Single-Step Direct Laser Writing of Multimetal Oxygen Evolution Catalysts from Liquid Precursors

  • Shannon McGee
    Shannon McGee
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Yu Lei
    Yu Lei
    Department of Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for Atomically Thin Multifunctional Coatings, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    More by Yu Lei
  • James Goff
    James Goff
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    More by James Goff
  • Collin J. Wilkinson
    Collin J. Wilkinson
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Nabila Nabi Nova
    Nabila Nabi Nova
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Cody Matthew Kindle
    Cody Matthew Kindle
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Fu Zhang
    Fu Zhang
    Center for Atomically Thin Multifunctional Coatings, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    More by Fu Zhang
  • Kazunori Fujisawa
    Kazunori Fujisawa
    Research Initiative for Supra-Materials, Shinshu University, Wakasato 4-17-1, Nagano 380-8553, Japan
  • Edgar Dimitrov
    Edgar Dimitrov
    Department of Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Susan B. Sinnott
    Susan B. Sinnott
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Penn State Institutes of Energy and the Environment, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
  • Ismaila Dabo
    Ismaila Dabo
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Penn State Institutes of Energy and the Environment, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    More by Ismaila Dabo
  • Mauricio Terrones*
    Mauricio Terrones
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Department of Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for Atomically Thin Multifunctional Coatings, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Research Initiative for Supra-Materials, Shinshu University, Wakasato 4-17-1, Nagano 380-8553, Japan
    *Email: [email protected]
  • , and 
  • Lauren D. Zarzar*
    Lauren D. Zarzar
    Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    *Email: [email protected]
Cite this: ACS Nano 2021, 15, 6, 9796–9807
Publication Date (Web):June 1, 2021
https://doi.org/10.1021/acsnano.1c00650
Copyright © 2021 American Chemical Society
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Abstract

We investigate a laser direct-write method to synthesize and deposit metastable, mixed transition metal oxides and evaluate their performance as oxygen evolution reaction catalysts. This laser processing method enabled the rapid synthesis of diverse heterogeneous alloy and oxide catalysts directly from cost-effective solution precursors, including catalysts with a high density of nanocrystalline metal alloy inclusions within an amorphous oxide matrix. The nanoscale heterogeneous structures of the synthesized catalysts were consistent with reactive force-field Monte Carlo calculations. By evaluating the impact of varying transition metal oxide composition ratios, we created a stable Fe0.63Co0.19Ni0.18Ox/C catalyst with a Tafel slope of 38.23 mV dec–1 and overpotential of 247 mV, a performance similar to that of IrO2. Synthesized Fe0.63Co0.19Ni0.18Ox/C and Fe0.14Co0.46Ni0.40Ox/C catalysts were experimentally compared in terms of catalytic performance and structural characteristics to determine that higher iron content and a less crystalline structure in the secondary matrix decrease the charge transfer resistance and thus is beneficial for electrocatalytic activity. This conclusion is supported by density-functional theory calculations showing distorted active sites in ternary metal catalysts are key for lowering overpotentials for the oxygen evolution reaction.

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  • Electrochemical data, Raman, XRD, TEM and EDS data, additional details of the Monte Carlo and DFT structures and computations, EDS and electrochemical performance data of the samples, comparisons to other OER catalysts in literature, and the predicted reaction energies and overpotentials for different phases and compositions of OER catalysts (PDF)

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