Direct Laser Writing of Multimetal Bifunctional Catalysts for Overall Water Splitting

Water electrolysis is of interest as a sustainable way to produce clean hydrogen and oxygen fuel and help mitigate the rising problems of climate change while meeting global energy demands. High-efficiency, stable, and earth-abundant bifunctional catalysts are needed to enable more effective electrochemical cells for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Here, we investigate the synthesis, composition, performance, and mechanism of multimetal catalysts serving dual functionality in both OER and HER of water electrolysis. Through a laser synthesis method, we synthesized heterogeneous catalysts of nanocrystalline multimetallic alloy pockets embedded within an amorphous oxide matrix. We evaluated the performance and composition of a range of mixed transition-metal oxide materials for both OER and HER, ultimately synthesizing a Cr0.01Fe0.27Co0.34Ni0.38Ox/Cy catalyst that has a stable, high-rate, and competitive overall water splitting performance of 1.76 V at 100 mA cm-2 in an alkaline medium. Using density functional theory to gain insight as the active site and mechanism, we propose that the inclusion of a minor amount of Cr increases the degeneracy of energetic states that lowers the cost of forming the O 2 p-d bond and H 1 s-d bond due to the hybridization of s, p, and d orbitals from Cr. Using a two-electrode water electrolysis cell with a constant potential of 1.636 V to mimic the setup for fuel production, we found the catalyst to be stable at 14-15 mA cm-2 for 40 h. This laser synthesis method allowing for facile and rapid synthesis of complex multimetal systems demonstrates how doping a Fe, Co, and Ni heterogeneous amorphous/nanocrystalline structure with small amounts of Cr is important for bifunctional catalytic behavior, particularly for increasing HER functionality in advancing our understanding for future electrocatalytic design.

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Work Title Direct Laser Writing of Multimetal Bifunctional Catalysts for Overall Water Splitting
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Open Access
Creators
  1. Shannon McGee
  2. Andres Fest
  3. Cierra Chandler
  4. Nabila N. Nova
  5. Yu Lei
  6. James Goff
  7. Susan B. Sinnott
  8. Ismaila Dabo
  9. Mauricio Terrones
  10. Lauren D. Zarzar
Keyword
  1. Laser writing
  2. Multimetal catalysis
  3. Oxygen evolution reaction
  4. Hydrogen evolution reaction
  5. Water splitting
  6. Transition-metal oxides
  7. Nanostructured materials
License In Copyright (Rights Reserved)
Work Type Article
Publisher
  1. ACS Applied Energy Materials
Publication Date March 24, 2023
Publisher Identifier (DOI)
  1. https://doi.org/10.1021/acsaem.2c03973
Deposited February 12, 2024

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Version 1
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  • Created
  • Added mcgee-et-al-2023-direct-laser-writing-of-multimetal-bifunctional-catalysts-for-overall-water-splitting.pdf
  • Added Creator Shannon McGee
  • Added Creator Andres Fest
  • Added Creator Cierra Chandler
  • Added Creator Nabila N. Nova
  • Added Creator Yu Lei
  • Added Creator James Goff
  • Added Creator Susan B. Sinnott
  • Added Creator Ismaila Dabo
  • Added Creator Mauricio Terrones
  • Added Creator Lauren D. Zarzar
  • Published
  • Updated Keyword, Publication Date Show Changes
    Keyword
    • Laser writing, Multimetal catalysis, Oxygen evolutionreaction
    Publication Date
    • 2023-04-10
    • 2023-03-24
  • Updated Keyword Show Changes
    Keyword
    • Laser writing, Multimetal catalysis, Oxygen evolutionreaction
    • Laser writing, Multimetal catalysis, Oxygen evolution reaction, Hydrogen evolution reaction, Water splitting, Transition-metal oxides, Nanostructured materials
  • Updated