Understanding Degradation Mechanisms in SrIrO3 Oxygen Evolution Electrocatalysts: Chemical and Structural Microscopy at the Nanoscale

Micha Ben-Naim; Yunzhi Liu; Michaela Burke Stevens; Kyuho Lee; Melissa R. Wette; Alexey Boubnov; Artem A. Trofimov; Anton V. Ievlev; Alex Belianinov; Ryan C. Davis; Bruce M. Clemens; Simon R. Bare; Yasuyuki Hikita; Harold Y. Hwang; Drew C. Higgins; Robert Sinclair; Thomas F. Jaramillo

doi:10.1002/adfm.202101542

Understanding Degradation Mechanisms in SrIrO₃ Oxygen Evolution Electrocatalysts: Chemical and Structural Microscopy at the Nanoscale

Micha Ben-Naim, Yunzhi Liu, Michaela Burke Stevens, Kyuho Lee, Melissa R. Wette, Alexey Boubnov, Artem A. Trofimov, Anton V. Ievlev, Alex Belianinov, Ryan C. Davis, Bruce M. Clemens, Simon R. Bare, Yasuyuki Hikita, Harold Y. Hwang, Drew C. Higgins, Robert Sinclair, Thomas F. Jaramillo

Functional Atomic Force Microscopy Group

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

Designing acid-stable oxygen evolution reaction electrocatalysts is key to developing sustainable energy technologies such as polymer electrolyte membrane electrolyzers but has proven challenging due to the high applied anodic potentials and corrosive electrolyte. This work showcases advanced nanoscale microscopy techniques supported by complementary structural and chemical characterization to develop a fundamental understanding of stability in promising SrIrO₃ thin film electrocatalyst materials. Cross-sectional high-resolution transmission electron microscopy illustrates atomic-scale bulk and surface structure, while secondary ion mass spectrometry imaging using a helium ion microscope provides the nanoscale lateral elemental distribution at the surface. After accelerated degradation tests under anodic potential, the SrIrO₃ film thins and roughens, but the lateral distribution of Sr and Ir remains homogeneous. A layer-wise dissolution mechanism is hypothesized, wherein anodic potential causes the IrO_x-rich surface to dissolve and be regenerated by Sr leaching. The characterization approaches utilized herein and mechanistic insights into SrIrO₃ are translatable to a wide range of catalyst systems.

Original language	English
Article number	2101542
Journal	Advanced Functional Materials
Volume	31
Issue number	34
DOIs	https://doi.org/10.1002/adfm.202101542
State	Published - Aug 20 2021

Funding

M.B. and Y.L. are the primary authors and contributed equally to this work. This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program to the SUNCAT Center for Interface Science and Catalysis. Y.L., M.B.S., and R.S. acknowledge the support from the Toyota Research Institute–Accelerated Materials Design and Discovery (TRI‐AMDD) program (Stanford University) for efforts in TEM and SIMS. K.L., Y.H., and H.Y.H. acknowledge support from the Laboratory Directed Research and Development program at SLAC National Accelerator Laboratory, and the US Department of Energy, Office of Basic Energy sciences, Division of Materials Sciences and Engineering, under contract number DE‐AC02‐76SF00515, for efforts in material synthesis, characterization, and testing. The authors acknowledge Apurva Mehta for his support with XAS measurements and analysis. Part of this work (XPS and TEM characterization) was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS‐1542152. HIM‐SIMS and ToF‐SIMS characterization was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility, using instrumentation within ORNL's Materials Characterization Core provided by UT‐Battelle, LLC under contract no. DE‐AC05‐00OR22725 with the US DOE. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the US DoE, Office of BES under contract no. DE‐AC02‐76SF00515. M.B. and Y.L. are the primary authors and contributed equally to this work. This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program to the SUNCAT Center for Interface Science and Catalysis. Y.L., M.B.S., and R.S. acknowledge the support from the Toyota Research Institute–Accelerated Materials Design and Discovery (TRI-AMDD) program (Stanford University) for efforts in TEM and SIMS. K.L., Y.H., and H.Y.H. acknowledge support from the Laboratory Directed Research and Development program at SLAC National Accelerator Laboratory, and the US Department of Energy, Office of Basic Energy sciences, Division of Materials Sciences and Engineering, under contract number DE-AC02-76SF00515, for efforts in material synthesis, characterization, and testing. The authors acknowledge Apurva Mehta for his support with XAS measurements and analysis. Part of this work (XPS and TEM characterization) was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. HIM-SIMS and ToF-SIMS characterization was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility, using instrumentation within ORNL's Materials Characterization Core provided by UT-Battelle, LLC under contract no. DE-AC05-00OR22725 with the US DOE. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the US DoE, Office of BES under contract no. DE-AC02-76SF00515.

