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Title: Heat-Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction

Abstract

Aerogels are fascinating materials that can be used for a wide range of applications, one of which is electrocatalysis of the important oxygen reduction reaction. In their inorganic form, aerogels can have ultrahigh catalytic site density, high surface area, and tunable physical properties and chemical structures—important features in heterogeneous catalysis. Herein, we report on the synthesis and electrocatalytic properties of an iron–porphyrin aerogel. 5,10,15,20-(Tetra-4-aminophenyl)porphyrin (H2TAPP) and FeII were used as building blocks of the aerogel, which was later heat-treated at 600 °C to enhance electronic conductivity and catalytic activity, while preserving its macrostructure. The resulting material has a very high concentration of atomically dispersed catalytic sites (9.7×1020 sites g–1) capable of catalyzing the oxygen reduction reaction in alkaline solution (Eonset=0.92 V vs. RHE, TOF=0.25 e– site–1 s–1 at 0.80 V vs. RHE).

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Bar-Ilan Univ., Ramat-Gan (Israel)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1709106
Alternate Identifier(s):
OSTI ID: 1580132; OSTI ID: 1776773
Report Number(s):
LA-UR-21-22950
Journal ID: ISSN 1433-7851
Grant/Contract Number:  
AC05-00OR22725; 89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 6; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Energy sciences; aerogels; covalent organic frameworks; electrocatalysis; oxygen reduction; porphyrins

Citation Formats

Zion, Noam, Cullen, David A., Zelenay, Piotr, and Elbaz, Lior. Heat-Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction. United States: N. p., 2019. Web. doi:10.1002/anie.201913521.
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Zion, Noam, Cullen, David A., Zelenay, Piotr, & Elbaz, Lior. Heat-Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction. United States. https://doi.org/10.1002/anie.201913521
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Zion, Noam, Cullen, David A., Zelenay, Piotr, and Elbaz, Lior. Wed . "Heat-Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction". United States. https://doi.org/10.1002/anie.201913521. https://www.osti.gov/servlets/purl/1709106.
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@article{osti_1709106,
title = {Heat-Treated Aerogel as a Catalyst for the Oxygen Reduction Reaction},
author = {Zion, Noam and Cullen, David A. and Zelenay, Piotr and Elbaz, Lior},
abstractNote = {Aerogels are fascinating materials that can be used for a wide range of applications, one of which is electrocatalysis of the important oxygen reduction reaction. In their inorganic form, aerogels can have ultrahigh catalytic site density, high surface area, and tunable physical properties and chemical structures—important features in heterogeneous catalysis. Herein, we report on the synthesis and electrocatalytic properties of an iron–porphyrin aerogel. 5,10,15,20-(Tetra-4-aminophenyl)porphyrin (H2TAPP) and FeII were used as building blocks of the aerogel, which was later heat-treated at 600 °C to enhance electronic conductivity and catalytic activity, while preserving its macrostructure. The resulting material has a very high concentration of atomically dispersed catalytic sites (9.7×1020 sites g–1) capable of catalyzing the oxygen reduction reaction in alkaline solution (Eonset=0.92 V vs. RHE, TOF=0.25 e– site–1 s–1 at 0.80 V vs. RHE).},
doi = {10.1002/anie.201913521},
journal = {Angewandte Chemie (International Edition)},
number = 6,
volume = 59,
place = {United States},
year = {Wed Nov 27 00:00:00 EST 2019},
month = {Wed Nov 27 00:00:00 EST 2019}
}
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https://doi.org/10.1002/anie.201913521
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Works referenced in this record:

A review on non-precious metal electrocatalysts for PEM fuel cells
journal, January 2011

  • Chen, Zhongwei; Higgins, Drew; Yu, Aiping
  • Energy & Environmental Science, Vol. 4, Issue 9
  • DOI: 10.1039/c0ee00558d

Bioinspired Electrocatalysis of Oxygen Reduction Reaction in Fuel Cells Using Molecular Catalysts
journal, April 2018

Conducting Stacked Metallophthalocyanines and Related Compounds
journal, November 1994

Heat-Treated Non-precious-Metal-Based Catalysts for Oxygen Reduction
book, January 2013

Efficient approach to iron/nitrogen co-doped graphene materials as efficient electrochemical catalysts for the oxygen reduction reaction
journal, January 2015

  • Dong, Qingqing; Zhuang, Xiaodong; Li, Zhi
  • Journal of Materials Chemistry A, Vol. 3, Issue 15
  • DOI: 10.1039/C5TA00556F

Degradation Mechanisms of Pt/C Fuel Cell Catalysts under Simulated Start–Stop Conditions
journal, April 2012

  • Meier, Josef C.; Galeano, Carolina; Katsounaros, Ioannis
  • ACS Catalysis, Vol. 2, Issue 5
  • DOI: 10.1021/cs300024h

Metallocorroles as Non-Precious Metal Electrocatalysts for Highly Efficient Oxygen Reduction in Alkaline Media
journal, August 2016

In situ electrochemical quantification of active sites in Fe–N/C non-precious metal catalysts
journal, October 2016

  • Malko, Daniel; Kucernak, Anthony; Lopes, Thiago
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13285

Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs
journal, March 2005

  • Gasteiger, Hubert A.; Kocha, Shyam S.; Sompalli, Bhaskar
  • Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 9-35
  • DOI: 10.1016/j.apcatb.2004.06.021

A Crystalline Imine-Linked 3-D Porous Covalent Organic Framework
journal, April 2009

