Myoglobin-based non-precious metal carbon catalysts for an oxygen reduction reaction

Akira Onoda, Yuta Tanaka, Toshikazu Ono, Shotaro Takeuchi, Akira Sakai, Takashi Hayashi

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

A non-precious metal catalyst (NPMC) promoting a four-electron oxygen reduction reaction (ORR) was synthesized by heat treatment of myoglobin (Mb) containing a heme (iron protoporphyrin IX) as a source of iron, nitrogen, and carbon atoms. Samples of the mixture of Mb and carbon black (Vulcan XC72R: VC) were pyrolyzed at 740, 840, 940, 1040 or 1140°C under N2 flow. The microstructures of the carbonized Mb catalysts were characterized by XRD, Raman spectroscopy, XPS, and TEM. Results indicate that the iron-containing active site is embedded within the surface structure in an amorphous domain of the carbon materials. The catalyst ink in a 0.05 wt% Nafion solution in isopropanol was coated onto a glassy carbon electrode and the ORR activity of Mb-based NPMCs was evaluated in a rotating disk electrode experiment in an O2-saturated 0.1 M HClO4 solution at 25°C. The catalyst synthesized at 940°C has the highest ORR activity in terms of the onset potential and the current density. In contrast, pyrolytic temperatures above 940°C decrease the activity, suggesting that the active structure of the catalyst apparently decomposes at higher temperatures. The Koutecky-Levich plots indicate that the Mb-based catalyst prepared at 940°C catalyzes four-electron ORR (n = ca. 4). The catalysts prepared at other temperatures have n values of 3.6 at 740°C, 3.7 at 840°C, and 2.9 at 1040°C. The ORR of Mb/VC is diffusion-controlled at potentials lower than 0.3 V (vs. RHE) and the onset potential is 0.84 ± 0.01 V.

Original languageEnglish
Pages (from-to)510-516
Number of pages7
JournalJournal of Porphyrins and Phthalocyanines
Volume19
Issue number1-3
DOIs
Publication statusPublished - Jan 1 2015

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Myoglobin
Carbon
Metals
Oxygen
Catalysts
Iron
Soot
Electrodes
2-Propanol
Electrons
Glassy carbon
Rotating disks
Heme
Ink
Surface structure
Temperature
Raman spectroscopy
Current density
Nitrogen
X ray photoelectron spectroscopy

All Science Journal Classification (ASJC) codes

  • Chemistry(all)

Cite this

Myoglobin-based non-precious metal carbon catalysts for an oxygen reduction reaction. / Onoda, Akira; Tanaka, Yuta; Ono, Toshikazu; Takeuchi, Shotaro; Sakai, Akira; Hayashi, Takashi.

In: Journal of Porphyrins and Phthalocyanines, Vol. 19, No. 1-3, 01.01.2015, p. 510-516.

Research output: Contribution to journalArticle

Onoda, Akira ; Tanaka, Yuta ; Ono, Toshikazu ; Takeuchi, Shotaro ; Sakai, Akira ; Hayashi, Takashi. / Myoglobin-based non-precious metal carbon catalysts for an oxygen reduction reaction. In: Journal of Porphyrins and Phthalocyanines. 2015 ; Vol. 19, No. 1-3. pp. 510-516.
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abstract = "A non-precious metal catalyst (NPMC) promoting a four-electron oxygen reduction reaction (ORR) was synthesized by heat treatment of myoglobin (Mb) containing a heme (iron protoporphyrin IX) as a source of iron, nitrogen, and carbon atoms. Samples of the mixture of Mb and carbon black (Vulcan XC72R: VC) were pyrolyzed at 740, 840, 940, 1040 or 1140°C under N2 flow. The microstructures of the carbonized Mb catalysts were characterized by XRD, Raman spectroscopy, XPS, and TEM. Results indicate that the iron-containing active site is embedded within the surface structure in an amorphous domain of the carbon materials. The catalyst ink in a 0.05 wt{\%} Nafion solution in isopropanol was coated onto a glassy carbon electrode and the ORR activity of Mb-based NPMCs was evaluated in a rotating disk electrode experiment in an O2-saturated 0.1 M HClO4 solution at 25°C. The catalyst synthesized at 940°C has the highest ORR activity in terms of the onset potential and the current density. In contrast, pyrolytic temperatures above 940°C decrease the activity, suggesting that the active structure of the catalyst apparently decomposes at higher temperatures. The Koutecky-Levich plots indicate that the Mb-based catalyst prepared at 940°C catalyzes four-electron ORR (n = ca. 4). The catalysts prepared at other temperatures have n values of 3.6 at 740°C, 3.7 at 840°C, and 2.9 at 1040°C. The ORR of Mb/VC is diffusion-controlled at potentials lower than 0.3 V (vs. RHE) and the onset potential is 0.84 ± 0.01 V.",
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