Article, 2024

Zeolitic Imidazolate Framework-Derived Pt–Co in Nanofibrous Networks as Stable Oxygen Reduction Electrocatalysts with Low Pt Loading

ACS Applied Materials & Interfaces, ISSN 1944-8252, 1944-8244, Volume 16, 5, Pages 5803-5812, 10.1021/acsami.3c15818

Contributors

Jiang, Tao [1] Im, Han Seo [2] Seo, Daye [3] Dou, Yi-Bo 0000-0003-0802-9898 [4] Park, Sunghak [5] Lim, Sung Yul 0000-0002-2838-6967 (Corresponding author) [2] Shao, Jing 0000-0002-0514-5642 (Corresponding author) [6] Zhang, Wenjing 0000-0002-5011-1951 (Corresponding author) [1]

Affiliations

  1. [1] Technical University of Denmark
  2. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD];
  3. [2] Kyung Hee University
  4. [NORA names: South Korea; Asia, East; OECD];
  5. [3] Seoul National University
  6. [NORA names: South Korea; Asia, East; OECD];
  7. [4] Beijing University of Chemical Technology
  8. [NORA names: China; Asia, East];
  9. [5] Leiden University
  10. [NORA names: Netherlands; Europe, EU; OECD];

Abstract

Proton-exchange membrane fuel cell technology is a key component in the future zero-carbon energy system, generating power from carbon-free fuels, such as green hydrogen. However, the high Pt loading in conventional fuel cell electrodes to maintain electrocatalytic activity and durability, especially on the cathode for oxygen reduction, is the Achilles heel for the worldwide deployment of fuel cell technologies. To minimize Pt consumption for oxygen reduction, we synthesized Pt-Co-based electrocatalysts with meticulous structuring from micrometer to the atomic scale based on reaction pathways. The resulting Pt-Co-based electrocatalysts contain only 1.9 wt% Pt, which is 20 times lower than the conventional Pt-C catalysts for fuel cells. By utilizing electrospinning and in situ synthesis, we anchored three-dimensionally structured zeolitic imidazolate frameworks on continuously connected nanofibrous electrospun mats. The Pt-Co@Pt-free nanowire (PC@PFN) electrocatalysts contain Pt-Co nanoparticles (NPs) and non-Pt elements, Co-containing sites comprising NPs, nanoclusters, and N-coordinated Co single atoms. Despite the ultralow Pt loading in PC@PFN, the mass activity exceeds the U.S. Department of Energy 2025 target by 2.8 times and retains 85.5% of the initial activity after 80,000 durability test cycles, possibly owing to synergistic reaction pathways between Pt and non-Pt sites.

Keywords

Achilles, Achilles heel, Co single atoms, Co-containing, Department of Energy, Pt, Pt consumption, Pt loading, Pt-C catalyst, Pt-Co, Pt-Co nanoparticles, U.S., U.S. Department, U.S. Department of Energy, activity, atomic scale, atoms, carbon-free fuel, catalyst, cathode, cell electrodes, cell technology, cells, components, consumption, cycle, deployment, durability, electrocatalysts, electrocatalytic activity, electrode, electrospun mats, elements, energy, energy systems, framework, fuel, fuel cell electrodes, fuel cell technology, fuel cells, green hydrogen, heel, hydrogen, imidazolate frameworks, in situ synthesis, load, low Pt loading, low-, mass, mass activity, mats, meticulous structure, nanoclusters, nanofibrous network, nanoparticles, nanowires, network, oxygen, oxygen reduction, oxygen reduction electrocatalysts, pathway, proton exchange membrane fuel cell technology, reaction, reaction pathways, reduction, reduction electrocatalysts, scale, single atoms, sites, structure, synergistic reaction pathways, synthesis, system, target, technology, test cycle, ultralow Pt loading, zeolite, zeolitic imidazolate framework, zero-carbon energy system

Funders

  • National Natural Science Foundation of China
  • National Research Foundation of Korea
  • Ministry of Science and ICT
  • The Velux Foundations

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