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Title: Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network

Abstract

Fuel cell vehicles, the only all-electric technology with a demonstrated >300 miles per fill travel range, use Pt as the electrode catalyst. The high price of Pt creates a major cost barrier for large-scale implementation of polymer electrolyte membrane fuel cells. Nonprecious metal catalysts (NPMCs) represent attractive low-cost alternatives. However, a significantly lower turnover frequency at the individual catalytic site renders the traditional carbon-supported NPMCs inadequate in reaching the desired performance afforded by Pt. Unconventional catalyst design aiming at maximizing the active site density at much improved mass and charge transports is essential for the next-generation NPMC. We report here a method of preparing highly efficient, nanofibrous NPMC for cathodic oxygen reduction reaction by electrospinning a polymer solution containing ferrous organometallics and zeolitic imidazolate framework followed by thermal activation. The catalyst offers a carbon nanonetwork architecture made of microporous nanofibers decorated by uniformly distributed high-density active sites. In a single-cell test, the membrane electrode containing such a catalyst delivered unprecedented volumetric activities of 3.3 A∙cm-3 at 0.9 V or 450 A∙cm-3 extrapolated at 0.8 V, representing the highest reported value in the literature. Improved fuel cell durability was also observed.

Authors:
 [1];  [2];  [3];  [4];  [2]
  1. Argonne National Lab., Argonne, IL (United States). Chemical Sciences and Engineering Div.; Beihang Univ., Beijing (China). School of Materials Science and Engineering.
  2. Argonne National Lab., Argonne, IL (United States). Chemical Sciences and Engineering Div.
  3. Argonne National Lab., Argonne, IL (United States). Chemical Sciences and Engineering Div.; Alcoa Technical Center, New Kinsington, PA (United States)
  4. National Univ. of Singapore (Singapore). Dept. of Chemical and Biomolecular Engineering.
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO)
OSTI Identifier:
1215638
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 112; Journal Issue: 34; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; 36 MATERIALS SCIENCE; 33 ADVANCED PROPULSION SYSTEMS; nanofibrous; nonprecious metal catalyst; metal-organic framework; fuel cell; oxygen reduction

Citation Formats

Shui, Jianglan, Chen, Chen, Grabstanowicz, Lauren, Zhao, Dan, and Liu, Di -Jia. Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network. United States: N. p., 2015. Web. doi:10.1073/pnas.1507159112.
Shui, Jianglan, Chen, Chen, Grabstanowicz, Lauren, Zhao, Dan, & Liu, Di -Jia. Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network. United States. https://doi.org/10.1073/pnas.1507159112
Shui, Jianglan, Chen, Chen, Grabstanowicz, Lauren, Zhao, Dan, and Liu, Di -Jia. Tue . "Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network". United States. https://doi.org/10.1073/pnas.1507159112. https://www.osti.gov/servlets/purl/1215638.
@article{osti_1215638,
title = {Highly efficient nonprecious metal catalyst prepared with metal–organic framework in a continuous carbon nanofibrous network},
author = {Shui, Jianglan and Chen, Chen and Grabstanowicz, Lauren and Zhao, Dan and Liu, Di -Jia},
abstractNote = {Fuel cell vehicles, the only all-electric technology with a demonstrated >300 miles per fill travel range, use Pt as the electrode catalyst. The high price of Pt creates a major cost barrier for large-scale implementation of polymer electrolyte membrane fuel cells. Nonprecious metal catalysts (NPMCs) represent attractive low-cost alternatives. However, a significantly lower turnover frequency at the individual catalytic site renders the traditional carbon-supported NPMCs inadequate in reaching the desired performance afforded by Pt. Unconventional catalyst design aiming at maximizing the active site density at much improved mass and charge transports is essential for the next-generation NPMC. We report here a method of preparing highly efficient, nanofibrous NPMC for cathodic oxygen reduction reaction by electrospinning a polymer solution containing ferrous organometallics and zeolitic imidazolate framework followed by thermal activation. The catalyst offers a carbon nanonetwork architecture made of microporous nanofibers decorated by uniformly distributed high-density active sites. In a single-cell test, the membrane electrode containing such a catalyst delivered unprecedented volumetric activities of 3.3 A∙cm-3 at 0.9 V or 450 A∙cm-3 extrapolated at 0.8 V, representing the highest reported value in the literature. Improved fuel cell durability was also observed.},
doi = {10.1073/pnas.1507159112},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 34,
volume = 112,
place = {United States},
year = {Tue Aug 25 00:00:00 EDT 2015},
month = {Tue Aug 25 00:00:00 EDT 2015}
}

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Pt-free carbon-based fuel cell catalyst prepared from spherical polyimide for enhanced oxygen diffusion
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Recent developments of nano-structured materials as the catalysts for oxygen reduction reaction
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Bimetallic Metal-Organic Framework Derived Metal-Carbon Hybrid for Efficient Reversible Oxygen Electrocatalysis
journal, November 2019