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Bifunctional Single Atom Electrocatalysts: Coordination-Performance Correlations and Reaction Pathways.

Wenchao Wan1, Carlos A Triana1, Jinggang Lan1

  • 1University of Zurich, Department of Chemistry, Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.

ACS Nano
|October 13, 2020
PubMed
Summary
This summary is machine-generated.

This study introduces a soft-landing molecular strategy using metal phthalocyanines on graphene oxide to create well-defined single atom catalysts. This advances understanding of coordination-activity relationships for improved oxygen evolution and reduction reactions.

Keywords:
grapheneoperando X-ray absorption spectroscopyoxygen reductionphthalocyaninesingle atom catalystwater oxidation

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Area of Science:

  • Catalysis
  • Materials Science
  • Surface Chemistry

Background:

  • Single atom catalysts (SACs) are crucial for understanding fundamental catalytic mechanisms.
  • Defining active metal centers and their interactions with coordinating atoms is key to catalyst performance.

Purpose of the Study:

  • To develop a strategy for creating well-defined single atom catalysts (SACs) for mechanistic studies.
  • To elucidate the coordination-activity relationships in metal phthalocyanine-graphene oxide (MPc-GO) systems for oxygen reactions.

Main Methods:

  • Soft-landing molecular deposition of metal phthalocyanines (MPcs) onto graphene oxide (GO) layers.
  • Density Functional Theory (DFT) calculations to analyze electronic structures and reaction mechanisms.
  • Operando X-ray absorption spectroscopy to study catalyst behavior under reaction conditions.

Main Results:

  • MPc-GO systems exhibit enhanced performance in oxygen evolution reactions (OER) and oxygen reduction reactions (ORR).
  • FePc-GO shows superior ORR activity due to high affinity of Fe for O2.
  • OER performance is linked to thermodynamic or kinetic control depending on the potential range.
  • Ligating N and C atoms contribute to OER activity in NiPc-GO and CoPc-GO.

Conclusions:

  • The soft-landing strategy yields well-defined SACs for mechanistic investigations.
  • Understanding coordination-activity relationships enables optimization of SACs for specific catalytic processes.
  • Tailored combinations of metal centers and ligands are essential for high-performance SACs.