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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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Potential- and Buffer-Dependent Catalyst Decomposition during Nickel-Based Water Oxidation Catalysis.

Joeri Hessels¹, Fengshou Yu¹, Remko J Detz²

¹Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van 't Hoff institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH, Amsterdam (The, Netherlands.

|September 22, 2020

Summary

This summary is machine-generated.

Nickel catalysts for water oxidation can decompose into active nickel oxide (NiO_x) layers in specific pH conditions. This decomposition, dependent on pH and buffer type, necessitates careful in situ characterization for accurate catalyst design rules.

Keywords:

electrocatalysis electrochemistry nanoparticles nickel water splitting

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Area of Science:

Electrochemistry
Catalysis
Materials Science

Background:

Hydrogen production via water electrolysis requires efficient water oxidation catalysts.
Molecular catalyst reactivity can be obscured by decomposition into nanoparticles, leading to misinterpretation of design rules.

Purpose of the Study:

To investigate the catalytic behavior of the nickel-based water oxidation catalyst [Ni^II (meso-L)](ClO₄ )₂.
To determine if the catalyst operates as a molecular species or decomposes under operational conditions.

Main Methods:

Controlled potential electrolysis
Electrochemical quartz crystal microbalance
X-ray photoelectron spectroscopy (XPS)

Main Results:

The nickel catalyst decomposes into a NiO_x layer in pH 7.0 phosphate buffer.
The NiO_x layer desorbs at lower potentials, leaving no detectable nickel species.
Decomposition is pH and buffer-dependent; no NiO_x forms at pH 6.5 (phosphate) or pH 7.0 (acetate).

Conclusions:

In situ characterization is crucial for identifying catalyst decomposition and metal oxide formation.
Previously proposed design rules for nickel-based catalysts require revision due to decomposition phenomena.