxide surfaces, and the drastic surface reconstruction observed for the most active OER catalysts. Here we demonstrate, using La2LiIrO6 as a model catalyst, that the exceptionally high activity found for Ir-based catalysts arises from the formation of active surface oxygen atoms that act as electrophilic centres for water to react. Moreover, with the help of transmission electron microscopy, we observe drastic surface reconstruction and iridium migration from the bulk to the surface. Therefore, we establish a correlation between surface activity and surface stability for OER catalysts that is rooted in the formation of surface reactive oxygen.

https://hal.archives-ouvertes.fr/hal-03315781/document

Activation of surface oxygen sites on an iridium-based model catalyst for the oxygen evolution reaction

New Ir(VI) containing perovskite oxides, (ALa)LiIrO6-δ,(A ˭ Ca,Sr,Ba) were synthesized in a belt-type reaction cell, where in situ generation of high oxygen pressure was made by the thermal decomposition of KCIO3. The crystal structure and their oxygen stoichiometry depend on the A cation species (Ca, Sr, Ba) in the same preparation conditions. The long range magnetic interaction was not observed in the stoichiometric(BaLa)LiIrO6, by the magnetic susceptibility measurements. Complex paramagnetic behavior of SrLaLiIrO5.82, and CaLaLiIrO5.62 is attributed to the partial formation of pentavalent iridium (+ V) characterized by a T-ground term.

Preparation under oxygen pressures of new perovskites: (ALa)LiIrO6-δ (A = Ca, Sr, Ba)

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Preparation under oxygen pressures of new perovskites: (ALa)LiIrO6-δ (A = Ca, Sr, Ba)