Iridium Incorporation into MnO2 for an Enhanced Electrocatalytic Oxygen Evolution Reaction

Kakati, Uddipana; Elzinga, Evert J.; Mansley, Zachary R.; Roe, Benjamin; Alimohammadi, Farbod; Schwenk, Gregory; Ning, Jinliang; Zhu, Yimei; Ji, Hai‐Feng; Sun, Jianwei; Strongin, Daniel R.

doi:10.1002/cctc.202201549

Iridium Incorporation into MnO₂ for an Enhanced Electrocatalytic Oxygen Evolution Reaction

Journal Article · Tue Feb 28 00:00:00 EST 2023 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.202201549· OSTI ID:1975239

^[1]; ^[2]; ^[3]; Roe, Benjamin ^[1]; ^[1]; ^[4]; ^[5]; Zhu, Yimei ^[3]; Ji, Hai‐Feng ^[4]; ^[5]; ^[1]

Temple Univ., Philadelphia, PA (United States)
Rutgers University, Newark, NJ (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Drexel Univ., Philadelphia, PA (United States)
Tulane Univ., New Orleans, LA (United States)

Here, we have investigated the structure and activity of electrocatalysts for the oxygen evolution reaction (OER) that had low loadings of Ir incorporated into the 2D layered MnO₂, (birnessite, nominally δ-MnO₂) and the 3D MnO₂ (pyrolusite, β-MnO₂). The Ir-incorporated β-MnO₂ (Ir/β-MnO₂) electrocatalysts were prepared for the first time via a thermally induced phase transition of δ-MnO₂ containing 16-22 wt% Ir. This phase transition of δ-MnO₂ to β-MnO₂ was facilitated by the presence of Ir in the structure, as both Ir in IrO₂ and Mn in β-MnO₂ could adopt a thermodynamically favored rutile structure. Extended X-ray absorption fine structure (EXAFS) of Ir/β-MnO₂ showed that the catalyst consisted of Ir substituted into the crystalline β-MnO₂ lattice. 22 wt% Ir/β-MnO₂ (60 μg_Ir cm $$\ ^{-2}_{geo}$$) exhibited an OER overpotential (η) of 337 mV, lower than the η for commercial IrO₂. This η was constant for 6 h, at 10 mA cm $$\ ^{-2}_{geo}$$ in 0.5 M H₂SO₄. EXAFS, high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption near edge structure (XANES) showed that 22 wt% Ir/β-MnO₂ had a strained structure containing ~41% Mn³⁺, an OER active species, along with a modified Ir bond covalency consisting of both Ir-O-Ir and Ir-O-Mn.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 1975239

Alternate ID(s):: OSTI ID: 1971281

Report Number(s):: BNL-224444-2023-JAAM

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 8 Vol. 15; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
EXAFS
HAADF-STEM
iridium oxide
manganese oxide
oxygen evolution reaction

Iridium Incorporation into MnO2 for an Enhanced Electrocatalytic Oxygen Evolution Reaction

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Iridium Incorporation into MnO₂ for an Enhanced Electrocatalytic Oxygen Evolution Reaction