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Cation insertion to break the activity/stability relationship for highly active oxygen evolution reaction catalyst.

ABSTRACT: The production of hydrogen at a large scale by the environmentally-friendly electrolysis process is currently hampered by the slow kinetics of the oxygen evolution reaction (OER). We report a solid electrocatalyst α-Li₂IrO₃ which upon oxidation/delithiation chemically reacts with water to form a hydrated birnessite phase, the OER activity of which is five times greater than its non-reacted counterpart. This reaction enlists a bulk redox process during which hydrated potassium ions from the alkaline electrolyte are inserted into the structure while water is oxidized and oxygen evolved. This singular charge balance process for which the electrocatalyst is solid but the reaction is homogeneous in nature allows stabilizing the surface of the catalyst while ensuring stable OER performances, thus breaking the activity/stability tradeoff normally encountered for OER catalysts.

SUBMITTER: Yang C

PROVIDER: S-EPMC7069983 | biostudies-literature | 2020 Mar

REPOSITORIES: biostudies-literature

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Cation insertion to break the activity/stability relationship for highly active oxygen evolution reaction catalyst.

Yang Chunzhen C Rousse Gwenaëlle G Louise Svane Katrine K Pearce Paul E PE Abakumov Artem M AM Deschamps Michael M Cibin Giannantonio G Chadwick Alan V AV Dalla Corte Daniel Alves DA Anton Hansen Heine H Vegge Tejs T Tarascon Jean-Marie JM Grimaud Alexis A

Nature communications 20200313 1

The production of hydrogen at a large scale by the environmentally-friendly electrolysis process is currently hampered by the slow kinetics of the oxygen evolution reaction (OER). We report a solid electrocatalyst α-Li<sub>2</sub>IrO<sub>3</sub> which upon oxidation/delithiation chemically reacts with water to form a hydrated birnessite phase, the OER activity of which is five times greater than its non-reacted counterpart. This reaction enlists a bulk redox process during which hydrated potassi ...[more]

PMID: 32170137

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Project description:Polymer electrolyte membrane fuel cells (PEMFCs) have reached the commercialization phase, representing a promising approach to curbing carbon emissions. However, greater durability of PEMFCs is of paramount importance to ensure their long-term viability and effectiveness, and catalyst development has become a focal point of research. Pt nanoparticles supported on carbon materials (Pt/C) are the primary catalysts used in PEMFCs. Accomplishing both a high dispersion of uniform metal particles on the carbon support and robust adhesion between the metal particles and the carbon support is imperative for superior stability, and will thereby, advance the practical applications of PEMFCs in sustainable energy solutions. Ultrasound-assisted polyol synthesis (UPS) has emerged as a suitable method for synthesizing catalysts with a well-defined metal-support structure, characterized by the high dispersion and uniformity of metal nanoparticles. In this study, we focused on the effect of ultrasound on the synthesis of Pt/C via UPS and the resulting enhanced stability of Pt/C catalysts. Therefore, we compared Pt/C synthesized using a conventional polyol synthesis (Pt/C_P) and Pt/C synthesized via UPS (Pt/C_U) under similar synthesis conditions. The two catalysts had a similar Pt content and the average particle size of the Pt nanoparticles was similar; however, the uniformity and dispersion of Pt nanoparticles in Pt/C_U were better than those of Pt/C_P. Moreover, ex/in-situ analyses performed in a high-temperature environment, in which nanoparticles tend to agglomerate, have revealed that Pt/C_U exhibited a notable improvement in the adhesion of Pt particles to the carbon support compared with that of Pt/C_P. The enhanced adhesion is crucial for maintaining the stability of the catalyst, ultimately contributing to a better durability in practical applications. Ultrasound was applied to the carbon support without the Pt precursor under the same UPS conditions used to synthesize Pt/C_U to identify the reason for the increased adhesion between the Pt particles and the carbon support in Pt/C_U, and we discovered that oxygen functional groups (C-O, C = O, and O-C = O) for anchoring site of Pt particles were generated in the carbon support. Pt/C_U displayed an increase in stability in an electrochemical accelerated stress test (AST) in an acidic electrolyte. The physical and chemical effects of ultrasound on the synthesis of Pt/C via UPS were identified, and we concluded that UPS is suitable for synthesizing carbon supported electrocatalysts with high stability.

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Cation insertion to break the activity/stability relationship for highly active oxygen evolution reaction catalyst.

Publications

Cation insertion to break the activity/stability relationship for highly active oxygen evolution reaction catalyst.

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