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Journal ArticleDOI

On the Lattice Oxygen Evolution Mechanism: Avoiding Pitfalls

07 Oct 2021-Chemcatchem (John Wiley & Sons, Ltd)-Vol. 13, Iss: 19, pp 4066-4074
About: This article is published in Chemcatchem.The article was published on 2021-10-07 and is currently open access. It has received 15 citations till now. The article focuses on the topics: Oxygen evolution.
Citations
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Journal ArticleDOI
TL;DR: In this paper , the authors summarized the construction strategies of high valence metals as dopants or formed heterostructures with the iron/cobalt/nickel (Fe/Co/Ni)-based catalysts.

35 citations

Journal ArticleDOI
TL;DR: In this paper , a series of B-site mixed, Ruddlesden-Popper phase of Sr2(RuxIr1−x)O4 was examined for oxygen evolution reaction (OER) in acidic media.

13 citations

Journal ArticleDOI
TL;DR: In this paper , overpotential and kinetic effects are factored into the volcano plot for the selective nitrogen reduction (NRR) over transition-metal oxides by making use of the recently introduced activity descriptor Gmax(η).

11 citations

Journal ArticleDOI
TL;DR: In this paper , a data-driven methodology is used to understand bifunctional oxygen electrocatalysis and demonstate that electrocatalysts for the oxygen evolution and oxygen reduction reactions haven't exhausted their full potential.
Abstract: Comprehending bifunctional oxygen electrocatalysis: using a data-driven methodology, we demonstate that electrocatalysts for the oxygen evolution and oxygen reduction reactions haven't exhausted their full potential yet.

9 citations

Journal ArticleDOI
TL;DR: In this article, the authors investigated the energy and structural properties of cation substitutional doping (TM-X) and anion anion doping (F and S), as well as a cation-anion dopant complexes incorporated in an IrO2 (110) surface slab.

9 citations

References
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Journal ArticleDOI
TL;DR: In this paper, the authors report a protocol for evaluating the activity, stability, and Faradaic efficiency of electrodeposited oxygen-evolving electrocatalysts for water oxidation.
Abstract: Objective evaluation of the activity of electrocatalysts for water oxidation is of fundamental importance for the development of promising energy conversion technologies including integrated solar water-splitting devices, water electrolyzers, and Li-air batteries. However, current methods employed to evaluate oxygen-evolving catalysts are not standardized, making it difficult to compare the activity and stability of these materials. We report a protocol for evaluating the activity, stability, and Faradaic efficiency of electrodeposited oxygen-evolving electrocatalysts. In particular, we focus on methods for determining electrochemically active surface area and measuring electrocatalytic activity and stability under conditions relevant to an integrated solar water-splitting device. Our primary figure of merit is the overpotential required to achieve a current density of 10 mA cm–2 per geometric area, approximately the current density expected for a 10% efficient solar-to-fuels conversion device. Utilizing ...

4,808 citations

Journal ArticleDOI
TL;DR: In this article, a large database of HO* and HOO* adsorption energies on oxide surfaces was used to analyze the reaction free energy diagrams of all the oxides in a general way.
Abstract: Trends in electrocatalytic activity of the oxygen evolution reaction (OER) are investigated on the basis of a large database of HO* and HOO* adsorption energies on oxide surfaces. The theoretical overpotential was calculated by applying standard density functional theory in combination with the computational standard hydrogen electrode (SHE) model. We showed that by the discovery of a universal scaling relation between the adsorption energies of HOO* vs HO*, it is possible to analyze the reaction free energy diagrams of all the oxides in a general way. This gave rise to an activity volcano that was the same for a wide variety of oxide catalyst materials and a universal descriptor for the oxygen evolution activity, which suggests a fundamental limitation on the maximum oxygen evolution activity of planar oxide catalysts.

2,923 citations

Journal ArticleDOI
TL;DR: This Account introduces the energetic span model that enables one to evaluate TOFs in a straightforward manner and in affinity with the Curtin-Hammett principle, and concludes that a change in the conceptualization of catalytic cycles is in order.
Abstract: A computational study of a catalytic cycle generates state energies (the E-representation), whereas experiments lead to rate constants (the k-representation). Based on transition state theory (TST), these are equivalent representations. Nevertheless, until recently, there has been no simple way to calculate the efficiency of a catalytic cycle, that is, its turnover frequency (TOF), from a theoretically obtained energy profile. In this Account, we introduce the energetic span model that enables one to evaluate TOFs in a straightforward manner and in affinity with the Curtin−Hammett principle. As shown herein, the model implies a change in our kinetic concepts.Analogous to Ohm’s law, the catalytic chemical current (the TOF) can be defined by a chemical potential (independent of the mechanism) divided by a chemical resistance (dependent on the mechanism and the nature of the catalyst). This formulation is based on Eyring’s TST and corresponds to a steady-state regime.In many catalytic cycles, only one transi...

1,217 citations

Journal ArticleDOI
TL;DR: This article summarized the recent progress in understanding OER mechanisms, which include the conventional adsorbate evolution mechanism (AEM) and lattice-oxygen-mediated mechanism (LOM) from both theoretical and experimental aspects, and introduced strategies to reduce overpotential.
Abstract: Electricity-driven water splitting can facilitate the storage of electrical energy in the form of hydrogen gas. As a half-reaction of electricity-driven water splitting, the oxygen evolution reaction (OER) is the major bottleneck due to the sluggish kinetics of this four-electron transfer reaction. Developing low-cost and robust OER catalysts is critical to solving this efficiency problem in water splitting. The catalyst design has to be built based on the fundamental understanding of the OER mechanism and the origin of the reaction overpotential. In this article, we summarize the recent progress in understanding OER mechanisms, which include the conventional adsorbate evolution mechanism (AEM) and lattice-oxygen-mediated mechanism (LOM) from both theoretical and experimental aspects. We start with the discussion on the AEM and its linked scaling relations among various reaction intermediates. The strategies to reduce overpotential based on the AEM and its derived descriptors are then introduced. To further reduce the OER overpotential, it is necessary to break the scaling relation of HOO* and HO* intermediates in conventional AEM to go beyond the activity limitation of the volcano relationship. Strategies such as stabilization of HOO*, proton acceptor functionality, and switching the OER pathway to LOM are discussed. The remaining questions on the OER and related perspectives are also presented at the end.

1,107 citations

Journal ArticleDOI
TL;DR: In this paper, the authors evaluated the stability and activity of iridium and ruthenium thin film electrodes in acidic and alkaline electrolytes using an electrochemical scanning flow cell (SFC) connected to an inductively coupled plasma mass spectrometer (ICP-MS).

884 citations