  • Uribe-Romo, Fernando J.; Hunt, Joseph R.; Furukawa, Hiroyasu
  • Journal of the American Chemical Society, Vol. 131, Issue 13, p. 4570-4571
  • DOI: 10.1021/ja8096256

A Systematic Approach toward Designing Functional Ionic Porphyrin Crystalline Materials
journal, July 2018

Organic aerogels from the polycondensation of resorcinol with formaldehyde
journal, September 1989

Highly efficient nonprecious metal catalysts towards oxygen reduction reaction based on three-dimensional porous carbon nanostructures
journal, January 2016

  • Zhu, Chengzhou; Li, He; Fu, Shaofang
  • Chemical Society Reviews, Vol. 45, Issue 3
  • DOI: 10.1039/C5CS00670H

Electrical conductivity of thermal carbon blacks
journal, July 2001

Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation
journal, October 2007

  • Borup, Rod; Meyers, Jeremy; Pivovar, Bryan
  • Chemical Reviews, Vol. 107, Issue 10
  • DOI: 10.1021/cr050182l

Electropolymerization of PGM-free molecular catalyst for formation of 3D structures with high density of catalytic sites
journal, July 2019

Metallocorroles as Nonprecious-Metal Catalysts for Oxygen Reduction
journal, October 2015

  • Levy, Naomi; Mahammed, Atif; Kosa, Monica
  • Angewandte Chemie International Edition, Vol. 54, Issue 47
  • DOI: 10.1002/anie.201505236

Aerogels Handbook
book, January 2011

Oxygen Binding to Active Sites of Fe–N–C ORR Electrocatalysts Observed by Ambient-Pressure XPS
journal, January 2017

  • Artyushkova, Kateryna; Matanovic, Ivana; Halevi, Barr
  • The Journal of Physical Chemistry C, Vol. 121, Issue 5
  • DOI: 10.1021/acs.jpcc.6b11721

An XPS analysis of the interaction of meso -tetrakis( N -methylpyridinium-4-yl)porphyrin with exfoliated manganese thiophosphate
journal, June 2006

Characterization of the “native” surface thin film on pure polycrystalline iron: A high resolution XPS and TEM study
journal, February 2007

Just a Dream—or Future Reality?
journal, April 2009

A New Fuel Cell Cathode Catalyst
journal, March 1964

  • Jasinski, Raymond
  • Nature, Vol. 201, Issue 4925, p. 1212-1213
  • DOI: 10.1038/2011212a0

Highly dispersed platinum on carbon aerogels as supported catalysts for PEM fuel cell-electrodes: comparison of two different synthesis paths
journal, December 2004

The materials chemistry of porphyrins and metalloporphyrins
journal, June 2000

Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts
journal, October 2015

  • Sahraie, Nastaran Ranjbar; Kramm, Ulrike I.; Steinberg, Julian
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9618

Heterogeneous metal-insertion: a novel reaction with porphyrins
journal, April 1978

  • Herrmann, Otto; Mehdi, S. Husain; Corsini, Alfio
  • Canadian Journal of Chemistry, Vol. 56, Issue 8
  • DOI: 10.1139/v78-184

Comparative XPS surface study of polyaniline thin films
journal, December 2008

Heat- or Water-Driven Malleability in a Highly Recyclable Covalent Network Polymer
journal, March 2014

  • Taynton, Philip; Yu, Kai; Shoemaker, Richard K.
  • Advanced Materials, Vol. 26, Issue 23
  • DOI: 10.1002/adma.201400317

The Aerocapacitor: An Electrochemical Double-Layer Energy-Storage Device
journal, January 1993

  • Mayer, S. T.
  • Journal of The Electrochemical Society, Vol. 140, Issue 2
  • DOI: 10.1149/1.2221066

A pure organic heterostructure of μ-oxo dimeric iron( iii ) porphyrin and graphitic-C 3 N 4 for solar H 2 roduction from water
journal, January 2016

  • Wang, D. H.; Pan, J. N.; Li, H. H.
  • Journal of Materials Chemistry A, Vol. 4, Issue 1
  • DOI: 10.1039/C5TA07278F

Recent advances in non-precious metal catalysis for oxygen-reduction reaction in polymer electrolyte fuelcells
journal, January 2011

  • Jaouen, Frédéric; Proietti, Eric; Lefèvre, Michel
  • Energy Environ. Sci., Vol. 4, Issue 1, p. 114-130
  • DOI: 10.1039/C0EE00011F

Aerogel applications
journal, April 1998

Synthesis–structure–performance correlation for polyaniline–Me–C non-precious metal cathode catalysts for oxygen reduction in fuel cells
journal, January 2011

  • Wu, Gang; Johnston, Christina M.; Mack, Nathan H.
  • Journal of Materials Chemistry, Vol. 21, Issue 30
  • DOI: 10.1039/c0jm03613g

Conductive polymers derived from iron, ruthenium, and osmium metalloporphyrins: The shish-kebab approach
journal, July 1986

  • Collman, J. P.; McDevitt, J. T.; Yee, G. T.
  • Proceedings of the National Academy of Sciences, Vol. 83, Issue 13
  • DOI: 10.1073/pnas.83.13.4581

Self-templated chemically stable hollow spherical covalent organic framework
journal, April 2015

  • Kandambeth, Sharath; Venkatesh, V.; Shinde, Digambar B.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7786

Metallocorroles as Nonprecious-Metal Catalysts for Oxygen Reduction
journal, October 2015

Efficient Bio-Inspired Oxygen Reduction Electrocatalysis with Electropolymerized Cobalt Corroles
journal, April 2018

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