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

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Communication: Water activation and splitting by single metal-atom anions.

Gaoxiang Liu¹, Evangelos Miliordos², Sandra M Ciborowski¹

¹Department of Chemistry, Johns Hopkins University, Baltimore, Maryland 21218, USA.

The Journal of Chemical Physics

|December 17, 2018

Summary

Single atomic platinum anions activate and split water molecules, forming reaction intermediates and products like platinum oxide anion (PtO⁻) and hydrogen gas (H₂). This water-splitting capability extends to nickel and palladium anions.

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Area of Science:

Inorganic Chemistry
Physical Chemistry
Surface Science

Background:

Water splitting is crucial for clean energy technologies.
Understanding the role of single metal atoms in chemical reactions is key to designing efficient catalysts.
Anion photoelectron spectroscopy and mass spectrometry are powerful tools for studying reaction intermediates.

Purpose of the Study:

To investigate the activation and splitting of single water molecules by single atomic platinum anions.
To identify reaction intermediates and products formed during the process.
To explore the water-splitting capabilities of other transition metal anions, such as nickel and palladium.

Main Methods:

Anion photoelectron spectroscopy of [Pt(H₂O)]⁻ and related species.
Mass spectrometry to detect reaction products.
Computational chemistry using coupled cluster singles and doubles with perturbatively connected triples (CCSD(T)) level of theory.

Main Results:

Experimental evidence for the formation of Pt⁻(H₂O), HPtOH⁻, and H₂PtO⁻ intermediates.
Observation of PtO⁻ and H₂⁺, indicating water splitting via Pt⁻ + H₂O → PtO⁻ + H₂.
Similar water activation by nickel and palladium anions, forming HNiOH⁻ and HPdOH⁻ intermediates.
Good agreement between calculated and measured vertical detachment energies (VDEs) for intermediates.

Conclusions:

Single atomic platinum anions can effectively activate and split water molecules.
The observed intermediates and products confirm the proposed water-splitting mechanism.
Nickel and palladium anions also exhibit water activation capabilities, suggesting broader applicability of this approach.
Computational results strongly support the experimental findings and intermediate identifications.