Enhancement of Oxygen Evolution Activity of Ruddlesden-Popper-Type Strontium Ferrite by Stabilizing Fe4&amp;lt;sup&amp;gt;+&amp;lt;/sup&amp;gt;

An experimental setup and routine is presented for evaluating potential catalysts for water splitting by means of measuring the faradaic efficiency in real time through coupled potentiometry and mass spectrometry. The aim was to scale up an analytical cell unit towards the simulation of industrial conditions and generate results such as H 2 production versus power input at a certain potential or current density in addition to electrochemical parameters. Three types of electrodes were tested: A) planar metal electrodes; B) metal-foam-based electrodes; C) porous electrodes with carbon additive. The results verify that the experimental routine yields the desired accuracy, sensitivity, and a negligible accumulation of gaseous products in the cell; thus the faradaic efficiency is measured in real time. The metal-based electrodes of category A and B proved to be durable with low overpotentials and high gas output to power input, whereas three tested metal oxide electrodes in C revealed i) potential-dependent deviation in the faradaic efficiency, ii) phase decomposition, and iii) an optimum operational power range.

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Water Splitting Catalysis Studied by using Real‐Time Faradaic Efficiency Obtained through Coupled Electrolysis and Mass Spectrometry

Svengren

Chamoun

Grîns

et al. 2017

ChemElectroChem

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Synthesis and electrocatalytic properties of LaFe1-xZnxO3 perovskites

Omari

2020

J Sol-Gel Sci Technol

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Element strategy of oxygen evolution electrocatalysis based on in situ spectroelectrochemistry

et al. 2017

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Oxygen evolution electrocatalysis has received extensive attention due to its significance in biology, chemistry, and technology. However, it is still unclear how the abundant 3d-elements can be used to drive the four-electron oxidation of water as efficiently as in Nature. In this Feature Article, we will propose a design strategy concerning the optimization of the charge accumulation process based on our ongoing spectroelectrochemical study on Mn, Fe, and Ir oxygen evolution catalysts. Spectroscopic identification of the reaction intermediates showed that the activity of MnO and FeO was dictated by the generation of Mn and Fe, whereas in the case of IrO, the activity did not correlate with the valence change of Ir. The efficiency of charge accumulation through valence change is closely linked with the spin configuration of the metal center, because charge disproportionation, which was found to inhibit charge accumulation in the high-spin 3d metals, requires an electron in the e orbital. In addition to directly increasing the overpotential through the generation of an unstable intermediate, charge disproportionation inhibits charge accumulation by dissipating the total oxidative energy of the system. A favorable charge accumulation process may also be beneficial for electrode kinetics due to the enhanced coupling between reaction rates and electrochemical driving force. The model proposed in this study may help explain why low-spin 4d/5d rare metals are often more active than the abundant high-spin 3d materials for multi-electron transfer reactions in general, and provides new insight into how active 3d-metal catalysts can be synthesized by optimizing the energetics of both bond formation and charge accumulation.

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Enhancement of Oxygen Evolution Activity of Ruddlesden-Popper-Type Strontium Ferrite by Stabilizing Fe4<sup>+</sup>

Cited by 3 publications

References 36 publications

Water Splitting Catalysis Studied by using Real‐Time Faradaic Efficiency Obtained through Coupled Electrolysis and Mass Spectrometry

Water Splitting Catalysis Studied by using Real‐Time Faradaic Efficiency Obtained through Coupled Electrolysis and Mass Spectrometry

Synthesis and electrocatalytic properties of LaFe1-xZnxO3 perovskites

Element strategy of oxygen evolution electrocatalysis based on in situ spectroelectrochemistry

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