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Understanding oxygen evolution mechanisms by tracking charge flow at the atomic level.

Changming Zhao1,2, Hao Tian1,3, Zhigang Zou1

  • 1School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518172, China.

Iscience
|July 10, 2023
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Summary
This summary is machine-generated.

This study reveals that water orbital positions dictate oxygen evolution reaction pathways, allowing for mixed metal and lattice-oxygen dominated oxidation steps. This advances understanding of water-splitting catalysts.

Keywords:
Molecular mechanics calculationsPhysical chemistryTheoretical chemistry

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Area of Science:

  • Catalysis
  • Surface Chemistry
  • Computational Materials Science

Background:

  • Current oxygen evolution catalyst classifications rely on clean catalyst energy levels.
  • It's generally assumed catalysts follow only specific reaction chemistries (e.g., lattice-oxygen mediated or adsorbed-metal mediated) without external triggers.

Purpose of the Study:

  • To investigate the charge flow in water-on-catalyst systems using *ab initio* theory.
  • To determine the factors controlling electron transfer steps in oxygen evolution reactions (OER).
  • To elucidate the microscopic pathways of photocatalytic water splitting on TiO2(110).

Main Methods:

  • Utilized *ab initio* theory to track charge flow in water-on-catalyst systems.
  • Analyzed the influence of water orbital positions on oxidation pathways.
  • Examined the photocatalytic pathways of TiO2(110) for oxygen evolution.

Main Results:

  • The position of water orbitals is crucial in determining if an electron transfer step is water-dominated oxidation (WDO), lattice-oxygen dominated oxidation (LoDO), or metal-dominated oxidation (MDO).
  • For TiO2(110), viable OER pathways can involve either purely adsorbed-metal exchange (AEM) steps or mixed AEM-LOM steps.
  • Demonstrated that mixing between AEM and LOM steps is possible without external triggers.

Conclusions:

  • Provides an accurate atomic-level description of redox chemistries in water splitting.
  • Advances the fundamental understanding of how water-splitting catalysts generate desorbed oxygen.
  • Challenges existing classifications by showing flexibility in OER pathway mechanisms.