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journal article·2026-04Open access

Breaking the ORR Trade‐Off via Mg‐Steered Fe‐N 4 Pyridinic Conversion

Si‐Qi Sun, Ya‐Peng Cheng, Hai‐Ning Zhang, Jia‐Min Lyu, Xiao‐Yun Li, Ke Lyu, Ming‐Hui Sun, Shen Yu, Wen‐Mao Tu, Andreu Cabot, Li‐Hua Chen

Small· Volume 22· Issue 19
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Abstract

ABSTRACT Single‐atom Fe sites coordinated by pyrrolic nitrogen (Fe‐N pyrr ‐C) are highly active for the oxygen reduction reaction (ORR) but suffer from rapid demetalization‐induced deactivation. Here, we overcome this limitation via a Mg‐assisted sacrificial templating strategy that precisely reconstructs Fe‐N 4 coordination, driving partial conversion of unstable pyrrolic‐N to robust pyridinic‐N ligands. The resulting Fe(Mg)‐N‐C(1) catalyst exhibits exceptional ORR performance (half‐wave potential E 1/2 = 0.91 V) and outstanding durability, retaining 95.2% of its initial current after 55 h, surpassing both Fe‐N‐C and Pt/C. In Zn‐air batteries, it enables stable operation for > 530 h (peak power density: 271 mW cm − 2 ). This work demonstrates that enriching pyridinic‐N‐coordinated Fe‐N 4 sites simultaneously enhances activity and suppresses demetalization, offering a general coordination‐engineering strategy to unify activity and stability in Fe‐N‐C electrocatalysts.
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Research context

Energy storageCatalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · Ammonia Synthesis and Nitrogen Reduction · Advancements in Battery Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan P. R. China

Catalonia Institute for Energy Research‐IREC Jardins de les Dones de Negre Sant Adrià de Besòs Catalonia Spain

Universitat de Barcelona Martí i Franquès 1 Barcelona Catalonia Spain

Hubei Key Laboratory of Fuel Cell Wuhan University of Technology Wuhan P. R. China

State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology Wuhan P. R. China

ICREA Pg. Lluis Company Barcelona Catalonia Spain

Funding

National Natural Science Foundation of China · Natural Science Foundation of Hubei Province · China Scholarship Council · Fundamental Research Funds for Central Universities of the Central South University

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