4.8 Article

Synergistic Catalysis of the Lattice Oxygen and Transition Metal Facilitating ORR and OER in Perovskite Catalysts for Li-O2 Batteries

Journal

ACS CATALYSIS
Volume 11, Issue 1, Pages 424-434

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02608

Keywords

surface lattice oxygen; perovskite LaMnO3; Li-O-2 battery; collective redox; surface atomic structure; Mn termination; La termination; electrocatalyst

Funding

  1. International Energy Joint R&D Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) from Ministry of Trade, Industry & Energy, Republic of Korea [20168510011350]
  2. National Research Foundation of Korea (NRF) - Korea government (MSIT) [NRF-2017R1A2B3004383, NRF-2017R1A5A1015365, NRF-2020M3D1A1110527, NRF-2015M3D1A1068062]
  3. National Research Foundation of Korea (NRF) - Korean government [NRF-2019R1G1A1011320]
  4. National Natural Science Foundation of China [51902339]
  5. National Research Foundation of Korea (NRF) - Ministry of Education [4199990514635]
  6. National Research Foundation of Korea [4199990514635] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The study utilized a precisely surface-engineered model catalyst, perovskite (LaMnO3), to investigate the catalytic nature of oxide catalysts in aprotic Li-O-2 batteries. It was found that the collective redox of lattice oxygen and transition metal on the catalyst surface plays a crucial role in determining the electrochemical performance of the catalyst in Li-O-2 batteries.
The role of catalysts in aprotic Li-O-2 batteries remains unclear. To identify the exact catalytic nature of oxide catalysts, a precisely surface-engineered model catalyst, perovskite (LaMnO3), was investigated for oxygen reduction reaction/oxygen evolution reaction (ORR/OER) in both aqueous and aprotic solutions. By using integrated theoretical and experimental approaches, we explicitly show that H+-ORR/OER catalytic activity on transition-metal sites fails to completely describe the electrochemical performance of LaMnO3 catalysts in aprotic Li-O-2 batteries, whereas the collective redox of the lattice oxygen and transition metal on the catalyst surface during initial Li2O2 formation determines their discharge capacity and charge overpotential. This work applies oxide catalyst design to tailor both the surface lattice oxygen and the transition-metal arrangement for an aprotic Li-O-2 battery. The optimized model catalyst shows good performance for Li-O-2 batteries under both oxygen and ambient air (real air) conditions.

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