Two-Dimensional Conductive Ni-HAB as a Catalyst for the Electrochemical Oxygen Reduction Reaction

Jihye Park, Zhihua Chen, Raul A. Flores, Gustaf Wallnerström, Ambarish Kulkarni, Jens K. Nørskov*, Thomas F. Jaramillo*, Zhenan Bao*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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Abstract

Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal-organic framework consisting of M-N4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB's catalytic activity, and they suggest that M-HAB's organic linker acts as the active site with the role of the metal being to modulate the linker sites' binding strength.
Original languageEnglish
JournalACS Applied Materials and Interfaces
Volume12
Issue number35
Pages (from-to)39074-39081
ISSN1944-8244
DOIs
Publication statusPublished - 2020

Keywords

  • Metal−organic frameworks
  • Electrical conductivity
  • Electrocatalysis
  • Active sites
  • Oxygen reduction reactions
  • Density functional theory

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