Structure of Active Sites of Fe-N-C Nano-Catalysts for Alkaline Exchange Membrane Fuel Cells

Kishi, Hirofumi; Sakamoto, Tomokazu; Asazawa, Koichiro; Yamaguchi, Susumu; Kato, Takeshi; Zulevi, Barr; Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen; Matsumura, Daiju; Tamura, Kazuhisa; Nishihata, Yasuo; Tanaka, Hirohisa

doi:10.3390/nano8120965

Title: Structure of Active Sites of Fe-N-C Nano-Catalysts for Alkaline Exchange Membrane Fuel Cells

Journal Article · 21 November 2018 · Nanomaterials

DOI: https://doi.org/10.3390/nano8120965 · OSTI ID:2372745

Kishi, Hirofumi; Sakamoto, Tomokazu; Asazawa, Koichiro; Yamaguchi, Susumu; Kato, Takeshi; Zulevi, Barr; Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen; Matsumura, Daiju; Tamura, Kazuhisa; Nishihata, Yasuo;

Platinum group metal-free (PGM-free) catalysts based on transition metal-nitrogen-carbon nanomaterials have been studied by a combination of ex situ and in situ synchrotron X-ray spectroscopy techniques; high-resolution Transmission Electron Microscope (TEM); Mößbauer spectroscopy combined with electrochemical methods and Density Functional Theory (DFT) modeling/theoretical approaches. The main objective of this study was to correlate the HO2− generation with the chemical nature and surface availability of active sites in iron-nitrogen-carbon (Fe-N-C) catalysts derived by sacrificial support method (SSM). These nanomaterials present a carbonaceous matrix with nitrogen-doped sites and atomically dispersed and; in some cases; iron and nanoparticles embedded in the carbonaceous matrix. Fe-N-C oxygen reduction reaction electrocatalysts were synthesized by varying several synthetic parameters to obtain nanomaterials with different composition and morphology. Combining spectroscopy, microscopy and electrochemical reactivity allowed the building of structure-to-properties correlations which demonstrate the contributions of these moieties to the catalyst activity, and mechanistically assign the active sites to individual reaction steps. Associated with Fe-Nx motive and the presence of Fe metallic particles in the electrocatalysts showed the clear differences in the variation of composition; processing and treatment conditions of SSM. From the results of material characterization; catalytic activity and theoretical studies; Fe metallic particles (coated with carbon) are main contributors into the HO2− generation.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: EE0000459

OSTI ID:: 2372745

Journal Information:: Nanomaterials, Journal Name: Nanomaterials Journal Issue: 12 Vol. 8; ISSN 2079-4991; ISSN NANOKO

Publisher:: MDPI AGCopyright Statement

Country of Publication:: Switzerland

Language:: English

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