Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction

Andrea Zitolo (), Nastaran Ranjbar-Sahraie, Tzonka Mineva, Jingkun Li, Qingying Jia, Serban Stamatin, George F. Harrington, Stephen Mathew Lyth, Petr Krtil, Sanjeev Mukerjee, Emiliano Fonda and Frédéric Jaouen ()
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Andrea Zitolo: Synchrotron SOLEIL, L’orme des Merisiers
Nastaran Ranjbar-Sahraie: Institut Charles Gerhardt Montpellier, UMR 5253, CNRS, Université Montpellier
Tzonka Mineva: Institut Charles Gerhardt Montpellier, UMR 5253, CNRS, Université Montpellier
Jingkun Li: Northeastern University
Qingying Jia: Northeastern University
Serban Stamatin: Academy of Sciences of the Czech Republic
George F. Harrington: Kyushu University
Stephen Mathew Lyth: Kyushu University
Petr Krtil: Academy of Sciences of the Czech Republic
Sanjeev Mukerjee: Northeastern University
Emiliano Fonda: Synchrotron SOLEIL, L’orme des Merisiers
Frédéric Jaouen: Institut Charles Gerhardt Montpellier, UMR 5253, CNRS, Université Montpellier

Nature Communications, 2017, vol. 8, issue 1, 1-11

Abstract: Abstract Single-atom catalysts with full utilization of metal centers can bridge the gap between molecular and solid-state catalysis. Metal-nitrogen-carbon materials prepared via pyrolysis are promising single-atom catalysts but often also comprise metallic particles. Here, we pyrolytically synthesize a Co–N–C material only comprising atomically dispersed cobalt ions and identify with X-ray absorption spectroscopy, magnetic susceptibility measurements and density functional theory the structure and electronic state of three porphyrinic moieties, CoN4C12, CoN3C10,porp and CoN2C5. The O2 electro-reduction and operando X-ray absorption response are measured in acidic medium on Co–N–C and compared to those of a Fe–N–C catalyst prepared similarly. We show that cobalt moieties are unmodified from 0.0 to 1.0 V versus a reversible hydrogen electrode, while Fe-based moieties experience structural and electronic-state changes. On the basis of density functional theory analysis and established relationships between redox potential and O2-adsorption strength, we conclude that cobalt-based moieties bind O2 too weakly for efficient O2 reduction.

Date: 2017
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DOI: 10.1038/s41467-017-01100-7

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