Enhanced Activity in Layered Metal-Oxide-Based Oxygen Evolution Catalysts by Layer-by-Layer Modulation of Metal-Ion Identity

Ding, Ran; Maldonado-Lopez, Daniel; Henebry, Jacob E.; Mendoza-Cortes, Jose; Zdilla, Michael J.

doi:10.1021/acscatal.5c02788

Title: Enhanced Activity in Layered Metal-Oxide-Based Oxygen Evolution Catalysts by Layer-by-Layer Modulation of Metal-Ion Identity

Journal Article · Mon Nov 24 00:00:00 UTC 2025 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.5c02788 · OSTI ID:3008122

Ding, Ran ^[1]; Maldonado-Lopez, Daniel ^[2]; Henebry, Jacob E. ^[3];

^[2];

^[3]

Temple University, Philadelphia, PA (United States); North Carolina State University, Raleigh, NC (United States)
Michigan State University, East Lansing, MI (United States)
Temple University, Philadelphia, PA (United States)

Few-layered potassium nickel and cobalt oxides show drastic differences in catalytic activity based on metal ion preorganization. Uniform compositions [(CoO₂/K)₆ or (NiO₂/K)₆] show limited activity, while homogeneously mixed-metal cobalt/nickel oxides [(Co_nNi_(1–n)O₂/K)₆] display moderate improvement. However, a layer-by-layer arrangement of alternating cobalt and nickel oxide sheets [e.g., (CoO₂/K/NiO₂/K)] provides superior catalytic performance, reducing the oxygen evolution overpotential by ∼200–400 mV. Density functional theory simulations provide an illustration of the electronic properties (density of states and localization of orbitals) that promote catalysis in the layer-segregated materials over those of homogeneous composition. This study reveals that atomic preorganization of metal ions within layered catalysts plays a more crucial role than the overall metal composition in enhancing catalytic efficiency for oxygen evolution.

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Research Organization:: US Department of Energy (USDOE), Washington, DC (United States). Office of Science

Sponsoring Organization:: National Science Foundation (NSF) Major Research Instrumentation; National Science Foundation Graduate Research Fellowship; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012575; SC0023356

OSTI ID:: 3008122

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 23 Vol. 15; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Enhanced Activity in Layered Metal-Oxide-Based Oxygen Evolution Catalysts by Layer-by-Layer Modulation of Metal-Ion Identity

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