Funders	Funder number
Apurva Mehta
Catalysis Science Program
TRI-AMDD
TRI‐AMDD
National Science Foundation	ECCS‐1542152
U.S. Department of Energy
Stanford University
Office of Science	DE-AC05-00OR22725
Basic Energy Sciences
Laboratory Directed Research and Development
Division of Materials Sciences and Engineering	DE‐AC02‐76SF00515
Chemical Sciences, Geosciences, and Biosciences Division
Toyota Research Institute

Keywords

electrocatalysis
mass spectrometry imaging
oxygen evolution reaction
secondary ion mass spectrometry
transmission electron microscopy

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/adfm.202101542

Cite this

Ben-Naim, M., Liu, Y., Stevens, M. B., Lee, K., Wette, M. R., Boubnov, A., Trofimov, A. A., Ievlev, A. V., Belianinov, A., Davis, R. C., Clemens, B. M., Bare, S. R., Hikita, Y., Hwang, H. Y., Higgins, D. C., Sinclair, R., & Jaramillo, T. F. (2021). Understanding Degradation Mechanisms in SrIrO₃ Oxygen Evolution Electrocatalysts: Chemical and Structural Microscopy at the Nanoscale. Advanced Functional Materials, 31(34), Article 2101542. https://doi.org/10.1002/adfm.202101542

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abstract = "Designing acid-stable oxygen evolution reaction electrocatalysts is key to developing sustainable energy technologies such as polymer electrolyte membrane electrolyzers but has proven challenging due to the high applied anodic potentials and corrosive electrolyte. This work showcases advanced nanoscale microscopy techniques supported by complementary structural and chemical characterization to develop a fundamental understanding of stability in promising SrIrO3 thin film electrocatalyst materials. Cross-sectional high-resolution transmission electron microscopy illustrates atomic-scale bulk and surface structure, while secondary ion mass spectrometry imaging using a helium ion microscope provides the nanoscale lateral elemental distribution at the surface. After accelerated degradation tests under anodic potential, the SrIrO3 film thins and roughens, but the lateral distribution of Sr and Ir remains homogeneous. A layer-wise dissolution mechanism is hypothesized, wherein anodic potential causes the IrOx-rich surface to dissolve and be regenerated by Sr leaching. The characterization approaches utilized herein and mechanistic insights into SrIrO3 are translatable to a wide range of catalyst systems.",

keywords = "electrocatalysis, mass spectrometry imaging, oxygen evolution reaction, secondary ion mass spectrometry, transmission electron microscopy",

author = "Micha Ben-Naim and Yunzhi Liu and Stevens, {Michaela Burke} and Kyuho Lee and Wette, {Melissa R.} and Alexey Boubnov and Trofimov, {Artem A.} and Ievlev, {Anton V.} and Alex Belianinov and Davis, {Ryan C.} and Clemens, {Bruce M.} and Bare, {Simon R.} and Yasuyuki Hikita and Hwang, {Harold Y.} and Higgins, {Drew C.} and Robert Sinclair and Jaramillo, {Thomas F.}",

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Ben-Naim, M, Liu, Y, Stevens, MB, Lee, K, Wette, MR, Boubnov, A, Trofimov, AA, Ievlev, AV, Belianinov, A, Davis, RC, Clemens, BM, Bare, SR, Hikita, Y, Hwang, HY, Higgins, DC, Sinclair, R & Jaramillo, TF 2021, 'Understanding Degradation Mechanisms in SrIrO₃ Oxygen Evolution Electrocatalysts: Chemical and Structural Microscopy at the Nanoscale', Advanced Functional Materials, vol. 31, no. 34, 2101542. https://doi.org/10.1002/adfm.202101542

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AU - Clemens, Bruce M.

AU - Bare, Simon R.

AU - Hikita, Yasuyuki

AU - Hwang, Harold Y.

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AU - Sinclair, Robert

AU - Jaramillo, Thomas F.

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N2 - Designing acid-stable oxygen evolution reaction electrocatalysts is key to developing sustainable energy technologies such as polymer electrolyte membrane electrolyzers but has proven challenging due to the high applied anodic potentials and corrosive electrolyte. This work showcases advanced nanoscale microscopy techniques supported by complementary structural and chemical characterization to develop a fundamental understanding of stability in promising SrIrO3 thin film electrocatalyst materials. Cross-sectional high-resolution transmission electron microscopy illustrates atomic-scale bulk and surface structure, while secondary ion mass spectrometry imaging using a helium ion microscope provides the nanoscale lateral elemental distribution at the surface. After accelerated degradation tests under anodic potential, the SrIrO3 film thins and roughens, but the lateral distribution of Sr and Ir remains homogeneous. A layer-wise dissolution mechanism is hypothesized, wherein anodic potential causes the IrOx-rich surface to dissolve and be regenerated by Sr leaching. The characterization approaches utilized herein and mechanistic insights into SrIrO3 are translatable to a wide range of catalyst systems.

AB - Designing acid-stable oxygen evolution reaction electrocatalysts is key to developing sustainable energy technologies such as polymer electrolyte membrane electrolyzers but has proven challenging due to the high applied anodic potentials and corrosive electrolyte. This work showcases advanced nanoscale microscopy techniques supported by complementary structural and chemical characterization to develop a fundamental understanding of stability in promising SrIrO3 thin film electrocatalyst materials. Cross-sectional high-resolution transmission electron microscopy illustrates atomic-scale bulk and surface structure, while secondary ion mass spectrometry imaging using a helium ion microscope provides the nanoscale lateral elemental distribution at the surface. After accelerated degradation tests under anodic potential, the SrIrO3 film thins and roughens, but the lateral distribution of Sr and Ir remains homogeneous. A layer-wise dissolution mechanism is hypothesized, wherein anodic potential causes the IrOx-rich surface to dissolve and be regenerated by Sr leaching. The characterization approaches utilized herein and mechanistic insights into SrIrO3 are translatable to a wide range of catalyst systems.

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KW - mass spectrometry imaging

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