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ACS Publications. Most Trusted. Most Cited. Most Read
Oxygen Reduction Electrocatalysis with Epitaxially Grown Spinel MnFe2O4 and Fe3O4

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Catal. 2022, 12, 6, 3577-3588
    Research Article

    Oxygen Reduction Electrocatalysis with Epitaxially Grown Spinel MnFe2O4 and Fe3O4
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    ACS Catalysis

    Cite this: ACS Catal. 2022, 12, 6, 3577–3588
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    https://doi.org/10.1021/acscatal.1c05172
    Published March 7, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Nanocrystalline MnFe2O4 has shown promise as a catalyst for the oxygen reduction reaction (ORR) in alkaline solutions, but the material has been sparingly studied as highly ordered thin-film catalysts. To examine the role of surface termination and Mn and Fe site occupancy, epitaxial MnFe2O4 and Fe3O4 spinel oxide films were grown on (001)- and (111)-oriented Nb:SrTiO3 perovskite substrates using molecular beam epitaxy and studied as electrocatalysts for the oxygen reduction reaction (ORR). High-resolution X-ray diffraction (HRXRD) and X-ray photoelectron spectroscopy (XPS) show the synthesis of pure phase materials, while scanning transmission electron microscopy (STEM) and reflection high-energy electron diffraction (RHEED) analysis demonstrate island-like growth of (111) surface-terminated pyramids on both (001)- and (111)-oriented substrates, consistent with the literature and attributed to the lattice mismatch between the spinel films and the perovskite substrate. Cyclic voltammograms under a N2 atmosphere revealed distinct redox features for Mn and Fe surface termination based on comparison of MnFe2O4 and Fe3O4. Under an O2 atmosphere, electrocatalytic reduction of oxygen was observed at both Mn and Fe redox features; however, a diffusion-limited current was only achieved at potentials consistent with Fe reduction. This result contrasts with that of nanocrystalline MnFe2O4 reported in the literature where the diffusion-limited current is achieved with Mn-based catalysis. This difference is attributed to a low density of Mn surface termination, as determined by the integration of current from CVs collected under N2, in addition to low conductivity through the MnFe2O4 film due to the degree of inversion. Such low densities are attributed to the synthetic method and island-like growth pattern and highlight challenges in studying ORR catalysis with single-crystal spinel materials.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.1c05172.

    • RHEED, AFM, XRR, EDS, and XPS characterization of epitaxial films; cyclic voltammograms and Koutecky–Levich analysis of ORR electrocatalysis; ECSA, specific surface capacitance, and surface charge density calculations (PDF)

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    Cited By

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    This article is cited by 7 publications.

    1. Chunbo Yang, Xiang Yan, Weiwei Gao, Yang Xia, Hongjie Liu, Liuyi Hu, Wenlong Song, Wenkui Zhang, Xinhui Xia, Hui Huang. Facile Synthesis of Laminated Si@C–Fe3O4 Composite from Exfoliation of Zintl Phase: A Promising Lithium Battery Anode with Superior Rate Capability and Cycling Stability. ACS Applied Energy Materials 2024, 7 (3) , 1313-1319. https://doi.org/10.1021/acsaem.3c02974
    2. Liuyi Hu, Zhihang Lu, Fei Chen, Jun Zhang, Yang Xia, Wenkui Zhang, Yongping Gan, Xinping He, Wenlong Song, Hui Huang. Supercritical-Assisted Ball-Milling Synthesis of Multicomponent Si/Fe3O4/C Composites for Outstanding Lithium-Storage Capability. Energy & Fuels 2023, 37 (11) , 8042-8050. https://doi.org/10.1021/acs.energyfuels.3c01074
    3. Shailendra K. Jha Niki S. Jha . Electrocatalysts and Electrocatalysis: From Fundamental Mechanisms to Fuel Cell Applications. , 53-71. https://doi.org/10.1021/bk-2022-1431.ch003
    4. Jingru Ren, Zihan Shi, Yongmin Huang. Zeolitic-imidazolate-framework-derived Fe-NC catalysts towards efficient oxygen reduction reaction. International Journal of Hydrogen Energy 2023, 48 (33) , 12333-12341. https://doi.org/10.1016/j.ijhydene.2022.12.099
    5. Ilgar Ayyubov, Emília Tálas, Camelia Berghian-Grosan, Loránd Románszki, Irina Borbáth, Zoltán Pászti, Ágnes Szegedi, Judith Mihály, Adriana Vulcu, András Tompos. Nitrogen doped carbonaceous materials as platinum free cathode electrocatalysts for oxygen reduction reaction (ORR). Reaction Kinetics, Mechanisms and Catalysis 2023, 136 (1) , 125-147. https://doi.org/10.1007/s11144-022-02331-6
    6. K.A. Dosaev, S.Ya. Istomin, D.A. Strebkov, G.A. Tsirlina, E.V. Antipov, E.R. Savinova. AMn2O4 spinels (A - Li, Mg, Mn, Cd) as ORR catalysts: The role of Mn coordination and oxidation state in the catalytic activity and their propensity to degradation. Electrochimica Acta 2022, 428 , 140923. https://doi.org/10.1016/j.electacta.2022.140923
    7. Lin Tang, Feng Qin, Fei Huang, Dongping Xu, Qiyan Hu, Wu Zhang. Magnetic Fe 3 O 4 @Ag nanoparticles catalyzed C–C cross‐coupling reaction of aromatic alcohols. Applied Organometallic Chemistry 2022, 36 (7) https://doi.org/10.1002/aoc.6723
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    ACS Catalysis

    Cite this: ACS Catal. 2022, 12, 6, 3577–3588
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.1c05172
    Published March 7, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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