Biomimetic Fe–Cu Porphyrrole Aerogel Electrocatalyst for Oxygen Reduction Reaction

Persky, Yeela; Kielesiński, Łukasz; Reddy, Samala Nagaprasad; Zion, Noam; Friedman, Ariel; Honig, Hilah C.; Koszarna, Beata; Zachman, Michael J.; Grinberg, Ilya; Gryko, Daniel T.; Elbaz, Lior

doi:10.1021/acscatal.3c01972

Title: Biomimetic Fe–Cu Porphyrrole Aerogel Electrocatalyst for Oxygen Reduction Reaction

Journal Article · Fri Aug 04 00:00:00 UTC 2023 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.3c01972 · OSTI ID:1999003

Persky, Yeela ^[1]; Kielesiński, Łukasz ^[2]; Reddy, Samala Nagaprasad ^[1]; Zion, Noam ^[1];

^[1]; Honig, Hilah C. ^[1];

^[2];

^[3]; Grinberg, Ilya ^[1];

^[2];

^[1]

Bar-Ilan Univ., Ramat Gan (Israel)
Polish Academy of Sciences (PAS), Warsaw (Poland)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The development of bioinspired catalysts for oxygen reduction reaction is one of the most prominent pathways in the search for active materials to replace Pt-based catalysts in fuel cells. Herein, we report innovative bioinspired catalysts using a directed synthetic pathway to create adjacent Cu and Fe sites. This catalyst is composed of a covalent 3D framework in an aerogel form. Aerogels are high surface area and porous hierarchical structures that can allow the formation of ultrahigh active site density and optimized mass transport of reactants and products to and from the catalytic sites. The aerogel-based catalyst exhibits high performance in a half-cell in 0.1 M KOH, with an onset potential of 0.94 V vs RHE and half-wave potential of E_1/2 = 0.80 V vs RHE, high selectivity toward the four-electron reduction of oxygen to hydroxide anions, and high durability. These results are well-translated to the anion exchange membrane fuel cell (AEMFC), reaching an open circuit potential of 0.97 V and iR-corrected peak power density of 0.51 W cm^–2. Based on density functional theory calculations, the improved activity relative to the Fe-porphyrin and Cu-corrole is ascribed to the effect of the extended carbon network and the proximity of the metal sites.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1999003

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 16 Vol. 13; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
PGM-free
aerogel
corrole
electrocatalysis
oxygen reduction reaction
porphyrin

Title: Biomimetic Fe–Cu Porphyrrole Aerogel Electrocatalyst for Oxygen Reduction Reaction

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