4.7 Article

Tailoring the stability of Fe-N-C via pyridinic nitrogen for acid oxygen reduction reaction

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 437, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135320

Keywords

Oxygen reduction reaction; Durability; PEMFC; Fe-N-C; Metal-organic frameworks

Funding

  1. National Natural Science Foundation of China [21773049, 21433003, 22102041]
  2. China Postdoctoral Science Foundation [2020TQ0084]

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Fe-pyridinic N-C catalysts exhibit remarkable ORR activity and outstanding stability, representing promising alternatives to platinum-based catalysts for electrochemical energy conversion devices.
Developing advanced non-precious metal catalysts towards acidic oxygen reduction reaction (ORR) is critical for electrochemical energy conversion devices. Fe-N-C catalysts are demonstrated to be the most promising alternatives to platinum-based catalysts for ORR. Herein, Fe single atoms (SAs) coordinated by pyridinic nitrogen catalysts (denoted as Fe-pyridinic N-C) are synthesized through pyrolysis of ZIF-8 encapsulating ferrocene. Owing to the synergistic effects between Fe SAs and pyridinic N, Fe-pyridinic N-C exhibits remarkable ORR activity and outstanding stability in acid media, evidenced by golden kinetic current density of 9.71 mA cm-2 at 0.8 V, along with only 21 mV decrease in half-wave potential after 20,000 cycles. Theoretical calculations demonstrate that pyridine-type N possesses stronger binding energy with Fe SAs compared with pyrrole-type N, in other words, high pyridinic N content will help stabilize the catalyst. This study will be of great significance for the development of non-noble metal catalysts towards ORR with enhanced stability in acidic media.

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