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Boosting Surface Reconstruction for the Oxygen Evolution Reaction: A Combined Effect of Heteroatom Incorporation and Anion Etching in Cobalt Silicate Precatalyst
Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Nanomat Res Lab, Mohanpur 741246, W Bengal, India..
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Nanomat Res Lab, Mohanpur 741246, W Bengal, India.;Uppsala Univ, Mol Biomimet, Angstrom Lab, Dept Chem, S-75120 Uppsala, Sweden..ORCID iD: 0000-0002-1209-1689
Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Nanomat Res Lab, Mohanpur 741246, W Bengal, India..
Indian Inst Sci Educ & Res IISER Kolkata, Dept Chem Sci, Nanomat Res Lab, Mohanpur 741246, W Bengal, India..
2022 (English)In: ChemElectroChem, E-ISSN 2196-0216, Vol. 9, no 5, article id e202101140Article in journal (Refereed) Published
Abstract [en]

Electrochemical water splitting is one of the most desirable techniques for combatting the global challenge of sustainable fuel generation. The generation of highly active electrocatalysts for efficient oxygen evolution reaction (OER) requires the rational design of a precatalyst that can enhance the number density of the active catalyst generated during water splitting. In this work, we report sulfurincorporated iron-doped cobalt silicate (CoFeSiO-S) nanoparticles, which exhibit a unique ability to show gradual improvement in the electrocatalytic behavior with time. The precatalyst could reach a low overpotential of 267 +/- 6 mV at benchmark current density of 10 mA/cm(2) and 300 mV at 100 mA/cm(2) current density after applying chronopotentiometry for 30 h. The exceptional OER performance is further evidence by a low Tafel slope of 37.0 +/- 0.5 mV/dec with a very high TOF value of 1.05 s(-1). This improved activity is attributed to 1) facilitation of Co2+/Co3+ by Fe doping, 2) faster catalyst activation due to lower metal-sulfur bond energy compared to metal-oxygen bond energy, 3) higher pore diameter that enables faster diffusion of reactants and products, 4) lower charge transfer resistance of sulfur incorporated iron-doped cobalt phyllosilicate than pristine, and 5) silicate anion etching in the electrolyte. This work establishes a fundamental understanding of the surface reconstruction occurring during the OER process where silicates are employed as precatalyst.

Place, publisher, year, edition, pages
John Wiley & Sons, 2022. Vol. 9, no 5, article id e202101140
Keywords [en]
oxygen evolution reaction, anion etching, silicates, surface reconstruction, cobalt
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-478298DOI: 10.1002/celc.202101140ISI: 000736074300001OAI: oai:DiVA.org:uu-478298DiVA, id: diva2:1703530
Available from: 2022-10-13 Created: 2022-10-13 Last updated: 2023-03-07Bibliographically approved

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Ganguli, Sagar

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